Coherent band-edge oscillations and dynamic longitudinal-optical phonon mode splitting as evidence for polarons in perovskites

Liu, Z.; Vaswani, C.; Luo, L.; Cheng, D.; Yang, X.; Zhao, X.; Yao, Y.; Song, Z.; Brenes, R.; Kim, R. J.  H.; Jean, J.; Bulović, V.; Yan, Y.; Ho, K.-M.; Wang, J.

doi:10.1103/PhysRevB.101.115125

Title: Coherent band-edge oscillations and dynamic longitudinal-optical phonon mode splitting as evidence for polarons in perovskites

Journal Article · Mon Mar 16 00:00:00 EDT 2020 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.101.115125· OSTI ID:1607928

Liu, Z. ^[1]; Vaswani, C. ^[1]; Luo, L. ^[1]; Cheng, D. ^[1]; Yang, X. ^[1]; Zhao, X. ^[1]; Yao, Y. ^[1]; Song, Z. ^[2]; Brenes, R. ^[3]; Kim, R. J. H. ^[1]; Jean, J. ^[3]; Bulović, V. ^[3]; Yan, Y. ^[2]; Ho, K.-M. ^[1];

^[1]

Ames Lab., and Iowa State Univ., Ames, IA (United States)
Univ. of Toledo, OH (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

The coherence of collective modes, such as phonons and polarons, and their modulation of electronic states is long sought in complex systems, which is a crosscutting issue in photovoltaics and quantum electronics. In photovoltaic cells and lasers based on metal halide perovskites, the presence of polarons, i.e., photocarriers dressed by the macroscopic motion of charged lattice, assisted by terahertz (THz) longitudinal-optical (LO) phonons, has been intensely studied yet is still debated. This may be key for explaining the remarkable properties of the perovskite materials, e.g., defect tolerance, long charge lifetimes, and diffusion lengths. In this work we use the intense single-cycle THz pulse with peak electric field up to $E_{THz} = 1000$ kV/cm to drive coherent polaronic band-edge oscillations at room temperature in CH₃NH₃PbI₃ (MAPbI₃). We reveal the oscillatory behavior is dominated by a specific quantized lattice vibration mode at $$ω$$_LO ~ 4 THz, which is both dipole and momentum forbidden. THz-driven coherent polaron dynamics exhibits distinguishing features: room temperature coherent oscillations at $ω_{LO}$ longer than 1 ps in both single crystals and thin films, mode-selective modulation of different band-edge states assisted by electron-phonon interaction, and dynamic mode splitting at low temperature due to entropy and anharmonicity of organic cations. Our results demonstrate intense THz-driven coherent band-edge modulation is a powerful probe of electron-lattice coupling phenomena and polaronic quantum control in perovskites.

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Research Organization:: Ames Laboratory (AMES), Ames, IA (United States); Iowa State Univ., Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF)

Grant/Contract Number:: AC02-07CH11358; DMR 1807818; 1122374; EECS 1611454

OSTI ID:: 1607928

Alternate ID(s):: OSTI ID: 1604859

Report Number(s):: IS-J-10184; PRBMDO; TRN: US2104999

Journal Information:: Physical Review B, Vol. 101, Issue 11; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 14 works

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Title: Coherent band-edge oscillations and dynamic longitudinal-optical phonon mode splitting as evidence for polarons in perovskites

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