The vibrational photon echo measurement employs short pulses of coherent infrared radiation to discriminate among line broadening processes of different time scales. The measurement has been analyzed with the optical Bloch equations, in which the coupling of a quantum three-level system to a bath is represented by dephasing times. A detailed treatment of vibrational dynamics in a molecular liquid requires a Hamiltonian model. As such models are more readily treated in classical than in quantum mechanics, we consider the calculation of the vibrational echo in classical mechanics. Vibrational echoes are calculated for a solvated anharmonic oscillator. The classical mechanical echo is shown to share attributes of a quantum mechanical calculation.
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 CsPbI
3 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 CsPbI
3 nanocrystals. We analyze the statistical characteristics of PE via the second-order correlation function
g(2)(0) and the characteristic function for different combinations of the areas of the excitation pulses. Our results show that
g(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)=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.