Anharmonic Exciton‐Phonon Coupling in Metal‐Organic Chalcogenides Hybrid Quantum Wells

Kastl, Christoph; Bonfà, Pietro; Maserati, Lorenzo

doi:10.1002/adom.202202213

Anharmonic Exciton‐Phonon Coupling in Metal‐Organic Chalcogenides Hybrid Quantum Wells

Journal Article · Wed Jan 25 00:00:00 EST 2023 · Advanced Optical Materials

DOI:https://doi.org/10.1002/adom.202202213· OSTI ID:1922123

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The Molecular Foundry Lawrence Berkeley National Laboratory Berkeley California 94720 USA, Walter Schottky Institute and Physik Department Technical University of Munich 85748 Garching Germany
Dipartimento di Scienze Matematiche, Fisiche e Informatiche Universitá di Parma Parma 43124 Italy, Centro S3 CNR‐Istituto Nanoscienze via Campi 213/A Modena I‐41125 Italy
The Molecular Foundry Lawrence Berkeley National Laboratory Berkeley California 94720 USA, Center for Nano Science and Technology @PoliMi Istituto Italiano di Tecnologia Milan 20133 Italy, Dipartimento di Fisica e Astronomia Università di Bologna Viale Berti‐Pichat 6/2 Bologna 40127 Italy

Abstract

In contrast to inorganic quantum wells, hybrid quantum wells (HQWs) based on metal‐organic semiconductors are characterized by relatively soft lattices, in which excitonic states can strongly couple to lattice phonons. Therefore, understanding the lattice's impact on exciton dynamics is essential for harnessing the optoelectronic potential of HQWs. Beyond 2D metal halide perovskites, layered metal‐organic chalcogenides (MOCs), which are an air‐stable, underexplored material class hosting room‐temperature excitons, can be exploited as photodetectors, light emitting devices, and ultrafast photoswitches. Here, the role of phonons in the optical transitions of the prototypical MOC [AgSePh] _∞ is elucidated. Impulsive stimulated Raman scattering (ISRS) allows the detection of coherent exciton oscillations driven by Fröhlich interaction with low‐energy optical phonons. Steady state absorption and Raman spectroscopies reveal a strong exciton‐phonon coupling (Huang‐Rhys parameter ≈1.7) and its anharmonicity, manifested as a nontrivial temperature‐dependent Stokes shift. The ab initio calculations support these observations, hinting at an anharmonic behavior of the low‐energy phonons <200 cm ⁻¹ . These results untangle complex exciton‐phonon interactions in MOCs, establishing an ideal testbed for room‐temperature many‐body phenomena.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: German Research Foundation (DFG); Italian SuperComputing Resource Allocation (ISCRA); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1922123

Alternate ID(s):: OSTI ID: 1922124
OSTI ID: 2242437

Journal Information:: Advanced Optical Materials, Journal Name: Advanced Optical Materials Journal Issue: 7 Vol. 11; ISSN 2195-1071

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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36 MATERIALS SCIENCE
Fröhlich interaction
Raman spectroscopy
anharmonic lattice vibrations
exciton-phonon coupling
hybrid quantum wells
metal-organic chalcogenides
transient absorption

Anharmonic Exciton‐Phonon Coupling in Metal‐Organic Chalcogenides Hybrid Quantum Wells

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