Spin-dependent exciton-exciton interactions in a mixed lead halide perovskite crystal
arxiv(2024)
摘要
We investigate the two-pulse photon echo response of excitons in the mixed
lead halide perovskite crystal in dependence on the excitation
intensity and polarization of the incident laser pulses. Using spectrally
narrow picosecond laser pulses, we address localized excitons with long
coherence times T_2 ≈ 100ps. This approach offers high sensitivity
for the observation of excitation-induced changes in the homogeneous linewidth
Γ_2=2ħ/T_2 on the μeV scale. Through intensity-dependent
measurements, we evaluate the increase of Γ_2 by 10 μeV at an
exciton density of 10^17 cm^-3 being comparable with the intrinsic
linewidth of 14μeV. We observe that the decay of the photon echo and its
power dependence are sensitive to the polarization configuration of the
excitation pulses, which indicates that spin-dependent exciton-exciton
interactions contribute to excitation-induced dephasing. In cross-linear
polarization, the decay is faster and its dependence on exciton density is
stronger as compared to the co-polarized configuration. Using a two-exciton
model accounting for different spin configurations we are able to reproduce the
experimental results.
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