Ultrafast relaxation of lattice distortion in two-dimensional perovskites
- Rice University, Houston, TX (United States); SLAC
- Rice University, Houston, TX (United States)
- University of Rennes (France); University of Mons (Belgium)
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- 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)
- Northwestern University, Evanston, IL (United States)
- 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