Discovery of enhanced lattice dynamics in a single-layered hybrid perovskite

Zhang, Zhuquan; Zhang, Jiahao; Liu, Zi-Jie; Dahod, Nabeel S.; Paritmongkol, Watcharaphol; Brown, Niamh; Stollmann, Alexia; Lee, Woo Seok; Chien, Yu-Che; Dai, Zhenbang; Nelson, Keith A.; Tisdale, William A.; Rappe, Andrew M.; Baldini, Edoardo

doi:10.1126/sciadv.adg4417

Title: Discovery of enhanced lattice dynamics in a single-layered hybrid perovskite

Journal Article · 16 August 2023 · Science Advances

DOI: https://doi.org/10.1126/sciadv.adg4417 · OSTI ID:2471951

^[1];

^[2]; Liu, Zi-Jie ^[3]; Dahod, Nabeel S. ^[3];

^[3]; Brown, Niamh ^[3];

^[3];

^[3]; Chien, Yu-Che ^[3]; Dai, Zhenbang ^[2];

^[3];

^[2];

^[4]

Massachusetts Institute of Technology (MIT), Cambridge, MA (United States); OSTI
University of Pennsylvania, Philadelphia, PA (United States)
Massachusetts Institute of Technology (MIT), Cambridge, MA (United States)
University of Texas, Austin, TX (United States)

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.

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Research Organization:: Massachusetts Institute of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: National Science Foundation (NSF); Robert A. Welch Foundation; US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019126; SC0019345

OSTI ID:: 2471951

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 33 Vol. 9; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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