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Ultrafast relaxation of lattice distortion in two-dimensional perovskites

Journal Article · · Nature Physics
 [1];  [2];  [2];  [3];  [2];  [2];  [2];  [2];  [2];  [4];  [4];  [4];  [4];  [2];  [4];  [5];  [6];  [7];  [7];  [2] more »;  [2] « less
  1. Rice University, Houston, TX (United States); SLAC
  2. Rice University, Houston, TX (United States)
  3. University of Rennes (France); University of Mons (Belgium)
  4. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
  5. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE); University of Wisconsin, Madison, WI (United States)
  6. Northwestern University, Evanston, IL (United States)
  7. University of Rennes (France)

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. Then 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.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC); USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation; China Scholarships Council; Institut Universitaire de France; Office of Naval Research (ONR); European Union’s Horizon 2020; Agence Nationale pour la Recherche; Robert A. Welch Foundation
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1971217
Journal Information:
Nature Physics, Journal Name: Nature Physics Journal Issue: 4 Vol. 19; ISSN 1745-2473
Publisher:
Nature Publishing Group (NPG)Copyright Statement
Country of Publication:
United States
Language:
English

References (44)

Direct Observation of Bandgap Oscillations Induced by Optical Phonons in Hybrid Lead Iodide Perovskites journal April 2020
Tailored Engineering of an Unusual (C 4 H 9 NH 3 ) 2 (CH 3 NH 3 ) 2 Pb 3 Br 10 Two-Dimensional Multilayered Perovskite Ferroelectric for a High-Performance Photodetector journal September 2017
Vibrational Response of Methylammonium Lead Iodide: From Cation Dynamics to Phonon-Phonon Interactions journal September 2016
The calculation of the vibrational frequencies of crystalline compounds and its implementation in the CRYSTAL code: Crystalline Compounds and the CRYSTAL Code journal March 2004
Quantum-mechanical condensed matter simulations with CRYSTAL
  • Dovesi, Roberto; Erba, Alessandro; Orlando, Roberto
  • Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 8, Issue 4 https://doi.org/10.1002/wcms.1360
journal March 2018
Ruddlesden–Popper Hybrid Lead Iodide Perovskite 2D Homologous Semiconductors journal April 2016
Layer-Dependent Coherent Acoustic Phonons in Two-Dimensional Ruddlesden–Popper Perovskite Crystals journal August 2019
Dynamic Structural Response and Deformations of Monolayer MoS 2 Visualized by Femtosecond Electron Diffraction journal September 2015
Concept of Lattice Mismatch and Emergence of Surface States in Two-dimensional Hybrid Perovskite Quantum Wells journal August 2018
Rashba and Dresselhaus Effects in Hybrid Organic–Inorganic Perovskites: From Basics to Devices journal September 2015
Electron–Phonon Scattering in Atomically Thin 2D Perovskites journal October 2016
Real-Time Observation of Exciton–Phonon Coupling Dynamics in Self-Assembled Hybrid Perovskite Quantum Wells journal October 2017
Tuning Hot Carrier Cooling Dynamics by Dielectric Confinement in Two-Dimensional Hybrid Perovskite Crystals journal October 2019
Direct Observation of Electron–Phonon Coupling and Slow Vibrational Relaxation in Organic–Inorganic Hybrid Perovskites journal October 2016
Broadband Emission in Two-Dimensional Hybrid Perovskites: The Role of Structural Deformation journal December 2016
Hybrid Dion–Jacobson 2D Lead Iodide Perovskites journal February 2018
Carrier Relaxation and Lattice Heating Dynamics in Silicon Revealed by Femtosecond Electron Diffraction journal December 2006
High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells journal July 2016
Perovskite energy funnels for efficient light-emitting diodes journal June 2016
Observation of a hot-phonon bottleneck in lead-iodide perovskites journal October 2015
The dark exciton ground state promotes photon-pair emission in individual perovskite nanocrystals journal November 2020
Electron–phonon interaction in efficient perovskite blue emitters journal May 2018
Phonon coherences reveal the polaronic character of excitons in two-dimensional lead halide perovskites journal January 2019
Semiconductor physics of organic–inorganic 2D halide perovskites journal December 2020
Stable room-temperature continuous-wave lasing in quasi-2D perovskite films journal September 2020
Molecular disorder and translation/rotation coupling in the plastic crystal phase of hybrid perovskites journal January 2016
Structural origins of broadband emission from layered Pb–Br hybrid perovskites journal January 2017
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu journal April 2010
Observation of enhanced hot phonon bottleneck effect in 2D perovskites journal April 2018
Vibrational relaxation dynamics in layered perovskite quantum wells journal June 2021
Special points for Brillouin-zone integrations journal June 1976
Theory of transient excitonic optical nonlinearities in semiconductor quantum-well structures journal November 1985
Time dependence of the laser-induced femtosecond lattice instability of Si and GaAs: Role of longitudinal optical distortions journal March 1994
Picosecond strain pulses generated by a supersonically expanding electron-hole plasma in GaAs journal October 2012
Phonon-phonon interactions in photoexcited graphite studied by ultrafast electron diffraction journal March 2016
Ultrafast Dynamics of Charge Density Waves in 4 H b − TaSe 2 Probed by Femtosecond Electron Diffraction journal October 2012
Ultrafast Relaxation Dynamics of the Antiferrodistortive Phase in Ca Doped SrTiO 3 journal August 2018
Ultrafast Suppression of the Ferroelectric Instability in KTaO3 journal September 2022
Generalized Gradient Approximation Made Simple journal October 1996
Transient Strain Driven by a Dense Electron-Hole Plasma journal October 2003
Exciton-polaron spectral structures in two-dimensional hybrid lead-halide perovskites journal June 2018
Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites journal July 2017
Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites journal March 2017
Room-temperature excitonic nonlinear-optical effects in semiconductor quantum-well structures journal July 1985

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