Acoustic Phonon Sideband Dynamics During Polaron Formation in a Single Quantum Dot

Abstract

When an electron-hole pair is optically excited in a semiconductor quantum dot the host crystal lattice needs to adapt to the presence of the generated charge distribution. Therefore the coupled exciton-phonon system has to establish a new equilibrium, which is reached in the form of a quasiparticle called polaron. Especially, when the exciton is abruptly generated on a timescale faster than the typical lattice dynamics, the lattice displacement cannot follow adiabatically. Consequently, a rich dynamics on the picosecond timescale of the coupled system is expected. In this study we combine simulations and measurements of the ultrafast, coherent, nonlinear optical response, obtained by four-wave mixing spectroscopy, to resolve the formation of this polaron. By detecting and investigating the phonon sidebands in the four-wave mixing spectra for varying pulse delays and different temperatures we have access to the influence of phonon emission and absorption processes which finally result in the emission of an acoustic wave packet out from the quantum dot.

arXiv commentaccepted in Optics Letters

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• Fundamentals of heterodyne wave mixing spectroscopy: a tutorial
• An Exact Expression for Multidimensional Spectroscopy of a Spin-Boson Hamiltonian
• Entropy Dynamics of Phonon Quantum States Generated by Optical Excitation of a Two-Level System
• Spin dynamics of positively charged excitons in Cr${}^{+}$-doped quantum dots probed by resonant photoluminescence
• Probing Complex Decoherence Processes in Materials for Quantum Applications
• Suppression and amplification of phonon sidebands in transition metal dichalcogenides by optical feedback
• Phonon-induced Markovian and non-Markovian effects on absorption spectra of moiré excitons in twisted transition metal dichalcogenide bilayers