@article{10a84ad458264bf29d0d2f0a37432d79,
title = "Ultrafast relaxation of lattice distortion in two-dimensional perovskites",
abstract = "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.",
author = "Hao Zhang and Wenbin Li and Joseph Essman and Claudio Quarti and Isaac Metcalf and Chiang, \{Wei Yi\} and Siraj Sidhik and Jin Hou and Austin Fehr and Andrew Attar and Lin, \{Ming Fu\} and Alexander Britz and Xiaozhe Shen and Stephan Link and Xijie Wang and Uwe Bergmann and Kanatzidis, \{Mercouri G.\} and Claudine Katan and Jacky Even and Blancon, \{Jean Christophe\} and Mohite, \{Aditya D.\}",
note = "The work at Rice University was supported by the DOE-EERE 0008843 program. W.L. acknowledges the National Science Foundation Graduate Research Fellowship Program. This material is based on work supported by the National Science Foundation Graduate Research Fellowship Program under grant no. NSF 20-587. Any opinions, findings and conclusions or recommendations expressed in this material are those of the author and do not necessarily reflect the views of the National Science Foundation. J.H. acknowledges financial support from the China Scholarships Council (no. 202107990007). J. Even acknowledges financial support from the Institut Universitaire de France. Work at Northwestern University was supported by the Office of Naval Research (ONR) under grant N00014-20-1-2725. Part of the work at ISCR and Institut FOTON was funded by the European Union{\textquoteright}s Horizon 2020 research and innovation program under grant agreement no.861985 (PeroCUBE) and by the Agence Nationale pour la Recherche (MORELESS project). For DFT calculations, this work was granted access to the HPCresources of TGCC under the allocation 2020-A0090907682 made by GENCI. MeV-UED is operated as part of the Linac Coherent Light Source at the SLAC National Accelerator Laboratory, supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. S.L. thanks the Robert A. Welch Foundation for support through the Charles W. Duncan, Jr.-Welch Chair in Chemistry (C-0002), and acknowledges financial support from the US Department of Energy, Office of Science, Basic Energy Sciences, CPIMS program, under award no. DE-339SC0016534 (W.-Y.C). The work at Rice University was supported by the DOE-EERE 0008843 program. W.L. acknowledges the National Science Foundation Graduate Research Fellowship Program. This material is based on work supported by the National Science Foundation Graduate Research Fellowship Program under grant no. NSF 20-587. Any opinions, findings and conclusions or recommendations expressed in this material are those of the author and do not necessarily reflect the views of the National Science Foundation. J.H. acknowledges financial support from the China Scholarships Council (no. 202107990007). J. Even acknowledges financial support from the Institut Universitaire de France. Work at Northwestern University was supported by the Office of Naval Research (ONR) under grant N00014-20-1-2725. Part of the work at ISCR and Institut FOTON was funded by the European Union{\textquoteright}s Horizon 2020 research and innovation program under grant agreement no.861985 (PeroCUBE) and by the Agence Nationale pour la Recherche (MORELESS project). For DFT calculations, this work was granted access to the HPCresources of TGCC under the allocation 2020-A0090907682 made by GENCI. MeV-UED is operated as part of the Linac Coherent Light Source at the SLAC National Accelerator Laboratory, supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. S.L. thanks the Robert A. Welch Foundation for support through the Charles W. Duncan, Jr.-Welch Chair in Chemistry (C-0002), and acknowledges financial support from the US Department of Energy, Office of Science, Basic Energy Sciences, CPIMS program, under award no. DE-339SC0016534 (W.-Y.C).",
year = "2023",
month = apr,
doi = "10.1038/s41567-022-01903-6",
language = "English (US)",
volume = "19",
pages = "545--550",
journal = "Nature Physics",
issn = "1745-2473",
publisher = "Nature Research",
number = "4",
}