Phonon-driven intra-exciton Rabi oscillations in CsPbBr3 halide perovskites

Xuan Trung Nguyen, Katrin Winte, Daniel Timmer, Yevgeny Rakita, Davide Raffaele Ceratti, Sigalit Aharon, Muhammad Sufyan Ramzan, Caterina Cocchi, Michael Lorke, Frank Jahnke, David Cahen, Christoph Lienau, Antonietta De Sio

Research output: Contribution to journalArticlepeer-review

7 Scopus citations

Abstract

Coupling electromagnetic radiation with matter, e.g., by resonant light fields in external optical cavities, is highly promising for tailoring the optoelectronic properties of functional materials on the nanoscale. Here, we demonstrate that even internal fields induced by coherent lattice motions can be used to control the transient excitonic optical response in CsPbBr3 halide perovskite crystals. Upon resonant photoexcitation, two-dimensional electronic spectroscopy reveals an excitonic peak structure oscillating persistently with a 100-fs period for up to ~2 ps which does not match the frequency of any phonon modes of the crystals. Only at later times, beyond 2 ps, two low-frequency phonons of the lead-bromide lattice dominate the dynamics. We rationalize these findings by an unusual exciton-phonon coupling inducing off-resonant 100-fs Rabi oscillations between 1s and 2p excitons driven by the low-frequency phonons. As such, prevailing models for the electron-phonon coupling in halide perovskites are insufficient to explain these results. We propose the coupling of characteristic low-frequency phonon fields to intra-excitonic transitions in halide perovskites as the key to control the anharmonic response of these materials in order to establish new routes for enhancing their optoelectronic properties.

Original languageEnglish
Article number1047
JournalNature Communications
Volume14
Issue number1
DOIs
StatePublished - 24 Feb 2023
Externally publishedYes

Bibliographical note

Publisher Copyright:
© 2023, The Author(s).

Funding

Financial support by the Ministry of Science and Culture (MWK) of the State of Lower Saxony and the Volkswagen Foundation (“Niedersächsisches Vorab—Research Cooperation Lower Saxony-Israel”, “Niedersächsisches Vorab—SMART”, “Professorinnen für Niedersachsen”, “DyNano”), and by the Deutsche Forschungsgemeinschaft (DE 3578/3-1/Li 580/16-1, and SPP1839, SPP1840, SPP2196, GRK1885, SFB1372) is gratefully acknowledged. C.C. acknowledges additional funding from the German Federal Ministry of Education and Research (Professorinnenprogramm III). D.R.C. acknowledges funding from the European Union’s Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement No. 893194. Computational resources for the simulations were provided by the HPC cluster CARL of the Carl von Ossietzky University Oldenburg funded by the DFG (Project No. INST 184/157-1 FUGG) and by the MWK.

FundersFunder number
Ministry of Science and Culture
Horizon 2020 Framework Programme
H2020 Marie Skłodowska-Curie Actions893194
Carl von Ossietzky Universität Oldenburg
Deutsche ForschungsgemeinschaftSPP1840, DE 3578/3-1/Li 580/16-1, SPP1839, SPP2196, GRK1885, INST 184/157-1 FUGG, SFB1372
Volkswagen Foundation
Bundesministerium für Bildung und Forschung
Ministerium für Wissenschaft, Forschung und Kunst Baden-Württemberg

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