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3. Rare-Earth Molecular Crystals with Ultra-narrow Optical Linewidths for Photonic Quantum Technologies

Author

Serrano, Diana, Kumar, Kuppusamy Senthil, Heinrich, Benoît, Fuhr, Olaf, Hunger, David, Ruben, Mario, and Goldner, Philippe

Subjects
Physics - Optics, Condensed Matter - Materials Science, Quantum Physics
Abstract

Rare-earth ions are promising solid state systems to build light-matter interfaces at the quantum level. This relies on their potential to show narrow optical homogeneous linewidths or, equivalently, long-lived optical quantum states. In this letter, we report on europium molecular crystals that exhibit linewidths in the 10s of kHz range, orders of magnitude narrower than other molecular centers. We harness this property to demonstrate efficient optical spin initialization, coherent storage of light using an atomic frequency comb, and optical control of ion-ion interactions towards implementation of quantum gates. These results illustrate the utility of rare-earth molecular crystals as a new platform for photonic quantum technologies that combines highly coherent emitters with the unmatched versatility in composition, structure, and integration capability of molecular materials.

Published
2021
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4. Molecule-based coherent light-spin interfaces for quantum information processing -- optical spin state polarization in a binuclear Europium complex

Author

Kumar, Kuppusamy Senthil, Serrano, Diana, Nonat, Aline M., Heinrich, Benoît, Karmazin, Lydia, Charbonnière, Loïc J., Goldner, Philippe, and Ruben, Mario

Subjects
Quantum Physics, Condensed Matter - Mesoscale and Nanoscale Physics, Physics - Optics
Abstract

The success of the emerging field of solid-state optical quantum information processing (QIP) critically depends on the access to resonant optical materials. Rare-earth ions (REIs) are suitable candidates for QIP protocols due to their extraordinary photo-physical and magnetic quantum properties such as long optical and spin coherence lifetimes ($T_2$). However, molecules incorporating REIs, despite having advantageous properties such as atomically exact quantum tunability, inherent scalability, and large portability, have not yet been studied for QIP applications. As a first testimony of the usefulness of REI molecules for optical QIP applications, we demonstrate in this study that narrow spectral holes can be burned in the inhomogeneously broadened $^5$D$_0\to^7$F$_0$ optical transition of a binuclear Eu(III) complex, rendering a homogeneous linewidth ($\Gamma_h$) = 22 $\pm$ 1 MHz, which translates as $T_2 = 14.5$ $\pm$ 0.7 ns at 1.4 K. Moreover, long-lived spectral holes are observed, demonstrating efficient polarization of Eu(III) ground state nuclear spins, a fundamental requirement for all-optical spin initialization and addressing. These results elucidate the usefulness of REI-based molecular complexes as versatile coherent light-spin interfaces for applications in quantum communications and processing., Comment: 31 pages, 9 figures

Published
2020

5. Engineering on-surface spin crossover: spin-state switching in a self-assembled film of vacuum sublimable functional molecule

Author

Kumar, Kuppusamy Senthil, Studniarek, Michał, Heinrich, Benoît, Arabski, Jacek, Schmerber, Guy, Bowen, Martin, Boukari, Samy, Beaurepaire, Eric, Dreiser, Jan, and Ruben, Mario

Subjects
Physics - Applied Physics, Condensed Matter - Mesoscale and Nanoscale Physics
Abstract

Realization of spin crossover (SCO) based applications requires studying of spin state switching characteristics of SCO complex molecules at nanostructured environments especially on-surface. Except for a very few cases, the SCO of a surface bound thin molecular film is either quenched or heavily altered due to (i) strong molecule-surface interactions and (ii) differing intermolecular interactions in films relative to the bulk. By fabricating SCO complexes on a weakly interacting surface such as highly oriented pyrolytic graphite (HOPG) and copper nitride (CuN), the interfacial quenching problem has been tackled. However, engineering intermolecular interactions in thin SCO active films is rather difficult. This work proposes a molecular self-assembly strategy to fabricate thin spin switchable surface bound films with programmable intermolecular interactions. Molecular engineering of the parent complex system [Fe(H$_{2}$B(pz)$_{2}$)$_{2}$(bpy)] (pz = pyrazole, bpy = 2,2'-bipyridine) with a dodecyl (C$_{12}$) alkyl chain yielded a classical amphiphile-like functional and vacuum sublimable charge neutral Fe$^{\rm II}$ complex, [Fe(H$_{2}$B(pz)$_{2}$)$_{2}$(C$_{12}$-bpy)] (C$_{12}$-bpy = dodecyl[2,2'-bipyridine]-5-carboxylate). The bulk powder and 10 nm thin film, on quartz glass/SiO$_{\rm x}$ surface, of the complex showed comparable spin state switching characteristics mediated by similar lamellar bilayer like self-assembly/molecular interactions in both bulk and thin film states. This unprecedented observation augurs well for the development of SCO based applications, especially in molecular spintronics.

Published
2018

19. Grafting Electron‐Accepting Fragments on [4]cyclo‐2,7‐carbazole Scaffold: Tuning the Structural and Electronic Properties of Nanohoops

Author

Brouillac, Clément, primary, McIntosh, Nemo, additional, Heinrich, Benoît, additional, Jeannin, Olivier, additional, De Sagazan, Olivier, additional, Coulon, Nathalie, additional, Rault‐Berthelot, Joëlle, additional, Cornil, Jérôme, additional, Jacques, Emmanuel, additional, Quinton, Cassandre, additional, and Poriel, Cyril, additional

Published
2024
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22. Importance of the curvature in electronic, structural and charge transport properties: oligomers of N-pyridine carbazole.

Author

Brouillac, Clément, Serez, Ari, McIntosh, Nemo, Rault-Berthelot, Joëlle, Jeannin, Olivier, Heinrich, Benoît, Quinton, Cassandre, De Sagazan, Olivier, Jacques, Emmanuel, Cornil, Jérôme, and Poriel, Cyril

Abstract

The recent development of π-conjugated nanohoops in organic electronics has opened new perspectives for this family of curved materials. Addressing the difference arising from curved vs. non-curved materials is an important concern in order to highlight the specific properties of curved materials. Herein, we discuss the significant differences arising between [4]-cyclo-N-pyridine-2,7-carbazole [4]C-Py-Cbz and its linear counterpart, N-pyridine-2,7-tetracarbazole [4]L-Py-Cbz. This study gathers optical, electrochemical, structural, morphological and charge transport properties and highlights the key role played by the curvature. We notably show how the electronic effects of the pending pyridines differently affect the molecular orbitals energies. We have also shown how structural rearrangements between ground and first excited states can be at the origin of the peculiar emission of nanohoops. Finally, the huge difference in terms of charge transport properties was discussed. Nanohoop [4]C-Py-Cbz displays a field-effect mobility in the saturated regime μFEsat of 3.4 × 10-6 cm² V-1 s-1, six times higher than that of its linear analogue [4]L-Py-Cbz (5.7 × 10-7 cm² V-1 s-1). However, the detailed study of the charge transport properties shows that the linear analogue forms a semi-conducting layer with a lower trap density, more favourable to the charge hopping processes. Theoretical calculations have provided clues on the origin of these differences, revealing that despite the intensity of electronic couplings is significantly in favor of [4]L-Py-Cbz, their highly anisotropic character renders them more sensitive to defects and disorder. This is consistent with the fact that [4]C-Py-Cbz displays experimentally better charge transport properties than [4]L-Py-Cbz. Such a type of structure-property relationship study provides fundamental findings of interest for the future design of high-performance nanohoops. [ABSTRACT FROM AUTHOR]

Published
2024
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28. Side chains in organic conjugated materials, a key parameter

Author

Leclerc, Nicolas, Ibraikulov, Olzhas, Durand, Pablo, Zeng, Huiyan, Heinrich, Benoît, Heiser, Thomas, Lévêque, Patrick, Brinkmann, Martin, Méry, Stéphane, Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Laboratoire des sciences de l'ingénieur, de l'informatique et de l'imagerie (ICube), École Nationale du Génie de l'Eau et de l'Environnement de Strasbourg (ENGEES)-Université de Strasbourg (UNISTRA)-Institut National des Sciences Appliquées - Strasbourg (INSA Strasbourg), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Institut National de Recherche en Informatique et en Automatique (Inria)-Les Hôpitaux Universitaires de Strasbourg (HUS)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Sadron (ICS), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), and univOAK, Archive ouverte

Subjects
[SPI.MAT] Engineering Sciences [physics]/Materials, [SPI.MAT]Engineering Sciences [physics]/Materials
Abstract

International audience

Published
2023

31. Artificial p–n‐like Junction Based on Pure 2D Organic–Inorganic Halide Perovskite Structure Having Naphthalene Diimide Acceptor Moieties

Author

Feng, Zhao, primary, Liu, Xuelong, additional, Imaoka, Kentaro, additional, Ishii, Tomohiro, additional, Tumen‐Ulzii, Ganbaatar, additional, Tang, Xun, additional, Harrington, George F., additional, Heinrich, Benoît, additional, Ribierre, Jean‐Charles, additional, Chamoreau, Lise‐Marie, additional, Sosa Vargas, Lydia, additional, Kreher, David, additional, Goushi, Kenichi, additional, Matsushima, Toshinori, additional, Zhou, Guijiang, additional, Mathevet, Fabrice, additional, and Adachi, Chihaya, additional

Published
2023
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45. How Halogenation Impacts the Polymer Backbone Conformation: Learning from Combination of Solid‐State MAS NMR and X‐Ray Scattering

Author

Olla, Théodore, primary, Jabbour, Ribal, additional, Labiod, Amina, additional, Boyron, Olivier, additional, Méry, Stéphane, additional, Heinrich, Benoît, additional, Heiser, Thomas, additional, Jacquemin, Denis, additional, Lévêque, Patrick, additional, Lesage, Anne, additional, and Leclerc, Nicolas, additional

Published
2022
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47. Spin-Crossover in Supramolecular Iron(II)-2,6-bis(1 H-Pyrazol-1-yl)pyridine Complexes: Toward Spin-State Switchable Single-Molecule Junctions

Author

Kuppusamy, Senthil Kumar (author), Mizuno, Asato (author), García-Fuente, Amador (author), van der Poel, S. (author), Heinrich, Benoît (author), Ferrer, Jaime (author), van der Zant, H.S.J. (author), Ruben, Mario (author), Kuppusamy, Senthil Kumar (author), Mizuno, Asato (author), García-Fuente, Amador (author), van der Poel, S. (author), Heinrich, Benoît (author), Ferrer, Jaime (author), van der Zant, H.S.J. (author), and Ruben, Mario (author)

Abstract

Spin-crossover (SCO) active iron(II) complexes are an integral class of switchable and bistable molecular materials. Spin-state switching properties of the SCO complexes have been studied in the bulk and single-molecule levels to progress toward fabricating molecule-based switching and memory elements. Supramolecular SCO complexes featuring anchoring groups for metallic electrodes, for example, gold (Au), are ideal candidates to study spin-state switching at the single-molecule level. In this study, we report on the spin-state switching characteristics of supramolecular iron(II) complexes 1 and 2 composed of functional 4-([2,2′-bithiophen]-5-ylethynyl)-2,6-di(1H-pyrazol-1-yl)pyridine (L1) and 4-(2-(5-(5-hexylthiophen-2-yl)thiophen-2-yl)ethynyl)-2,6-di(1H-pyrazol-1-yl)pyridine (L2) ligands, respectively. Density functional theory (DFT) studies revealed stretching-induced spin-state switching in a molecular junction composed of complex 1, taken as a representative example, and gold electrodes. Single-molecule conductance traces revealed the unfavorable orientation of the complexes in the junctions to demonstrate the spin-state dependence of the conductance., QN/van der Zant Lab

Published
2022
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48. Supporting Information - Spin-crossover in supramolecular iron(II)–2,6-bis(1H-pyrazol-1-yl)pyridine complexes: Toward spin-state switchable single-molecule junctions

Author

Kumar Kuppusamy, Senthil, Mizuto, Asano, García-Fuente, Amador, Poel, Sebastiaan van der, Heinrich, Benoît, Ferrer, Jaime, Zant, Herre S. J. van der, Ruben, Mario, Kumar Kuppusamy, Senthil, Mizuto, Asano, García-Fuente, Amador, Poel, Sebastiaan van der, Heinrich, Benoît, Ferrer, Jaime, Zant, Herre S. J. van der, and Ruben, Mario

Published
2022

49. Triphenylene-ethylammonium tetrachlorometallate salts: multicolumnar mesophases, thermochromism and Langmuir films

Author

Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Junta de Castilla y León, Centre National de la Recherche Scientifique (France), Université de Strasbourg, Barcenilla, María, Baena, María Jesús, Donnio, Bertrand, Heinrich, Benoît, Gutiérrez, Lucía, Coco, Silveiro, Espinet, Pablo, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Junta de Castilla y León, Centre National de la Recherche Scientifique (France), Université de Strasbourg, Barcenilla, María, Baena, María Jesús, Donnio, Bertrand, Heinrich, Benoît, Gutiérrez, Lucía, Coco, Silveiro, and Espinet, Pablo

Abstract

This study reports new mesomorphic benzylethylammonium salts containing a 2,3,6,7,10-pentakis(dodecyloxy)-11-(hexyloxy)triphenylene unit and Cl− or [MCl4]2− (M = Cu, Ni, Co, Mn) as counterions. They show a rich columnar polymesomorphism, characterized by polarized optical microscopy (POM), differential scanning calorimetry (DSC), and small- and wide-angle X-ray scattering (S/WAXS). All the compounds self-organize into multisegregated structures in the solid state and in the mesophases, with the alternation within large superlattices of triphenylene-containing columns and benzylammonium chloride or tetrachorometallate fragments. Interestingly, the nickel derivative displays a continuous and reversible thermochromic behavior in the range of 50–80 °C. Magnetic measurements and UV-Vis data at different temperatures, support changes in the coordination sphere of the Ni(II) atom from octahedral to tetrahedral. Furthermore, these systems form stable and homogeneous Langmuir films at the air–water interface. These films have been successfully transferred onto solid substrates giving rise to nanostructured LB films with a clearly defined bilayer structure in which each layer consists of molecular columns aligned along the surface.

Published
2022

50. Spin-crossover in supramolecular iron(II)–2,6-bis(1H-pyrazol-1-yl)pyridine complexes: Toward spin-state switchable single-molecule junctions

Author

German Research Foundation, Alexander von Humboldt Foundation, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), European Commission, Kumar Kuppusamy, Senthil, Mizuto, Asano, García-Fuente, Amador, Poel, Sebastiaan van der, Heinrich, Benoît, Ferrer, Jaime, Zant, Herre S. J. van der, Ruben, Mario, German Research Foundation, Alexander von Humboldt Foundation, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), European Commission, Kumar Kuppusamy, Senthil, Mizuto, Asano, García-Fuente, Amador, Poel, Sebastiaan van der, Heinrich, Benoît, Ferrer, Jaime, Zant, Herre S. J. van der, and Ruben, Mario

Abstract

Spin-crossover (SCO) active iron(II) complexes are an integral class of switchable and bistable molecular materials. Spin-state switching properties of the SCO complexes have been studied in the bulk and single-molecule levels to progress toward fabricating molecule-based switching and memory elements. Supramolecular SCO complexes featuring anchoring groups for metallic electrodes, for example, gold (Au), are ideal candidates to study spin-state switching at the single-molecule level. In this study, we report on the spin-state switching characteristics of supramolecular iron(II) complexes 1 and 2 composed of functional 4-([2,2′-bithiophen]-5-ylethynyl)-2,6-di(1H-pyrazol-1-yl)pyridine (L1) and 4-(2-(5-(5-hexylthiophen-2-yl)thiophen-2-yl)ethynyl)-2,6-di(1H-pyrazol-1-yl)pyridine (L2) ligands, respectively. Density functional theory (DFT) studies revealed stretching-induced spin-state switching in a molecular junction composed of complex 1, taken as a representative example, and gold electrodes. Single-molecule conductance traces revealed the unfavorable orientation of the complexes in the junctions to demonstrate the spin-state dependence of the conductance.

Published
2022

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