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Perovskite solar cells (PSCs) are the most promising technology for advancing current photovoltaic performance. However, the main challenge for their practical deployment and commercialization is their operational stability, affected by solar illumination and heating, as well as the electric field that is generated in the PV device by light exposure. Here, we propose a transparent multispectral photonic electrode placed on top of the glass substrate of solar cells, which simultaneously reduces the device solar heating and enhances its efficiency. Specifically, the proposed photonic electrode, composed of a low-resistivity metal and a conductive layer, simultaneously serves as a highly-efficient infrared filter and an ultra-thin transparent front contact, decreasing devices' solar heating and operating temperature. At the same time, it simultaneously serves as an anti-reflection coating, enhancing the efficiency. We additionally enhance the device cooling by coating the front glass substrate side with a visibly transparent film (PDMS), which maximizes substrate's thermal radiation. To determine the potential of our photonic approach and fully explore the cooling potential of PSCs, we first provide experimental characterizations of the absorption properties (in both visible and infrared wavelengths) of state-of-the-art PSCs among the most promising ones regarding the efficiency, stability, and cost. We then numerically show that applying our approach to promising PSCs can result in lower operating temperatures by over 9.0 oC and an absolute efficiency increase higher than 1.3%. These results are insensitive to varying environmental conditions. Our approach is simple and only requires modification of the substrate; it therefore points to a feasible photonic approach for advancing current photovoltaic performance with next-generation solar cell materials., Comment: 20 pages, 9 figures

Ultrathin, solution-processed emerging solar cells with high power-per-weight (PPW) outputs demonstrate unique potential for applications where low weight, high power output, and flexibility are indispensable. The following perspective explores the literature of emerging PVs and highlights the maximum reported PPW values of Perovskite Solar Cells (PSCs) 29.4 W/g, Organic Solar Cells (OSCs) 32.07 W/g and Quantum Dot Solar Cells (QDSC) 15.02 W/g, respectively. The record PPW values of OSCs and PSCs are approximately one order of magnitude higher compared to their inorganic ultrathin solar cells counterparts (approx. 3.2 W/g for CIGS and a-Si). This consists emerging PVs, very attractive for a variety of applications where the PPW is the key parameter. In particular, both OSCs and PSCs can be implemented in different scenarios of applications (indoor and biocompatible applications for OSCs and outdoor and high-energy radiation conversion conditions for the PSCs) due to their unique optoelectronic and physiochemical properties. Finally, our theoretical optical and electrical simulation and optimization study for the most promising and well-suited PV technologies, showed an impressive maximum realistic theoretical PPW limit of 74.3 and 93.7 W/g for PSCs and OSCs, respectively. Our finding shows that the literature PSCs and OSCs towards high PPW outputs, is not quite close to the theoretical maximum and thus more work needs to be done to further increase the PPW output of these promising PV technologies., Comment: 41 pages, 20 figues

Metal halide perovskites (MHPs) have shown an incredible rise in efficiency, reaching as high as 25.7%, which now competes with traditional photovoltaic technologies. Herein, we excluded CsX and RbX, the most commonly used cations to stabilize FAPbI3, from the bulk of perovskite thin films and applied them on the surface, as passivation agents. Extensive device optimization led to a power conversion efficiency (PCE) of 24.1% with a high fill factor (FF) of 82.2% upon passivation with CsI. We investigated in-depth the effect of CsI passivation on structural and optoelectronic properties using X-ray diffraction (XRD), angle resolved X-ray photoelectron spectroscopy (ARXPS), Kelvin Probe Force (KPFM) microscopy, time-resolved photoluminescence (TRPL), photoluminescence quantum yield (PLQY) and electroabsorption spectroscopy (TREAS). Furthermore, passivated devices exhibit enhanced operational stability, with optimized passivation with CsI leading to a retention of ~90% of initial PCE under 1 Sun illumination with maximum power point tracking for 600 h., Comment: 27 pages, 19 figures

The photocurrent density-voltage (J(V)) curve is the fundamental characteristic to assess opto-electronic devices, in particular solar cells. However, it only yields information on the performance integrated over the entire active device area. Here, a method to determine a spatially resolved photocurrent image by voltage-dependent photoluminescence microscopy is derived from basic principles. The opportunities and limitations of the approach are studied by the investigation of III-V and perovskite solar cells. This approach allows the real-time assessment of the microscopically resolved local J(V) curve, the steady-state Jsc, as well as transient effects. In addition, the measurement contains information on local charge extraction and interfacial recombination. This facilitates the identification of regions of non-ideal charge extraction in the solar cells and enables to link these to the processing conditions. The proposed technique highlights that, combined with potentiostatic measurements, luminescence microscopy turns out to be a powerful tool for the assessment of performance losses and the improvement of solar cells.

Two-dimensional (2D) halide perovskites feature a versatile structure, which not only enables the fine-tuning of their optoelectronic properties but also makes them appealing as model systems to investigate the fundamental properties of hybrid perovskites. In this study, we analyzed the changes in the optical absorption of 2D Dion-Jacobson mixed halide perovskite thin films (encapsulated) based on (PDMA)Pb(I0.5Br0.5)4 (PDMA: 1,4-phenylenedimethanammonium spacer) exposed to a constant illumination. We demonstrate that these 2D mixed-halide perovskites undergo photo de-mixing with direct transformation from the pristine phase to the de-mixed phases. Almost complete re-mixing of these phases occurs when the sample is left in the dark, showing that the process is reversible in terms of optical properties. On the other hand, exposure to light appears to induce structural changes in the thin film that are not reversible in the dark. We have further investigated temperature-dependent absorption measurements under light to extract the photo de-mixed compositions and to map the photo-miscibility-gap. This work thereby reveals that photo de-mixing occurs in Dion-Jacobson two-dimensional hybrid perovskites and provides strategies to address the role of light in the thermodynamic properties of these materials.

In the ongoing intense quest to increase the photoconversion efficiencies of lead halide perovskites, it has become evident that optimizing the morphology of the material is essential to achieve high peformance. Despite the fact that nucleation plays a key role in controlling the crystal morphology, very little is known about the nucleation and crystal growth processes. Here, we perform metadynamics simulations of nucleation of methylammonium lead triiodide (MAPI) in order to unravel the atomistic details of perovskite crystallization from a $\gamma$-butyrolactone solution. The metadynamics trajectories show that the nucleation process takes place in several stages. Initially, dense amorphous clusters mainly consisting of lead and iodide appear from the homogeneous solution. These clusters evolve into lead iodide (PbI$_{2}$) like structures. Subsequently, methylammonium (MA$^{+}$) ions diffuse into this PbI$_{2}$-like aggregates triggering the transformation into a perovskite crystal through a solid-solid transformation. Demonstrating the crucial role of the monovalent cations in crystallization, our simulations provide key insights into the evolution of the perovskite microstructure which is essential to make high-quality perovskite based solar cells and optoelectronics.

Organic-inorganic lead halide perovskites containing a mixture of iodide and bromide anions consistently perform better in donor-acceptor heterojunction solar cells than the standard methylammonium lead triiodide material. This observation is counterintuitive, as it is generally expected for photovoltaic materials that heterogeneities and compositional disorder cause reduced carrier diffusion length and conversion efficiency. Here, we combine ultrafast photoinduced electroabsorption and broadband fluorescence up-conversion spectroscopy measurements to scrutinize the carrier dynamics in mixed-cations, mixed-halide lead perovskite thin films. Our results evidence the formation of charge transfer excitons (CTE) across the boundaries of domains of various halide compositions. A global analysis of photoinduced transient Stark signals shows that CTE evolve gradually from Br-rich to I-rich domains over tens to hundreds of picoseconds. Rather than constituting recombination centres, boundaries between domains of various halide compositions appear then to favour charge carrier separation by driving photogenerated holes along channels of decreasing bromide content., Comment: 10 pages, 9 figures

Propionitrile electrolyte solutions mixed with sulfolane or with 1-ethyl 3-methyl imidazolium tetracyanoborate (ionic liquid) are optimized for Co(bpy)3+/Co(bpy)2+-mediated DSCs working at low illumination intensity.

Novel highly active, optically-transparent electrode catalyst containing Pt, PtOx, graphene oxide and stacked graphene platelet nanofibers is developed for a cathode of Cu(II/I)-mediated dye-sensitized solar cells.

Three Cu(II/I)-phenanthroline and Cu(II/I)-bipyridine redox mediators are studied on various electrodes and in variety of electrolyte solutions using cyclic voltammetry and impedance spectroscopy on symmetrical dummy cells.

Wave packet propagation succeeding electron transfer (ET) from alizarin dye molecules into the nanocrystalline TiO2 semiconductor has been studied by ultrafast transient absorption spectroscopy. Due to the ultrafast time scale of the ET reaction of about 6 fs the system shows substantial differences to molecular ET systems. We show that the ET process is not mediated by molecular vibrations and therefore classical ET theories lose their applicability. Here the ET reaction itself prepares a vibrational wave packet and not the electromagnetic excitation by the laser pulse. Furthermore, the generation of phonons during polaron formation in the TiO2 lattice is observed in real time for this system. The presented investigations enable an unambiguous assignment of the involved photoinduced mechanisms and can contribute to a corresponding extension of molecular ET theories to ultrafast ET systems like alizarin/TiO2., Comment: This work was supported by the German Research Foundation (DFG) (Hu 1006/6-1, WA 1850/6-1) and European Union projects FDML-Raman (FP7 ERC StG, contract no. 259158) and ENCOMOLE-2i (Horizon 2020, ERC CoG no. 646669)

We performed ab initio simulations aimed at identifying the atomistic and electronic structure origin of the high valence and conduction band, and band gap tunability of halide perovskites. We found that the two key ingredients are the overlap between bivalent cation and halide atomic orbitals, and the electronic charge of the bottom of the conduction band (CBM) state on the Sn or Pb atoms. In particular, we found that lower gaps are associated to higher negative antibonding overlap, and higher CBM charge on the bivalent cation. Both overlap and CBM charge on Sn/Pb can be tuned by the chemical nature of halide, bi and monovalent cation, as well as the symmetry of crystal structure. On the basis of our results we provide some practical rules to tune the valence band maximum, conduction band minimum, and band gap in this class of materials., Comment: 13 pages, 9 figures - contains SI

Electrochemical oxidation of hematite ({\alpha}-Fe2O3) nano-particulate films at 600 mV vs. Ag+/AgCl reference in KOH electrolyte forms a species at the hematite surface which causes a new transition in the upper Hubbard band between the Fe(3d)-O(2p) state region and the Fe(4sp)-O(2p) region, as evidenced by oxygen near edge x-ray absorption fine structure (NEXAFS) spectra. The electrochemical origin of this transition suggests that it is related with a surface state. This transition, not known for pristine {\alpha}-Fe2O3 is at about the same x-ray energy, where pristine 1% Si doped Si:Fe2O3 has such transition. Occurrence of this state coincides with the onset of an oxidative dark current wave at around 535 mV - a potential range, where the tunneling exchange current has been previously reported to increase by three orders of magnitude with the valence band and the transfer coefficient by a factor of 10. Oxidation to only 200 mV does not form such extra NEXAFS feature, supporting that a critical electrochemical potential between 200 and 600 mV is necessary to change the electronic structure of the iron oxide at the surface. Decrease of the surface roughness, as suggested by visual inspection, profilometry and x-ray reflectivity, points to faceting as potential structural origin of the surface state.