We study optically driven Rabi rotations of a quantum dot exciton transition between 5 and 50 K, and for pulse areas of up to 14π. In a high driving field regime, the decay of the Rabi rotations is nonmonotonic, and the period decreases with pulse area and increases with temperature. By comparing the experiments to a weak-coupling model of the exciton-phonon interaction, we demonstrate that the observed renormalization of the Rabi frequency is induced by fluctuations in the bath of longitudinal acoustic phonons, an effect that is a phonon analogy of the Lamb shift.
We study the excitonic dynamics of a driven quantum dot under the influence of a phonon environment, going beyond the weak exciton-phonon coupling approximation. By combining the polaron transform and time-local projection operator techniques we develop a master equation that can be valid over a much larger range of exciton-phonon coupling strengths and temperatures than the standard weak-coupling approach. For the experimentally relevant parameters considered here, we find that the weak-coupling and polaron theories give very similar predictions for low temperatures (below 30 K), while at higher temperatures we begin to see discrepancies between the two. This is due to the fact that, unlike the polaron approach, the weak-coupling theory is incapable of capturing multiphonon effects, while it also does not properly account for phonon-induced renormalisation of the driving frequency. In particular, we find that the weak-coupling theory often overestimates the damping rate when compared to that predicted by the polaron theory. Finally, we extend our theory to include non-Markovian effects and find that, for the parameters considered here, they have little bearing on the excitonic Rabi rotations when plotted as a function of pulse area.
Quantum systems are invariably open, evolving under surrounding influences rather than in isolation. Standard open quantum system methods eliminate all information on the environmental state to yield a tractable description of the system dynamics. By incorporating a collective coordinate of the environment into the system Hamiltonian, we circumvent this limitation. Our theory provides straightforward access to important environmental properties that would otherwise be obscured, allowing us to quantify the evolving system-environment correlations. As a direct result, we show that the generation of robust system-environment correlations that persist into equilibrium (heralded also by the emergence of non-Gaussian environmental states) renders the canonical system steady-state almost always incorrect. The resulting equilibrium states deviate markedly from those predicted by standard perturbative techniques and are instead fully characterised by thermal states of the mapped system-collective coordinate Hamiltonian. We outline how noncanonical system states could be investigated experimentally to study deviations from canonical thermodynamics, with direct relevance to molecular and solid-state nanosystems.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.