Author: "European Project: PeroCUBE" - Searchworks@Jio Institute Digital Library Search Results

Your search keyword '"European Project: PeroCUBE"' showing total 28 results

Start Over Author "European Project: PeroCUBE"

28 results on '"European Project: PeroCUBE"'

1. Deterministic fabrication of 3D/2D perovskite bilayer stacks for durable and efficient solar cells

Author: Sidhik, Siraj, Wang, Yafei, De Siena, Michael, Asadpour, Reza, Torma, Andrew J., Terlier, Tanguy, Ho, Kevin, Li, Wenbin, Puthirath, Anand B., Shuai, Xinting, Agrawal, Ayush, Traore, Boubacar, Jones, Matthew, Giridharagopal, Rajiv, Ajayan, Pulickel M., Strzalka, Joseph, Ginger, David S., Katan, Claudine, Alam, Muhammad Ashraful, Even, Jacky, Kanatzidis, Mercouri G., Mohite, Aditya D., Rice University [Houston], Northwestern University [Evanston], Purdue University [West Lafayette], University of Washington [Seattle], Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Argonne National Laboratory [Lemont] (ANL), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), J.E. acknowledges the financial support from the Institut Universitaire de France. This work was granted access to the HPC resources of [TGCC/CINES/IDRIS] under the allocations 2021-A0090907682 made by GENCI., and European Project: PeroCUBE
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Multidisciplinary
Abstract: Realizing solution-processed heterostructures is a long-enduring challenge in halide perovskites because of solvent incompatibilities that disrupt the underlying layer. By leveraging the solvent dielectric constant and Gutmann donor number, we could grow phase-pure two-dimensional (2D) halide perovskite stacks of the desired composition, thickness, and bandgap onto 3D perovskites without dissolving the underlying substrate. Characterization reveals a 3D–2D transition region of 20 nanometers mainly determined by the roughness of the bottom 3D layer. Thickness dependence of the 2D perovskite layer reveals the anticipated trends for n-i-p and p-i-n architectures, which is consistent with band alignment and carrier transport limits for 2D perovskites. We measured a photovoltaic efficiency of 24.5%, with exceptional stability of T 99 (time required to preserve 99% of initial photovoltaic efficiency) of >2000 hours, implying that the 3D/2D bilayer inherits the intrinsic durability of 2D perovskite without compromising efficiency.
Published: 2022
Full Text: View/download PDF

2. Interfacial engineering to modulate surface dipoles, work functions and dielectric confinement of halide perovskites

Author: Basera, Pooja, Traore, Boubacar, Even, Jacky, Katan, Claudine, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), J.E. acknowledgesthe financial support from the Institut Universitaire de France. This work was granted access tothe HPC resources of TGCC under the allocations 2021-A0110907682 and 2022-A0110907682made by GENCI., European Project: 899141,PoLLoC, and European Project: PeroCUBE
Subjects: [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: Authors are grateful to Maksym Kovalenko and Andriy Stelmakh for useful discussions and providing the MD snapshots.; International audience; The interfacial properties between perovskite photoactive and charge transport layers are critical for device performance and operational stability. Therefore, an accurate theoretical description of the link between surface dipoles and work functions is of scientific and practical interest. We show that for a CsPbBr 3 perovskite surface functionalized by dipolar ligand molecules, the interplay between surface dipoles, charge transfers, and local strain effects leads to upward or downward shifts of the valence level. We further demonstrate that the contribution of individual molecular entities to the surface dipoles and electric susceptibilities are essentially additive. Finally, we compare our results to those predicted from conventional classical approaches based on a capacitor model that links the induced vacuum level shift and the molecular dipole moment. Our findings identify recipes to fine-tune materials work functions that provide valuable insights into the interfacial engineering of this family of semiconductors.
Published: 2023
Full Text: View/download PDF

3. Halide Containing Short Organic Monocations in n = 1–4 2D Multilayered Halide Perovskite Thin Films and Crystals

Author: Skorokhod, Alla, Quarti, Claudio, Abhervé, Alexandre, Allain, Magali, Even, Jacky, Katan, Claudine, Mercier, Nicolas, MOLTECH-Anjou, Université d'Angers (UA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Mons (UMons), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), For DFT calculations, this work was granted access to the HPC resources of TGCC/CINES/IDRIS under the allocation 2020-A0090907682 made by GENCI., ANR-18-CE05-0026,MORELESS,Cellules solaires perovskite plus stables et à teneur réduite en plomb.(2018), and European Project: PeroCUBE
Subjects: General Chemical Engineering, Materials Chemistry, General Chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: International audience; Low electronic band gap 2D multilayered (n=3,4) lead-iodide perovskites with formula A’2An‑1PbnI3n+1 and A’’An‑1PbnI3n+1 are of great interest for photovoltaics, with recent demonstrations of stable solar cell operation based on 2D/3D bilayered heterostructures. Still, the difficulty in achieving optimal phase control, with potential formation of mixed n-domains, is a limiting factor for photovoltaic performance of 2D/3D heterostructures, and the current choice for multi n- layered compounds is limited. Here we report synthesis and XRD characterization of novel (I‑EA)2MAn-1PbnI3n+1 (n=1-4) compound series, along with (Br‑EA)2PbBr4 (n=1) compound, incorporating iodo-ethylammonium (I-EA) and bromo-ethylammonium (Br-EA) spacers. These halide-featuring spacers lead to small lattice mismatch between the inorganic and organic components, that explains the successful formation of multi n- layered compounds. The presence of bromine or iodine in the interlayer space impacts on the dielectric and electronic properties of these materials. Periodic DFT simulations predict vertical hole effective mass for n=1 (I‑EA)2PbI4 as small as 1.8 me, comparable to popular organic semiconductors, like rubrene. UV-vis characterization sets the optical absorption onset of these materials around 1.71 eV for n=3 and 4, hence suggesting these compounds can be successfully implemented in 2D/3D photovoltaic architectures.
Published: 2023
Full Text: View/download PDF

4. Non-Equilibrium Lattice Dynamics in Photo-Excited Two-Dimensional Perovskites

Author: Cuthriell, Shelby, Panuganti, Shobhana, Laing, Craig, Quintero, Michael, Guzelturk, Burak, Yazdani, Nuri, Traore, Boubacar, Brumberg, Alexandra, Malliakas, Christos, Lindenberg, Aaron, Wood, Vanessa, Katan, Claudine, Even, Jacky, Zhang, Xiaoyi, Kanatzidis, Mercouri, Schaller, Richard, Department of Chemistry [Northwestern University], Northwestern University [Evanston], Argonne National Laboratory [Lemont] (ANL), SLAC National Accelerator Laboratory (SLAC), Stanford University, Department of Information Technology and Electrical Engineering, ETH Zurich, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), J.E. acknowledges financial support from the Institute Universitaire de France. This work was granted access to the HPC resources of [TGCC/CINES/IDRIS] under the allocations 2020-A0100911434 and 2020-A0090907682 made by GENCI., and European Project: PeroCUBE
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, lead halide perovskites, transient structures, optical excitation
Abstract: International audience; Interplay between structural and photophysical properties of metal halide perovskites is critical to their utility in optoelectronics, but there is limited understanding of lattice response upon photoexcitation. Here, 2D perovskites butylammonium lead iodide, (BA) PbI , and phenethylammonium lead iodide, (PEA) PbI , are investigated using ultrafast transient X-ray diffraction as a function of optical excitation fluence to discern structural dynamics. Both powder X-ray diffraction and time-resolved photoluminescence linewidths narrow over 1 ns following optical excitation for the fluence range studied, concurrent with slight redshifting of the optical bandgaps. These observations are attributed to transient relaxation and ordering of distorted lead iodide octahedra stimulated mainly by electron-hole pair creation. The c axis expands up to 0.37% over hundreds of picoseconds; reflections sampling the a and b axes undergo one tenth of this expansion with the same timescale. Post-photoexcitation appearance of the (110) reflection in (BA) PbI would suggest a transient phase transition, however, through new single-crystal XRD, reflections are found that violate glide plane conditions in the reported Pbca structure. The static structure space group is reassigned as P2 2 2 . With this, a nonequilibrium phase transition is ruled out. These findings offer increased understanding of remarkable lattice response in 2D perovskites upon excitation.
Published: 2022
Full Text: View/download PDF

5. Lattice dynamics in 3D lead halide hybrid perovskites

Author: Even, Jacky, Hehlen, Bernard, Bourges, Philippe, Létoublon, Antoine, Rufflé, Benoit, Ecolivet, Claude, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Charles Coulomb (L2C), Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), LLB - Nouvelles frontières dans les matériaux quantiques (NFMQ), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Institut de Physique de Rennes (IPR), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Technical University of Munich - Institute for Advanced Study, European Project: PeroCUBE, and European Project: 899141,PoLLoC
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: International audience; Lattice dynamics in 3D lead halide hybrid perovskites is analyzed together with the possible consequences for device applications
Published: 2022

6. Metal halide perovskites and their interfaces: current issues and recent advances

Author: Even, Jacky, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), J.E. acknowledges financial support from the Institute Universitaire de France. This research received funding from the European Union’s Horizon 2020 research and innovation program, through an Innovation Action under the grant agreement No. 861985 (PeroCUBE) and a FET Open action under the grant agreement No. 899141 (PoLLoC)., European Project: 899141,PoLLoC, European Project: PeroCUBE, KATAN, Claudine, Polariton logic - PoLLoC - 899141 - INCOMING, and High-Performance Large Area Organic Perovskite devices for lighting, energy and Pervasive Communications - PeroCUBE - INCOMING
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, solar cells, LED, perovskites, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], DFT, [PHYS.COND] Physics [physics]/Condensed Matter [cond-mat]
Abstract: The considerable attention paid to metal halide perovskites (MHP) in recent years led to several scientific and technological advances, among which the creation of a new photovoltaic (PV) technology that competes with the most widespread ones[1]. With the ever-increasing diversity of applications explored, the need for fundamental understanding persists and may be gained either by smart and simple experimental protocols or models, or else via complex set-ups and computationally expensive ab-initio calculations.At present, MHP materials used in devices are frequently far from their ideal bulk structure, which hinders the use of state-of-the-art first principles simulations including many-body effects and calls for the design of dedicated models. For PV and LEDs, they are mixed with each other in complex alloys and heterostructures, including 2D/3D compositions, combined with additives or protecting layers to improve their stability and/or defectiveness as well as assembled with carrier selective layers. On the other hand, colloidal MHP nanocrystals are promising for devices exploiting both weak and strong light-matter interactions, such as lasers, single photon emitters if not all-optical logic gates. After a general introduction on MHPs, the talk will bring up some of the hot topics in the field and will summarize recent results obtained by the group in Rennes in collaboration with our partners from France and abroad[2-6]. References : [1] https://www.nrel.gov/pv/cell-efficiency.html and https://www.nrel.gov/pv/module-efficiency.html.[2] W. Li et al., Light-activated interlayer contraction in two-dimensional perovskites for high-efficiency solar cells, Nature Nanotechnology, 17, 45 (2022)[3] B. Traore et al., A theoretical framework for microscopic surface and interface dipoles, work functions and valence band alignments in 2D and 3D halide perovskite heterostructures, ACS Energy Lett. 7, 349 (2022) [4] B. Traore et al., Band gap and energy level alignment of 2D and 3D halide perovskites using DFT-1/2, Phys. Rev. Materials, 6, 014604 (2022)[5] S. Sidhik et al., Deterministic fabrication of 3D|2D 1 perovskite bilayer 2 stacks for durable and efficient solar cells, accepted. [6] Q. Akkerman, et al., Taming the nucleation and growth kinetics of lead halide perovskite quantum dots, https://doi.org/10.21203/rs.3.rs-1236393/v1
Published: 2022

7. Tuning the properties of multilayered perovskites and their interfaces for optoelectronic applications

Author: Even, Jacky, Traore, Boubacar, Quarti, Claudio, Jiang, Junke, Pedesseau, Laurent, Volonakis, Yorgos, Kepenekian, Mikaël, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Mons (UMons), and European Project: PeroCUBE
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: National audience; The presentation will focus on the interplay between structural, interfacial and optoelectronic properties in 2D multilayered halide perovskites, either in Ruddlesden Popper (RP) or Dion Jacobson (DJ) structure. At present, perovskite materials are mixed with each other in complex alloys and heterostructures, including 2D/3D compositions, combined with additives or protecting layers to improve their stability and/or defectiveness as well as assembled with carrier selective layers, other materials and components to turn them into devices. Considering the target applications, ambient conditions predominate with additional issues related, for example, to the intrinsic dynamics in action in the MHP structure that may not be well captured using static averaged structures.Based on a set of customized examples, this talk will summarize recent theoretical results obtained by our group that aimed at answering questions such as: i) How do these engineering strategies impact the work function and absolute valence band energy of the MHP material? ii) Is it correlated with surface/interface dipoles? iii) Can one quantitatively assess energy level alignments of MHP semiconductors based on first-principles electronic structure calculations? How can one get rid of the stochastic dynamics of organic cations and further include cation and anion alloying while computing materials properties? iv) Is it possible to extract semi-empirical formula for molecular passivation at surface or transitivity rules for interface dipoles?Special attention will be paid on newly discovered phases and compositions and opportunities to further engineer MHP properties in connection with their use in devices under working conditions. We will see that in practical cases the funneling of electronic carriers to the 2D crystal edges, important for ionization of electron-hole pairs in 2D RP phases, is also at work in bromide perovskites. Continuous and ultrafast photodoping will be further discussed, demonstrating their strong impact on the structural and carrier transport properties of DJ perovskites
Published: 2022

8. Pb-free halide perovskites for solar cells, light-emitting diodes, and photocatalysts

Author: Pingping Jiang, Debdipto Acharya, George Volonakis, Marios Zacharias, Mikaël Kepenekian, Laurent Pedesseau, Claudine Katan, Jacky Even, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), 862656, Horizon 2020 Framework Program, European Project: 862656,DROPIT, and European Project: PeroCUBE
Subjects: [PHYS]Physics [physics], General Engineering, General Materials Science
Abstract: International audience; Metal halide perovskites have recently emerged as one of the most promising classes of semiconductors for various applications, especially in the field of optoelectronics. Lead-based halide perovskite materials, virtually unexploited for decades, have become prominent candidates due to their unique and intrinsic physicochemical and optical properties. Current challenges faced by the scientific community to capitalize on the properties of Pb-based perovskites are mainly associated with environmental concerns due to the toxicity of Pb and their poor stability. Under this context, over recent years, a number of new Pb-free halide perovskite (and perovskite-like) semiconductor classes have been introduced. This Perspective reviews recent developments in Pb-free halide perovskites, which specifically target their application in solar cells, light-emitting devices, and photocatalysts. Each type of Pb-free material is paired with a specific optoelectronic application, and the latest record performances are reported. Although these materials do not yet exhibit as attractive intrinsic optoelectronic properties as the Pb-based halide perovskites, their potential as alternatives for well-suited applications is discussed.
Published: 2022
Full Text: View/download PDF

9. Influence of Chemical Engineering, Photodoping and Lattice Distortions on the Optoelectronic Properties of Multilayered Perovskites

Author: jacky even, claudine katan, wenbin li, hao zhang, boubacar traoré, claudio quarti, siraj sidhik, nicolas mercier, wei li, mercouri kanatzidis, jean-christophe blancon, aditya mohite, alia Skorokhod, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Rice University [Houston], Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Mons (UMons), Université d'Angers (UA), Nankai University (NKU), Northwestern University [Evanston], ANR-18-CE05-0026,MORELESS,Cellules solaires perovskite plus stables et à teneur réduite en plomb.(2018), and European Project: PeroCUBE
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: International audience; The presentation will give an insight into new results on the interplay between structural, interfacial and optoelectronic properties in 2D multilayered halide perovskites, either in Ruddlesden Popper (RP) or Dion Jacobson (DJ) structure. We will see that the funneling of electronic carriers to the 2D crystal edges, important for ionization of electron-hole pairs in 2D RP phases, is also at work in bromide perovskites. Continuous and ultrafast photodoping will be further discussed, demonstrating their strong impact on the structural and carrier transport properties of DJ perovskites. It will also be illustrated how chemical engineering allows tuning the optoelectronic properties of 2D perovskites. Finally, we will introduce a DFT-based semi-empirical methodology to simulate band alignments, interface or surface dipoles and dielectric mismatches in 2D multilayered perovskites.
Published: 2022
Full Text: View/download PDF

10. Recent results on metal halide perovskites and their interfaces*

Author: Traore, Boubacar, Quarti, Claudio, Jiang, Junke, Pedesseau, Laurent, Volonakis, George, Kepenekian, Mikael, Even, Jacky, Katan, Claudine, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), University of Mons [Belgium] (UMONS), This research received funding from the European Union’s Horizon 2020 program, through and Innovation Action under the grant agreement No. 861985 (PeroCUBE). J.E. acknowledges the Institut Universitaire de France., European Project: PeroCUBE, KATAN, Claudine, and High-Performance Large Area Organic Perovskite devices for lighting, energy and Pervasive Communications - PeroCUBE - INCOMING
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.MATE] Chemical Sciences/Material chemistry, [CHIM.MATE]Chemical Sciences/Material chemistry, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], [PHYS.COND] Physics [physics]/Condensed Matter [cond-mat]
Abstract: International audience; The considerable attention paid to metal halide perovskites (MHP) in recent years led to several scientific and technological advances. This in turn raised important questions that currently challenge the limits of available theoretical techniques and atomistic models. At present, perovskite materials are mixed with each other in complex alloys and heterostructures, including 2D/3D compositions, combined with additives or protecting layers to improve their stability and/or defectiveness as well as assembled with carrier selective layers, other materials and components to turn them into devices. Considering the target applications, ambient conditions predominate with additional issues related, for example, to the intrinsic dynamics in action in the MHP structure that may not be well captured using static averaged structures.Based on a set of customized examples, this talk will summarize recent theoretical results obtained by our group that aimed at answering questions such as: i) How do these engineering strategies impact the work function and absolute valence band energy of the MHP material? ii) Is it correlated with surface/interface dipoles? iii) Can one quantitatively assess energy level alignments of MHP semiconductors based on first-principles electronic structure calculations? How can one get rid of the stochastic dynamics of organic cations and further include cation and anion alloying while computing materials properties? iv) Is it possible to extract semi-empirical formula for molecular passivation at surface or transitivity rules for interface dipoles? Special attention will be paid on newly discovered phases and compositions and opportunities to further engineer MHP properties in connection with their use in devices under working conditions.*This research received funding from the European Union’s Horizon 2020 program, through and Innovation Action under the grant agreement No. 861985 (PeroCUBE). J.E. acknowledges the Institut Universitaire de France.
Published: 2022

11. Expanding the Cage of 2D Bromide Perovskites by Large A-Site Cations

Author: Xiaotong Li, Shelby A. Cuthriell, Ashanti Bergonzoni, Hao Dong, Boubacar Traoré, Constantinos C. Stoumpos, Peijun Guo, Jacky Even, Claudine Katan, Richard D. Schaller, Mercouri G. Kanatzidis, Northwestern University [Evanston], Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Yale University [New Haven], Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), University of Crete [Heraklion] (UOC), Argonne National Laboratory [Lemont] (ANL), A.B. acknowledges support from Region Bretagne through the PERFOTON project. This work was granted access to the HPC resources of [TGCC/CINES/IDRIS] under the allocations 2021-A0100911434 and 2021-A0110907682 made by GENCI. J.E. acknowledges financial support from the Institut Universitaire de France., and European Project: PeroCUBE
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, General Chemical Engineering, Materials Chemistry, General Chemistry
Abstract: International audience; Two-dimensional (2D) halide perovskites have outstanding optoelectronic properties, and they feature a variety of organic cation spacers and cage A-site cations that can be incorporated into their structures. It has recently been reported that the Goldschmidt tolerance factor can be relaxed and expanded in iodide 2D perovskites. Bromide 2D perovskites, whose multilayer structures and optical properties are much less studied, provide a great platform for studying structure–property relationships for 2D perovskites with large A-site cations. Herein, we report the synthesis and structure of three new 2D bromide perovskites─(BA)2(MHy)2Pb3Br10 (BA, butylammonium; MHy, methylhydrazinium), (BA)2(EA)2Pb3Br10 (EA is ethylammonium), and (BA)2(DMA)Pb2Br7 (DMA is dimethylammonium). We compared them with other 2D perovskites with different A-site cations but with the same spacer and layer thickness. Single-crystal structures show that the Pb–Br bonds are elongated to accommodate the large A-site cations. Additionally, the octahedra in (BA)2(MHy)2Pb3Br10 and (BA)2(EA)2Pb3Br10 are highly distorted, and their different stacking patterns of the inner and outer layers lead to the formation of the n = 3 phases. Density functional theory calculations show that 2D perovskites with larger A-site cations (e.g., DMA, MHy, and EA) have smaller band dispersions and larger effective masses than those with Cs+ and MA. (BA)2(MHy)2Pb3Br10 also exhibits one of the largest Rashba splittings in the literature. Structures with large cage cations also exhibit high band gaps within the same n number and short photoluminescence (PL) lifetimes. Temperature- and power-dependent PL measurements reveal that the broad shoulder in the PL peak originates from the trap states.
Published: 2022
Full Text: View/download PDF

12. A theoretical framework for microscopic surface and interface dipoles, work functions and valence band alignments in 2D and 3D halide perovskite heterostructures

Author: Traoré, Boubacar, Basera, Pooja, Ramadan, Alexandra J., Snaith, Henry J., Katan, Claudine, Even, Jacky, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), University of Oxford, Clarendon Laboratory [Oxford], J.E. acknowledges financial support from the Institute Universitaire de France., European Project: PeroCUBE, Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), and University of Oxford [Oxford]
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Fuel Technology, Renewable Energy, Sustainability and the Environment, Chemistry (miscellaneous), Materials Chemistry, Energy Engineering and Power Technology, 02 engineering and technology, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 0210 nano-technology, 01 natural sciences, 0104 chemical sciences
Abstract: The work was granted access to the HPC resources of [TGCC/CINES/IDRIS] under the allocations 2020-A0100911434 and 2020-A0090907682 made by GENCI.; International audience; We propose a computational methodology that highlights the intimate connection between surface and interface dipoles and work functions or valence band alignments. We apply the methodology to inspect the energy level alignments of halide perovskites and explore various situations relevant to perovskite-based heterostructures: i) the effect of surface termination, the ability to fine-tune and interpret the shift in energy alignments via ii) surface coating and iii) surface functionalization and/or passivation with molecules. We highlight the importance of local strain relaxation at the surfaces or interfaces, and revisit classical approaches based on capacitor models. Finally, we show that surface dipoles are additive in heterostructures and illustrate it through a 2D/3D perovskite interface. This provides a handy tool to interpret band alignments in complex perovskite-based heterostructures and buried interfaces. The scope of our work goes far beyond halide perovskites and can be useful to scrutinize the surfacial and interfacial behaviors of other semiconductors and heterojunctions. It allows bridging results from atomistic ab initio calculations and classical simulation approaches for multilayered thin film devices.
Published: 2022
Full Text: View/download PDF

13. Band gap, effective masses, and energy level alignment of 2D and 3D halide perovskites and heterostructures using DFT-1/2

Author: Boubacar Traore, Jacky Even, Laurent Pedesseau, Mikaël Képénekian, Claudine Katan, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA), J.E. acknowledges financial support from the Institute Universitaire de France., and European Project: PeroCUBE
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, Physics and Astronomy (miscellaneous), General Materials Science, [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract: The work was granted access to the HPC resources of [TGCC/CINES/IDRIS] under the allocations 2020-A0100911434 and 2020-A0090907682 made by GENCI.; International audience; We revisit the Slater half-occupation technique within the DFT-1/2 method to provide improved accuracy of 2D and 3D halide perovskites band gaps at a moderate computational cost. We propose an electron removal scheme from the halide states that drastically improve the predicted band gaps of 2D compounds. Concurrently, we compute the effective masses of the considered structures and show that DFT-1/2 describes them with a nice degree of accuracy when compared to available experimental data. Moreover, we assess the suitability of DFT-1/2 to compute the energy level alignments of this family of compounds. We compare the results in light of those we predict using the hybrid functional HSE06 and the many body perturbation theory within the $G0W0$ approximation. We discuss the limitations of our refined DFT-1/2 scheme, which tends to overestimate the downshift of the absolute valence energy levels of the layered perovskite systems. We anticipate that our results would be useful to initiate benchmark studies and investigate large systems such as heterostructures for which other approaches may be out of reach.
Published: 2022
Full Text: View/download PDF

14. Physics of 2D perovskites

Author: Even, Jacky, Blancon, Jean Christophe, Sidhik, Siraj, li, weibin, Zhang, Hao, Li, Wei, Traore, Boubacar, Pedesseau, Laurent, Volonakis, George, Kepenekian, Mikael, Stoumpos, Constantinos, Kanatzidis, Mercouri, Mohite, Aditya, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Rice University [Houston], Nankai University (NKU), Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), University of Crete [Heraklion] (UOC), Northwestern University [Evanston], European Project: PeroCUBE, European Project: 899141,PoLLoC, Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS]Physics [physics]
Abstract: International audience; In the past years, solution-processed organometallic perovskite based solar cells have emerged as a promising low-cost thin-film photovoltaic technology. 3D halide perovskite semiconductors and their 2D or OD nanostructures present specific symmetry and electronic properties, including giant spin-orbit coupling (SOC) effects. The ultrahigh softness of the halide perovskite lattice is also characteristic, and the role of the electron-phonon coupling, especially at temperatures relevant for device operation, is not fully understood. The presentation will focus on 2D perovskites, composed of perovskites layers sandwiched between two layers of large organic cations, described in the 90’s as self-assembled quantum and dielectric well systems.
Published: 2021

15. Using large scale scattering facilities to study structural and optoelectronic properties of 2D and 3D perovskites

Author: Even, Jacky, Sidhik, Siraj, li, weibin, Zhang, Hao, Traoré, Boubacar, Bourges, Philippe, Kanatzidis, Mercouri, Blancon, Jean Christophe, Mohite, Aditya, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Rice University [Houston], Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, Northwestern University [Evanston], Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), J. Even acknowledges the financial support from the Institut Universitaire de France., European Project: 899141,PoLLoC, European Project: PeroCUBE, European Project: 862656,DROPIT, even, jacky, Polariton logic - PoLLoC - 899141 - INCOMING, High-Performance Large Area Organic Perovskite devices for lighting, energy and Pervasive Communications - PeroCUBE - INCOMING, and DRop-on demand flexible Optoelectronics & Photovoltaics by means of Lead-Free halide perovskITes - DROPIT - 862656 - INCOMING
Subjects: [PHYS]Physics [physics], [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, [PHYS] Physics [physics]
Abstract: National audience; The presentation will describe a few recent results on the structural and optoelectronic properties in 2D and 3D halide perovskites, focusing on some possibilities offered by nowadays neutron, X-rays and electron large scale scattering facilities.
Published: 2021

16. Light-activated interlayer contraction leads to high-efficiency in 2D perovskite solarcells

Author: Traoré, Boubacar, Li, Wenbin, Sidhik, Siraj, Asadpour, Reza, Hou, Jin, Zhang, Hao, Fehr, Austin, Essman, Joseph, Wang, Yafei, Hoffman, Justin, Spanopoulos, Ioannis, Crochet, Jared, Tsai, Esther, Strzalka, Joseph, Alam, Muhammad, Kanatzidis, Mercouri, Katan, Claudine, Blancon, Jean Christophe, Mohite, Aditya, Even, Jacky, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Rice University [Houston], Purdue University [West Lafayette], Northwestern University [Evanston], Los Alamos National Laboratory (LANL), Brookhaven National Laboratory [Upton, NY] (BNL), UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), State University of New York (SUNY)-State University of New York (SUNY)-U.S. Department of Energy [Washington] (DOE), Argonne National Laboratory [Lemont] (ANL), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), J. Even acknowledges the financial support from the Institut Universitaire de France. DFT calculations were performed at Institut FOTON as well as Institut des Sciences Chimiques de Rennes, and the work was granted access to the HPC resources of Très Grand Centre de Calcul du CEA (TGCC), the Centre Informatique National de I’Enseignement Supérieur (CINES) and Institut du développement et des ressources en informatique scientifique (IDRIS) under allocations 2019-A0060906724 and 2019-A0070907682 made by Grand Équipement National de Calcul Intensif (GENCI)., CNRS Israeli French scientific cooperation (Joint Research Projects 2019-2021 ALLPOA)., European Project: PeroCUBE, Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), U.S. Department of Energy [Washington] (DOE)-UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), State University of New York (SUNY)-State University of New York (SUNY), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), even, jacky, and High-Performance Large Area Organic Perovskite devices for lighting, energy and Pervasive Communications - PeroCUBE - INCOMING
Subjects: [PHYS]Physics [physics], [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, [PHYS] Physics [physics]
Abstract: National audience; Despite their improved stability and versatility, 2D layered perovskites’ solar cell efficiencies lag behind those of their 3D counterparts, which currently exceed 25%. Through a proper selection of the organic spacer, 2D perovskites can be synthetized in different configurations adopting various phases such as the Ruddlesden-Popper (RP), the Alternating Cation Interlayer (ACI) or the Dion-Jacobson ones. Tailoring the organic spacer type has been shown to enhance the electronic coupling along the layered perovskite stacking axis and thereby enhance carrier transport resulting in improved efficiencies.
Published: 2021

17. Microscopic connection between absolute valence energy alignment and surface dipoles in halide perovskite heterostructures

Author: Traoré, Boubacar, Basera, Pooja, Ramadan, Alexandra, Snaith, Henry, Katan, Claudine, Even, Jacky, Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), University of Oxford, European Project: PeroCUBE, Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), and University of Oxford [Oxford]
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: National audience; In recent years, hybrid organic-inorganic perovskites (HOP) have undergone extensive research due to their excellent photovoltaic and optoelectronic properties. To further improve their device performance, there is a considerable ongoing research effort on their surface passivation and/or functionalization. This stems from the fact that surface passivation and/or functionalization, including the combination of 2D and 3D perovskites, directly influences the surface dipoles between adjacent layers in a device stack, which in turn changes materials' work functions and absolute energy level alignments. However, the link between the two lacks a general framework bridging classical electromagnetism and modern atomistic approaches. Shedding more light on this link is of great technological importance to fully exploit the potentials of these semiconductors. Hence, this contribution presents a theoretical methodology thatclearly shows the relationship between surface dipoles and work functions. We rely on a semiclassical approach, that will allow scientists not specialized in DFT computation, to make use of their chemical or physical intuitions. We demonstrate the potentials of the methodology through a variety of cases to clearly show i) the effect of surface termination on the absolute energy level alignments, the ability to modulate the work function via ii) surface coating and iii) surface functionalization and/or passivationwith molecules. Finally, we demonstrate the additivity of surface dipoles in heterostructures, which is analogous to the additivity of the dielectric susceptibility in these compounds. Our methodology transcends the limits of halide perovskites and provides a computational strategy to fine-tune the absolute energy level alignments for optimizing the performance of broader families of optoelectronic devices
Published: 2021

18. Theoretical insights to tune the surface dipoles and work functions of halide perovskites

Author: basera, pooja, Traoré, Boubacar, Even, Jacky, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Israeli-French scientific cooperation (Joint Research Projects 2019-2021 ALLPOA) CNRS., European Project: PeroCUBE, European Project: 899141,PoLLoC, Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: National audience; Lead halide perovskites have attracted considerable interest owing to their rich physics and rapidly burgeoning applications in the field of optoelectronic devices. Therefore, an accurate theoretical description of the link between surface dipoles and the work functions, especially to understand the interface effects in this class of materials is of scientific and practical interest. Herein, we briefly introduce our methodology that accentuates the relation between the surface dipoles and the work functions using concepts from classical physics combined with the state-of-the-art first-principles calculations.
Published: 2021

19. Interfacial engineering to modulate surface dipoles, work functions and dielectric confinement of halide perovskites via surface passivation

Author: basera, pooja, Traoré, Boubacar, Katan, Claudine, Even, Jacky, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), European Project: PeroCUBE, European Project: 899141,PoLLoC, Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences
Abstract: National audience; Lead halide perovskites have attracted considerable interest owing to their rich physics and rapidly burgeoning applications in the field of optoelectronic devices. Therefore, an accurate theoretical description of the link between surface dipoles and the work functions, especially to understand the interface effects in this class of materials is of scientific and practical interest.
Published: 2021

20. Importance of lattice softness and phonon anharmonicity for the optoelectronic properties of 3D, 2D and 0D halide perovskites

Author: Even, Jacky, Da Cunha Ferreira, Afonso, Paofai, Serge, Létoublon, Antoine, Ollivier, Jacques, Raymond, stéphane, Sébastien, Clément, VIALLA, Remy, HEHLEN, Bernard, RUFFLE, Benoit, Cordier, Stéphane, Katan, Claudine, Bourges, Philippe, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut Laue-Langevin (ILL), Magnétisme et Diffusion Neutronique (MDN ), Modélisation et Exploration des Matériaux (MEM), Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), Laboratoire Charles Coulomb (L2C), Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), European Project: 899141,PoLLoC, European Project: PeroCUBE, European Project: 862656,DROPIT, Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), ILL, and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS
Abstract: National audience
Published: 2021

21. Propriétés optoélectroniques et structurales des pérovskites halogénées 3D, 2D and 0D : quelques résultats récents

Author: Even, Jacky, Pedesseau, Laurent, Kepenekian, Mikael, Katan, Claudine, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), European Project: 899141,PoLLoC, European Project: PeroCUBE, European Project: 862656,DROPIT, Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS]Physics [physics], [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS
Abstract: National audience
Published: 2021

22. m -Phenylenediammonium as a New Spacer for Dion–Jacobson Two-Dimensional Perovskites

Author: Shengzhong Liu, Yalan Zhang, Boubacar Traoré, Xiaotong Li, Claudine Katan, Yu Han, Kui Zhao, Mercouri G. Kanatzidis, Lili Gao, Junjie Fang, Jacky Even, Shaanxi Normal University (SNNU), Northwestern University [Evanston], Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), J.E. acknowledges the financial support fromthe Institut Universitaire de France. The calculation work wasgranted access to the HPC resources of [TGCC/CINES/IDRIS] under the allocation 2020-A0080911434 made byGENCI., European Project: PeroCUBE, Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), and Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT)
Subjects: business.industry, Chemistry, Band gap, Stacking, Halide, 02 engineering and technology, General Chemistry, Crystal structure, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 7. Clean energy, 01 natural sciences, Biochemistry, Catalysis, 0104 chemical sciences, Crystallography, Colloid and Surface Chemistry, Semiconductor, [CHIM.CRIS]Chemical Sciences/Cristallography, Density functional theory, 0210 nano-technology, Dispersion (chemistry), business, Perovskite (structure)
Abstract: International audience; Two-dimensional (2D) halide perovskites have several distinct structural classes and exhibit great tunability, stability, and high potential for photovoltaic applications. Here, we report a new series of hybrid 2D perovskites in the Dion–Jacobson (DJ) class based on aromatic m-phenylenediammonium (mPDA) dications. The crystal structures of the DJ perovskite materials (mPDA)MAn–1PbnI3n+1 (n = 1–3) were solved and refined using single-crystal X-ray crystallography. The results indicate a short I···I interlayer distance of 4.00–4.04 Å for the (mPDA)MAn–1PbnI3n+1 (n = 2 and 3) structures, which is the shortest among DJ perovskites. However, Pb–I–Pb angles are as small as 158–160°, reflecting the large distortion of the inorganic framework, which results in larger band gaps for these materials than those in other DJ analogues. Density functional theory calculations suggest appreciable dispersion in the stacking direction, unlike the band structures of the Ruddlesden–Popper phases, which exhibit flat bands along the stacking direction. This is a consequence of the short interlayer I···I distances that can lead to interlayer electronic coupling across the layers. The solution-deposited films (nominal (mPDA)MAn–1PbnI3n+1 compositions of n = 1–6) reveal improved surface coverage with increasing nominal n value with the higher n films being composed of a mixture of n = 1 and bulk three-dimensional MAPbI3 perovskites. The films made from solutions of these materials behave differently from those of other 2D iodide perovskites, and their solar cells have a mixture of n = 1 DJ and MAPbI3 as light-absorbing semiconductors.
Published: 2021
Full Text: View/download PDF

23. Physical properties of bulk, defective, 2D and 0D metal halide perovskite semiconductors from a symmetry perspective

Author: Claudio Quarti, Claudine Katan, Jacky Even, University of Mons [Belgium] (UMONS), Institut des Sciences Chimiques de Rennes (ISCR), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), MORELESS, Agence Nationale de la Recherche, 861985, Horizon 2020 Framework Programme, ANR-18-CE05-0026,MORELESS,Cellules solaires perovskite plus stables et à teneur réduite en plomb.(2018), European Project: PeroCUBE, Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Materials science, Halide, 02 engineering and technology, Electronic structure, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Nanomaterials, Metal, [CHIM]Chemical Sciences, General Materials Science, ComputingMilieux_MISCELLANEOUS, Perovskite (structure), [PHYS]Physics [physics], Condensed matter physics, business.industry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Atomic and Molecular Physics, and Optics, Symmetry (physics), 0104 chemical sciences, Semiconductor, visual_art, visual_art.visual_art_medium, 0210 nano-technology, business, Group theory
Abstract: Metal halide perovskite-based nanostructures, nanosheets and nanoparticles at the forefront, show attractive optoelectronic properties, suitable for photovoltaics and light emission applications. Achieving a sounded understanding of these basic electronic and optical properties represents therefore a crucial step for the full technological exploitation of this class of semiconductors. The rapidly expanding chemical engineering and their unusual structural diversity is fascinating but also challenging for a rational description on par with those well-known for conventional semiconductors. In this sense, group theory-based symmetry analyses offer a general and rigorous approach to understand the properties of various bulk perovskites and perovskite-based nanostructures. In this work, we review the electronic and optical response of metal halide perovskite semiconductors using symmetry analysis from group theory, recalling the main results for the prototypical cubic Pm-3m lattice of AMX3 bulk perovskites (where A is cation, M metal and X halide), then extending the analysis to three cases of technological interest: AMX3 nanoparticles, A4MX6 isolated octahedra, A2MX4 layered systems, and recently introduced deficient halide perovskites (d-HP). On the basis of symmetry arguments, we will stress analogies and differences in the electronic and optical properties of these materials, as induced by the spatial confinement and dimensionality. Meanwhile, we will take advantage of this analysis to discuss recent results and debates from the literature, as the energetics of dark/bright states in the band-edge exciton fine structure of perovskite nanoparticles and nanosheets. From the present work, we also anticipate that the band-edge exciton fine structure of d-HP does not present optically dark states, in striking contrast to AMX3 nanoparticles and layered perovskites, a fact that can have important consequences on the photophysics of these novel perovskitoids.
Published: 2020
Full Text: View/download PDF

24. Structural Isomer of Fluorinated Ruddlesden-Popper Perovskites Toward Efficient and Stable 2D/3D Perovskite Solar Cells

Author: Byeon, Junseop, Cho, Seong Ho, Jiang, Junke, Jang, Jihun, Katan, Claudine, Even, Jacky, Xi, Jun, Choi, Mansoo, Lee, Yun Seog, Seoul National University [Seoul] (SNU), Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Xi'an Jiaotong University (Xjtu), 2012M3A6A7054855, National Research Foundation of Korea, 861985, H2020 European Institute of Innovation and Technology, Seoul National University, 62205264, National Natural Science Foundation of China, 11302291010704, Xi'an Jiaotong University Young Talents Support Program, and European Project: PeroCUBE
Subjects: 2D perovskite stability, structural isomer, 2D perovskite, [CHIM.MATE]Chemical Sciences/Material chemistry, Ruddlesden-Popper perovskite, stability
Abstract: International audience; Defect passivation using two-dimensional (2D)-layered perovskites with organic spacers on 3D bulk perovskites has been proposed as an effective strategy to improve perovskite solar cell stability and efficiency. Specifically, fluorination of the organic spacers has been employed due to the resulting hydrophobic nature and the defect passivation characteristics. In addition to the type of functional groups attached to the spacer molecules, conformational changes of fluorine isomers on layered perovskites can provide an extended strategy to control a variety of opto-electrical properties related to the interlayer spacing. As a model system for the structural isomer of fluorinated spacers, meta-CF3 and para-CF3 groups anchored to phenethylammonium iodide (PEAI) spacer molecules are employed to synthesize 2D perovskites and to investigate their full potential as an interfacial modifier for perovskite solar cells. The fluorination position change leads to altered opto-electrical characteristics in layered perovskites. Although they possess identical functional groups, the different orientations of the functional groups used in the perovskite layer deposited on the 3D perovskite absorber result in distinct electrical properties of 2D/3D heterostructures due to dissimilar intermolecular interactions. The 2D perovskite with meta-CF3-PEAI spacers exhibits an enhancement of the charge transport in the out-of-plane orientation and an improved suppression of the trap states of 3D perovskites while also providing a more favorable energy alignment for efficient charge transfers. Theoretical simulations are consistent with the experimental results. The structural isomers of fluorination anchoring to spacer cations alter the structural configuration of the spacer as well as the interlayer spacing that can improve the performance and the stability of 2D/3D perovskite solar cells.
Full Text: View/download PDF

25. Ordered Mixed-Spacer 2D Bromide Perovskites and the Dual Role of 1,2,4-Triazolium Cation

Author: Xiaotong Li, Hao Dong, George Volonakis, Constantinos C. Stoumpos, Jacky Even, Claudine Katan, Peijun Guo, Mercouri G. Kanatzidis, Department of Chemistry [Northwestern University], Northwestern University [Evanston], Yale University [New Haven], Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), University of Crete [Heraklion] (UOC), Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), At Rennes this work received funding from the Chaire de Recherche Rennes Metropole project and the European Union’s Horizon 2020 research and innovation program under grant agreement No. 861985 (PeroCUBE). J.E. acknowledges financial support from the Institute Universitaire de France., and European Project: PeroCUBE
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, General Chemical Engineering, Materials Chemistry, General Chemistry
Abstract: This work was granted access to the HPC resources of TGCC under Allocations No. 2021-A0100911434 and 2021-A0110907682 made by GENCI. We acknowledge PRACE for awarding us access to ARCHER2, United Kingdom.; International audience; Two-dimensional (2D) halide perovskites exhibit extraordinary stability and structural diversity because they can incorporate different organic cations (both cage A-site cation and the spacer). Here we report on the behavior of Tz = 1,2,4-triazolium as an A-site cation as well as a spacer cation in new perovskite compounds. We describe the synthesis and structure-property relationships of a new family of hydrogen-bonding stabilized 2D perovskites, (IPA)2(Tz)n-1PbnBr3n+1 (n = 1-3) (IPA = isopropylammonium, Tz = 1,2,4-triazolium), which represents the rare example of 2D perovskites incorporating large A-site cation (Tz) that can form both the n = 2 and 3 phases. However, excess of Tz cations can split the n = 2 layers to act as spacer, and combine with another spacer PA (PA = propylammonium) or BA (BA = butylammonium) to form n = 1 structures (PA)(Tz)PbBr4 and (BA)(Tz)PbBr4. These ordered mixed-spacer perovskites with different interlayer distances are unusual because the different spacers tend to stay in the same interlayer. (IPA)2(Tz)n-1PbnBr3n+1 all exhibit broad photoluminescence (PL) emission, but for different reasons. For the n = 1 phase, the large octahedral tilting (small Pb-Br-Pb angle) gives rise to the broad emission, while for the n = 2 and 3 phases, the individual octahedral distortion (large distortion index) plays a more important role. For the mixed-spacer (PA)(Tz)PbBr4 and (BA)(Tz)PbBr4, their bandgaps are in between the parent n = 1 compounds ((BA)2PbBr4 or (PA)2PbBr4 , and (Tz)2PbBr4). DFT calculations suggest that the band structures of (PA)(Tz)PbBr4 and (BA)(Tz)PbBr4 combine features from both parent compounds yet differ from a simple superposition. This work demonstrates the dual role of Tz molecules as the A-site cation in multilayer 2D perovskites and as the spacer in ordered mixed-spacer 2D phases.
Full Text: View/download PDF

26. 2D multilayered perovskites and 2D/3D bilayers for stable solar cells

Author: Even, Jacky, Sidhik, Siraj, Kepenekian, Mikael, Traoré, Boubacar, Katan, Claudine, Kanatzidis, Mercouri, Mohite, Aditya, Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Rice University [Houston], Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Northwestern University [Evanston], J.E. acknowledges financial support from the Institute Universitaire de France. This work was granted access to the HPC resources of [TGCC/CINES/IDRIS] under the allocations 2020-A0100911434 and 2020-A0090907682 made by GENCI., and European Project: PeroCUBE
Subjects: solar cell, elasticity, heterostructure, [CHIM.MATE]Chemical Sciences/Material chemistry, perovskite
Abstract: International audience; The contribution focuses on a theoretical analysis of 2D multilayered halide perovskites, and their interfaces with 3D perovskites. At present, perovskite materials are mixed with each other in complex alloys and heterostructures, including 2D/3D compositions, combined with additives or protecting layers to improve their stability as well as assembled with carrier selective layers. The specificities of the mechanical properties of halide perovskites by comparison to classical semiconductors and the role played by large cations in the interlayer of the 2D perovskite are discussed.
Full Text: View/download PDF

27. Ultrafast relaxation of lattice distortion in two-dimensional perovskites

Author: Hao Zhang, Wenbin Li, Joseph Essman, Claudio Quarti, Isaac Metcalf, Wei-Yi Chiang, Siraj Sidhik, Jin Hou, Austin Fehr, Andrew Attar, Ming-Fu Lin, Alexander Britz, Xiaozhe Shen, Stephan Link, Xijie Wang, Uwe Bergmann, Mercouri G. Kanatzidis, Claudine Katan, Jacky Even, Jean-Christophe Blancon, Aditya D. Mohite, Rice University [Houston], Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université de Mons (UMons), SLAC National Accelerator Laboratory (SLAC), Stanford University, University of Wisconsin-Madison, Northwestern University [Evanston], Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), ANR-18-CE05-0026,MORELESS,Cellules solaires perovskite plus stables et à teneur réduite en plomb.(2018), and European Project: PeroCUBE
Subjects: [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], General Physics and Astronomy
Abstract: International audience; Direct visualization of ultrafast coupling between charge carriers and lattice degrees of freedom in photoexcited semiconductors has remained a long-standing challenge and is critical for understanding the light-induced physical behaviour of materials under extreme non-equilibrium conditions. Here we obtain a direct visualization of the structural dynamics in monocrystalline 2D perovskites. We achieve this by monitoring the evolution of wavevector-resolved ultrafast electron diffraction intensity following above-bandgap high-density photoexcitation. Our analysis reveals a light-induced ultrafast reduction in antiferro-distortion resulting from a strong interaction between the electron–hole plasma and perovskite lattice, which induces an in-plane octahedra rotation towards a more symmetric phase. Correlated ultrafast spectroscopy performed at the same carrier density as ultrafast electron diffraction reveals that the creation of a dense electron–hole plasma triggers the relaxation of lattice distortion at shorter timescales by modulating the crystal cohesive energy. Finally, we show that the interaction between carrier gas and lattice can be altered by tailoring the rigidity of the 2D perovskite by choosing an appropriate organic spacer layer.
Full Text: View/download PDF

28. High-phase purity two-dimensional perovskites with 17.3% efficiency enabled by interface engineering of hole transport layer

Author: Xinjue Zhong, Ayush Agrawal, Ioannis Spanopoulos, Siraj Sidhik, Claudine Katan, Antoine Kahn, Boubacar Traore, Anamika Mishra, Amanda B. Marciel, Mercouri G. Kanatzidis, Wenbin Li, Jacky Even, Yafei Wang, Aditya D. Mohite, Jean-Christophe Blancon, Mohammad H. K. Samani, Ido Hadar, Hao Zhang, Rice University [Houston], Princeton University, Northwestern University [Evanston], Institut des Fonctions Optiques pour les Technologies de l'informatiON (Institut FOTON), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), J.E. acknowledges the financial support from the Institut Universitaire de France, European Project: PeroCUBE, Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-École Nationale Supérieure des Sciences Appliquées et de Technologie (ENSSAT)-Centre National de la Recherche Scientifique (CNRS)-IMT Atlantique Bretagne-Pays de la Loire (IMT Atlantique), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), and Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)
Subjects: Materials science, General Physics and Astronomy, Ruddlesden-Popper, nickel oxide, 02 engineering and technology, 2D perovskites, 010402 general chemistry, photostability, 01 natural sciences, law.invention, Crystallinity, law, General Materials Science, Diode, Perovskite (structure), business.industry, Nickel oxide, Photoresistor, Doping, General Engineering, phase purity, General Chemistry, 021001 nanoscience & nanotechnology, Suns in alchemy, 0104 chemical sciences, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, General Energy, Optoelectronics, 0210 nano-technology, business, lithium doping, Voltage
Abstract: International audience; State-of-the-art p-i-n-based 3D perovskite solar cells (PSCs) use nickel oxide (NiOX) as an efficient hole transport layer (HTL), achieving efficiencies >22%. However, translating this to phase-pure 2D perovskites has been unsuccessful. Here, we report 2D phase-pure Ruddlesden-Popper BA2MA3Pb4I13 perovskites with 17.3% efficiency enabled by doping the NiOX with Li. Our results show that progressively increasing the doping concentration transforms the photoresistor behavior to a typical diode curve, with an increase in the average efficiency from 2.53% to 16.03% with a high open-circuit voltage of 1.22 V. Analysis reveals that Li doping of NiOX significantly improves the morphology, crystallinity, and orientation of 2D perovskite films and also affords a superior band alignment, facilitating efficient charge extraction. Finally, we demonstrate that 2D PSCs with Li-doped NiOX exhibit excellent photostability, with T99 = 400 h at 1 sun and T90 of 100 h at 5 suns measured at relative humidity of 60% ± 5% without the need for external thermal management.
Full Text: View/download PDF

Catalog

Books, media, physical & digital resources

See catalog results

Searchworks

Select search scope, currently: Articles

Catalog

books, media & more in Jio Institute collections

Articles

journal articles & other e-resources

Refine your results

28 results on '"European Project: PeroCUBE"'

1. Deterministic fabrication of 3D/2D perovskite bilayer stacks for durable and efficient solar cells

2. Interfacial engineering to modulate surface dipoles, work functions and dielectric confinement of halide perovskites

3. Halide Containing Short Organic Monocations in n = 1–4 2D Multilayered Halide Perovskite Thin Films and Crystals

4. Non-Equilibrium Lattice Dynamics in Photo-Excited Two-Dimensional Perovskites

5. Lattice dynamics in 3D lead halide hybrid perovskites

6. Metal halide perovskites and their interfaces: current issues and recent advances

7. Tuning the properties of multilayered perovskites and their interfaces for optoelectronic applications

8. Pb-free halide perovskites for solar cells, light-emitting diodes, and photocatalysts

9. Influence of Chemical Engineering, Photodoping and Lattice Distortions on the Optoelectronic Properties of Multilayered Perovskites

10. Recent results on metal halide perovskites and their interfaces*

11. Expanding the Cage of 2D Bromide Perovskites by Large A-Site Cations

12. A theoretical framework for microscopic surface and interface dipoles, work functions and valence band alignments in 2D and 3D halide perovskite heterostructures

13. Band gap, effective masses, and energy level alignment of 2D and 3D halide perovskites and heterostructures using DFT-1/2

14. Physics of 2D perovskites

15. Using large scale scattering facilities to study structural and optoelectronic properties of 2D and 3D perovskites

16. Light-activated interlayer contraction leads to high-efficiency in 2D perovskite solarcells

17. Microscopic connection between absolute valence energy alignment and surface dipoles in halide perovskite heterostructures

18. Theoretical insights to tune the surface dipoles and work functions of halide perovskites

19. Interfacial engineering to modulate surface dipoles, work functions and dielectric confinement of halide perovskites via surface passivation

20. Importance of lattice softness and phonon anharmonicity for the optoelectronic properties of 3D, 2D and 0D halide perovskites

21. Propriétés optoélectroniques et structurales des pérovskites halogénées 3D, 2D and 0D : quelques résultats récents

22. m -Phenylenediammonium as a New Spacer for Dion–Jacobson Two-Dimensional Perovskites

23. Physical properties of bulk, defective, 2D and 0D metal halide perovskite semiconductors from a symmetry perspective

24. Structural Isomer of Fluorinated Ruddlesden-Popper Perovskites Toward Efficient and Stable 2D/3D Perovskite Solar Cells

25. Ordered Mixed-Spacer 2D Bromide Perovskites and the Dual Role of 1,2,4-Triazolium Cation

26. 2D multilayered perovskites and 2D/3D bilayers for stable solar cells

27. Ultrafast relaxation of lattice distortion in two-dimensional perovskites

28. High-phase purity two-dimensional perovskites with 17.3% efficiency enabled by interface engineering of hole transport layer

Catalog

Searchworks

Select search scope, currently: Articles Catalog books, media & more in Jio Institute collections Articles journal articles & other e-resources

Search

Search Constraints

Refine your results

Search Limiters

Topic

Publication Year Range

Language

Journal

Database

Publisher

28 results on '"European Project: PeroCUBE"'

Search Results

Catalog

Select search scope, currently: Articles

Catalog

books, media & more in Jio Institute collections

Articles

journal articles & other e-resources