Research output: Contribution to journal › Article › peer-review
Photon Echo Polarimetry of Excitons and Biexcitons in a CH3NH3PbI3Perovskite Single Crystal. / Trifonov, Artur V.; Grisard, Stefan; Kosarev, Alexander N.; Akimov, Ilya A.; Yakovlev, Dmitri R.; Höcker, Julian; Dyakonov, Vladimir; Bayer, Manfred.
In: ACS Photonics, Vol. 9, No. 2, 16.02.2022, p. 621-629.Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Photon Echo Polarimetry of Excitons and Biexcitons in a CH3NH3PbI3Perovskite Single Crystal
AU - Trifonov, Artur V.
AU - Grisard, Stefan
AU - Kosarev, Alexander N.
AU - Akimov, Ilya A.
AU - Yakovlev, Dmitri R.
AU - Höcker, Julian
AU - Dyakonov, Vladimir
AU - Bayer, Manfred
N1 - Publisher Copyright: ©
PY - 2022/2/16
Y1 - 2022/2/16
N2 - Lead halide perovskites show remarkable performance when used in photovoltaic and optoelectronic devices. However, the peculiarities of light-matter interactions in these materials in general are far from being fully explored experimentally and theoretically. Herein, we specifically address the energy level order of optical transitions and demonstrate photon echoes in a methylammonium lead triiodide single crystal, thereby determining the optical coherence times (T2) for excitons and biexcitons at cryogenic temperature to be 0.79 and 0.67 ps, respectively. Most importantly, we have developed an experimental photon-echo polarimetry method that not only identifies the contributions from exciton and biexciton complexes but also allows accurate determination of the biexciton binding energy of 2.4 meV, even though the period of quantum beats between excitons and biexcitons is much longer than the coherence times of the resonances. Our experimental and theoretical analysis methods contribute to the understanding of the complex mechanism of quasiparticle interactions at moderate pump density and show that even in high-quality perovskite crystals and at very low temperatures, inhomogeneous broadening of excitonic transitions due to local crystal potential fluctuations is a source of optical dephasing.
AB - Lead halide perovskites show remarkable performance when used in photovoltaic and optoelectronic devices. However, the peculiarities of light-matter interactions in these materials in general are far from being fully explored experimentally and theoretically. Herein, we specifically address the energy level order of optical transitions and demonstrate photon echoes in a methylammonium lead triiodide single crystal, thereby determining the optical coherence times (T2) for excitons and biexcitons at cryogenic temperature to be 0.79 and 0.67 ps, respectively. Most importantly, we have developed an experimental photon-echo polarimetry method that not only identifies the contributions from exciton and biexciton complexes but also allows accurate determination of the biexciton binding energy of 2.4 meV, even though the period of quantum beats between excitons and biexcitons is much longer than the coherence times of the resonances. Our experimental and theoretical analysis methods contribute to the understanding of the complex mechanism of quasiparticle interactions at moderate pump density and show that even in high-quality perovskite crystals and at very low temperatures, inhomogeneous broadening of excitonic transitions due to local crystal potential fluctuations is a source of optical dephasing.
KW - biexciton binding energy
KW - exciton coherence time
KW - lead halide perovskite crystals
KW - photon echo spectroscopy
KW - quantum beat spectroscopy
UR - http://www.scopus.com/inward/record.url?scp=85124585885&partnerID=8YFLogxK
U2 - 10.1021/acsphotonics.1c01603
DO - 10.1021/acsphotonics.1c01603
M3 - Article
AN - SCOPUS:85124585885
VL - 9
SP - 621
EP - 629
JO - ACS Photonics
JF - ACS Photonics
SN - 2330-4022
IS - 2
ER -
ID: 96949587