Discovery of enhanced lattice dynamics in a single-layered hybrid perovskite
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sciadv.adg4417.pdf
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Published version
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Author(s) • • • • • • • • •
Zhang, Zhuquan
Zhang, Jiahao
Liu, Zi-Jie
Dahod, Nabeel S
Paritmongkol, Watcharaphol
Brown, Niamh
Stollmann, Alexia
Lee, Woo Seok
Chien, Yu-Che
Dai, Zhenbang
Date Issued
August 16, 2023
Journal
Science Advances
Publisher
American Association for the Advancement of Science
Citation
Zhuquan Zhang et al. ,Discovery of enhanced lattice dynamics in a single-layered hybrid perovskite.Sci. Adv.9, eadg4417 (2023).
Version
Final published version
Abstract
Layered hybrid perovskites exhibit emergent physical properties and exceptional functional performances, but the coexistence of lattice order and structural disorder severely hinders our understanding of these materials. One unsolved problem regards how the lattice dynamics are affected by the dimensional engineering of the inorganic frameworks and their interaction with the molecular moieties. Here, we address this question by using a combination of spontaneous Raman scattering, terahertz spectroscopy, and molecular dynamics simulations. This approach reveals the structural dynamics in and out of equilibrium and provides unexpected observables that differentiate single- and double-layered perovskites. While no distinct vibrational coherence is observed in double-layered perovskites, an off-resonant terahertz pulse can drive a long-lived coherent phonon mode in the single-layered system. This difference highlights the dramatic change in the lattice environment as the dimension is reduced, and the findings pave the way for ultrafast structural engineering and high-speed optical modulators based on layered perovskites.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
Massachusetts Institute of Technology. Department of Chemical Engineering
Massachusetts Institute of Technology. Department of Materials Science and Engineering
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DOI of Published Version
10.1126/sciadv.adg4417