Coherent spin dynamics of electrons and holes photogenerated with large kinetic energy in lead halide perovskite crystals

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Auteurs principaux: Zhukov, Evgeny A., Yakovlev, Dmitri R., Kirstein, Erik, Kopteva, Nataliia E., Hordiichuk, Oleh, Kovalenko, Maksym V., Bayer, Manfred
Format: Preprint
Publié: 2025
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author Zhukov, Evgeny A.
Yakovlev, Dmitri R.
Kirstein, Erik
Kopteva, Nataliia E.
Hordiichuk, Oleh
Kovalenko, Maksym V.
Bayer, Manfred
author_facet Zhukov, Evgeny A.
Yakovlev, Dmitri R.
Kirstein, Erik
Kopteva, Nataliia E.
Hordiichuk, Oleh
Kovalenko, Maksym V.
Bayer, Manfred
contents The coherent spin dynamics of electrons and holes are studied in a FA0.9Cs0.1PbI2.8Br0.2 perovskite bulk crystal, using time-resolved Kerr ellipticity in a two-color pump-probe scheme. The probe photon energy is tuned to the exciton resonance, while the pump photon energy is detuned from it up to 0.75 eV to higher energies. The spin-oriented electrons and holes photogenerated with significant excess kinetic energy relax into states in vicinity of the band gap, where they undergo Larmor precession in an external magnetic field. At cryogenic temperatures down to 1.6 K, the spin dephasing time reaches the nanosecond range. During energy relaxation, the carrier spin relaxation is inefficient and only happens when the carriers become localized. In experiments with two pump pulses, all-optical control of the amplitudes and phases of the electron and hole spin signals is achieved in the additive regime by varying the intensities of the pump pulses and the time delay between them.
format Preprint
id arxiv_https___arxiv_org_abs_2501_12159
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Coherent spin dynamics of electrons and holes photogenerated with large kinetic energy in lead halide perovskite crystals
Zhukov, Evgeny A.
Yakovlev, Dmitri R.
Kirstein, Erik
Kopteva, Nataliia E.
Hordiichuk, Oleh
Kovalenko, Maksym V.
Bayer, Manfred
Mesoscale and Nanoscale Physics
The coherent spin dynamics of electrons and holes are studied in a FA0.9Cs0.1PbI2.8Br0.2 perovskite bulk crystal, using time-resolved Kerr ellipticity in a two-color pump-probe scheme. The probe photon energy is tuned to the exciton resonance, while the pump photon energy is detuned from it up to 0.75 eV to higher energies. The spin-oriented electrons and holes photogenerated with significant excess kinetic energy relax into states in vicinity of the band gap, where they undergo Larmor precession in an external magnetic field. At cryogenic temperatures down to 1.6 K, the spin dephasing time reaches the nanosecond range. During energy relaxation, the carrier spin relaxation is inefficient and only happens when the carriers become localized. In experiments with two pump pulses, all-optical control of the amplitudes and phases of the electron and hole spin signals is achieved in the additive regime by varying the intensities of the pump pulses and the time delay between them.
title Coherent spin dynamics of electrons and holes photogenerated with large kinetic energy in lead halide perovskite crystals
topic Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2501.12159