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Physical review. B./Physical review. B

Photon echo from free excitons in a CH3NH3PbI3 halide perovskite single crystal

Roman S. Nazarov, I. A. Solovev, Aleksei O. Murzin, N. I. Selivanov, Jacky Even, Alexei V. Emeline, Yury V. Kapitonov

Published Jun 13, 2022• 16 citations
Publisher

Abstract

Halide perovskites show great potential for a variety of optoelectronic applications. The presence of robust exciton resonance in these materials makes them promising for use in information photonics. In this paper, we demonstrate the possibility of writing and delayed reading of the optical coherence in halide perovskite by the spontaneous (two-pulse) photon echo in ${\mathrm{MAPbI}}_{3}$ (${\mathrm{MA}}^{+}$ = ${\mathrm{CH}}_{3}{\mathrm{NH}}_{3}^{+}$) lead-halide perovskite single crystal on picosecond time scales. The spectral and polarimetric measurements of the photon echo signal confirm the free excitonic origin of the excitation under study. Observed relatively long dephasing time, high exciton oscillator strength, and weakly pronounced excitation-induced dephasing make halide perovskites a promising media for applications.

DOI
10.1103/physrevb.105.245202

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Feb 9, 2006•0 citations
Halide perovskites show great potential for a variety of optoelectronic applications. The presence of robust exciton resonance in these materials makes them promising for use in information photonics. In this paper, we demonstrate the possibility of writing and delayed reading of the optical coherence in halide perovskite by the spontaneous (two-pulse) photon echo in MAPbI3{\mathrm{MAPbI}}_{3}MAPbI3​ (MA+{\mathrm{MA}}^{+}MA+ = CH3NH3+{\mathrm{CH}}_{3}{\mathrm{NH}}_{3}^{+}CH3​NH3+​) lead-halide perovskite single crystal on picosecond time scales. The spectral and polarimetric measurements of the photon echo signal confirm the free excitonic origin of the excitation under study. Observed relatively long dephasing time, high exciton oscillator strength, and weakly pronounced excitation-induced dephasing make halide perovskites a promising media for applications.
Photon echo (PE) spectroscopy is a powerful technique for probing decoherence mechanisms and charge carrier dynamics in semiconductor systems. Beyond traditional coherence measurements, characterizing the photon statistics of the echo signal is important for assessing its potential in quantum information applications and understanding the underlying quantum mechanical processes. Here, we study the photon statistics of PE signals generated by excitons in ensembles of lead halide perovskite CsPbI3_33​ nanocrystals at cryogenic temperature of 2 K using continuous-variable quantum state optical tomography based on homodyne detection. Pronounced Rabi oscillations of the PE amplitude allow us to evaluate the statistics for various pulse areas in the excitation sequence. The damping of the oscillations with increasing pulse area is attributed to spatial excitation inhomogeneity and excitation-induced dephasing. Despite the large ensemble of optically addressed excitons, the efficiency of generated PE signals is low which is attributed to the complex energy level structure of excitons and non-radiative recombination channels in CsPbI3_33​ nanocrystals. We analyze the statistical characteristics of PE via the second-order correlation function g(2)(0)g^{(2)}(0)g(2)(0) and the characteristic function for different combinations of the areas of the excitation pulses. Our results show that g(2)(0)=1g^{(2)}(0) = 1g(2)(0)=1, and the characteristic function of the PE signal corresponds to classical behavior. The formation of photon echoes as well as g(2)(0)=1g^{(2)}(0) = 1g(2)(0)=1 at the echo time is reproduced by a quantized free-space multimode model. Despite the relatively low efficiency, the photon echo exhibits a high degree of coherence and minimal classical noise, consistent with Poissonian statistics.
Long spin coherence times of carriers are essential for implementing quantum technologies using semiconductor devices for which, however, a possible obstacle is spin relaxation. For the spin dynamics, decisive features are the band structure, crystal symmetry, and quantum confinement. Perovskite semiconductors recently have come into focus of studies of their spin states, notivated by efficient optical access and potentially long-living coherence. Here, we report an electron spin coherence time T2T_2T2​ of the order of 1 ms, measured for a bulk FA0.95_{0.95}0.95​Cs0.05_{0.05}0.05​PbI3_33​ lead halide perovskite crystal. Using periodic laser pulses, we synchronize the electron spin Larmor precession about an external magnetic field in an inhomogeneous ensemble, the effect known as spin mode locking. It appears as a decay of the optically created ensemble spin polarization within the dephasing time T2∗T_2^*T2∗​ of up to 20 ns and its revival during the spin coherence time T2T_2T2​ reaching the millisecond range. This exceptionally long spin coherence time in a bulk crystal is complemented by millisecond-long longitudinal spin relaxation times T1T_1T1​ for electrons and holes, measured by optically-detected magnetic resonance. These long-lasting spin dynamics highlight perovskites as promising platform for the quantum devices with all-optical control.
Time-resolved demonstration of picosecond photon echoes due to intrinsic optical excitations of a semiconductor is presented. Phase relaxation times up to several hundred picoseconds are found for excitons localized by chemical disorder in CdSx{\mathrm{CdS}}_{\mathrm{x}}CdSx​${\mathrm{Se}}_{1\mathrm{\ensuremath{-}}\mathrm{x}}$ mixed crystals. These long dephasing times are attributed to reduced scattering of the localized excitons as compared to free excitons. Dephasing is identified as due to energy relaxation of the excitons.
An overview on photon echo spectroscopy under resonant excitation of the exciton complexes in semiconductor nanostructures is presented. The use of four-wave-mixing technique with the pulsed excitation and heterodyne detection allowed us to measure the coherent response of the system with the picosecond time resolution. It is shown that, for resonant selective pulsed excitation of the localized exciton complexes, the coherent signal is represented by the photon echoes due to the inhomogeneous broadening of the optical transitions. In case of resonant excitation of the trions or donor-bound excitons, the Zeeman splitting of the resident electron ground state levels under the applied transverse magnetic field results in quantum beats of photon echo amplitude at the Larmor precession frequency. Application of magnetic field makes it possible to transfer coherently the optical excitation into the spin ensemble of the resident electrons and to observe a long-lived photon echo signal. The described technique can be used as a high-resolution spectroscopy of the energy splittings in the ground state of the system. Next, we consider the Rabi oscillations and their damping under excitation with intensive optical pulses for the excitons complexes with a different degree of localization. It is shown that damping of the echo signal with increase of the excitation pulse intensity is strongly manifested for excitons, while on trions and donor-bound excitons this effect is substantially weaker.
The coherent excitation of a Wannier-exciton system by a short resonant light pulse is described through a simple model that takes into account explicitly the phase-space-filling effects due to the fermion nature of the electrons and holes composing the excitons. This formalism can describe both coherent-transient experiments, such as photon echoes, and optical observations at time scales longer than dephasing, such as absorption saturation. At high excitation densities the optical response of hydrogenic excitons deviates significantly from the response of the two-level model used traditionally to describe resonant effects. This suggests that coherent-optical-transient experiments, such as photon echoes, may be used to probe exciton interactions due to their internal structure, in addition to the relaxation processes that they probe in traditional experimental arrangements.
Optical coherence time and nonlinear optical response of excitons localized to quantum dots in a GaAs/AlGaAs single quantum well are investigated by the three-pulse photon echo technique. At low temperature, the optical coherence time is estimated to be 1.8 ns from the decay curve of the photon echo signal. The decay profile for short time delay shows the strong dependence on the input pulse area of the third pulse. Rabi oscillations are also observed. The oscillations exhibit nonlinear behavior, which is affected by the pre-excited polarization. Such behavior can be qualitatively explained by the local field effect due to the exciton-exciton interaction between the excitons.