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 and Antonietta De Sio ()
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Xuan Trung Nguyen: Institut für Physik, Carl von Ossietzky Universität
Katrin Winte: Institut für Physik, Carl von Ossietzky Universität
Daniel Timmer: Institut für Physik, Carl von Ossietzky Universität
Yevgeny Rakita: Weizmann Institute of Science
Davide Raffaele Ceratti: Weizmann Institute of Science
Sigalit Aharon: Weizmann Institute of Science
Muhammad Sufyan Ramzan: Institut für Physik, Carl von Ossietzky Universität
Caterina Cocchi: Institut für Physik, Carl von Ossietzky Universität
Michael Lorke: Institut für Theoretische Physik, Universität Bremen
Frank Jahnke: Institut für Theoretische Physik, Universität Bremen
David Cahen: Weizmann Institute of Science
Christoph Lienau: Institut für Physik, Carl von Ossietzky Universität
Antonietta De Sio: Institut für Physik, Carl von Ossietzky Universität

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-36654-2

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