Dara P. S. McCutcheon

Quantum dot Rabi rotations beyond the weak exciton–phonon coupling regime

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 in the case of 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 because, unlike the polaron approach, the weak-coupling theory is incapable of capturing multiphonon effects, while it also does not properly account for phonon-induced renormalization of the driving frequency. In particular, we find that the weak-coupling theory often overestimates the damping rate when compared to 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.

A general approach to quantum dynamics using a variational master equation: Application to phonon-damped Rabi rotations in quantum dots

We develop a versatile master equation approach to describe the nonequilibrium dynamics of a two-level system in contact with a bosonic environment, which allows for the exploration of a wide range of parameter regimes within a single formalism. As an experimentally relevant example, we apply this technique to the study of excitonic Rabi rotations in a driven quantum dot, and compare its predictions to the numerical Feynman integral approach. We find excellent agreement between the two methods across a generally difficult range of parameters. In particular, the variational master equation technique captures effects usually considered to be nonperturbative, such as multiphonon processes and bath-induced driving renormalization, and can give reliable results even in regimes in which previous master equation approaches fail.

Consistent treatment of coherent and incoherent energy transfer dynamics using a variational master equation

We investigate the energy transfer dynamics in a donor-acceptor model by developing a time-local master equation technique based on a variational transformation of the underlying Hamiltonian. The variational transformation allows a minimisation of the Hamiltonian perturbation term dependent on the system parameters, and consequently results in a versatile master equation valid over a range of system-bath coupling strengths, temperatures, and environmental spectral densities. While our formalism reduces to the well-known Redfield, Förster and polaron forms in the appropriate limits, in general it is not equivalent to perturbing in either the system-environment or donor-acceptor coupling strengths, and hence can provide reliable results between these limits as well. Moreover, we show how to include the effects of both environmental correlations and non-equilibrium preparations within the formalism.

Coherent and incoherent dynamics in excitonic energy transfer: Correlated fluctuations and off-resonance effects

We study the nature of the energy transfer process within a pair of coupled two-level systems (donor and acceptor) subject to interactions with the surrounding environment. Going beyond a standard weak-coupling approach, we derive a master equation within the polaron representation that allows for the investigation of both weak and strong system-bath couplings, as well as reliable interpolation between these two limits. With this theory, we are then able to explore both coherent and incoherent regimes of energy transfer within the donor-acceptor pair. We elucidate how the degree of correlation in the donor and acceptor fluctuations, the donor-acceptor energymismatch, and the range of the environment frequency distribution impact upon the energy transfer dynamics. In the resonant case (no energy mismatch) we describe in detail how a crossover from coherent to incoherent transfer dynamics occurs with increasing temperature [A. Nazir, Phys. Rev. Lett. 103, 146404 (2009)], and we also explore how fluctuation correlations are able to protect coherence in the energy transfer process. We show that a strict crossover criterion is harder to define when off-resonance, though we find qualitatively similar population dynamics to the resonant case with increasing temperature, while the amplitude of coherent population oscillations also becomes suppressed with growing site energy mismatch.

Model of the optical emission of a driven semiconductor quantum dot: phonon-enhanced coherent scattering and off-resonant sideband narrowing

We study the crucial role played by the solid-state environment in determining the photon emission characteristics of a driven quantum dot. For resonant driving, we predict a phonon enhancement of the coherently emitted radiation field with increasing driving strength, in stark contrast to the conventional expectation of a rapidly decreasing fraction of coherent emission with stronger driving. This surprising behavior results from thermalization of the dot with respect to the phonon bath and leads to a nonstandard regime of resonance fluorescence in which significant coherent scattering and the Mollow triplet coexist. Off resonance, we show that despite the phonon influence, narrowing of dot spectral sideband widths can occur in certain regimes, consistent with an experimental trend.

Temperature-dependent Mollow triplet spectra from a single quantum dot : Rabi frequency renormalization and sideband linewidth insensitivity

We investigate temperature-dependent resonance fluorescence spectra obtained from a single self-assembled quantum dot. A decrease of the Mollow triplet sideband splitting is observed with increasing temperature, an effect we attribute to a phonon-induced renormalization of the driven dot Rabi frequency. We also present first evidence for a nonperturbative regime of phonon coupling, in which the expected linear increase in sideband linewidth as a function of temperature is canceled by the corresponding reduction in Rabi frequency. These results indicate that dephasing in semiconductor quantum dots may be less sensitive to changes in temperature than expected from a standard weak-coupling analysis of phonon effects.

Long-lived spin entanglement induced by a spatially correlated thermal bath

We investigate how two spatially separated qubits coupled to a common heat bath can be entangled by purely dissipative dynamics. We identify a dynamical time scale associated with the lifetime of the dissipatively generated entanglement and show that it can be much longer than either the typical single-qubit decoherence time or the time scale on which a direct exchange interaction can entangle the qubits. We give an approximate analytical expression for the long-time evolution of the qubit concurrence and propose an ion trap scheme in which such dynamics should be observable.

Phonon scattering inhibits simultaneous near-unity efficiency and indistinguishability in semiconductor single-photon sources

Semiconductor quantum dots have recently emerged as a leading platform to efficiently generate highly indistinguishable photons [1-3], and this work addresses the timely question of how good these solid-state sources can ultimately be. Based on a microscopic theory, we establish the crucial impact that lattice relaxation has in these systems, which gives rise to a broad phonon sideband in bulk quantum dot emission spectra, as seen in Fig. (1) a. We show how both the indistinguishability and efficiency of a single photon source based on such a quantum dot in a modified photonic environment depends on the way in which this incoherent sideband is removed from the spectra [4].

Ground state and dynamics of the biased dissipative two-state system: Beyond variational polaron theory

We propose a ground-state ansatz for the Ohmic spin-boson model that improves upon the variational treatment of Silbey and Harris for biased systems in the scaling limit. In particular, it correctly captures the smooth crossover behavior expected for the ground-state magnetization when moving between the delocalized and localized regimes of the model, a feature that the variational treatment is unable to properly reproduce, while it also provides a lower ground-state energy estimate in the crossover region. We further demonstrate the validity of our intuitive ground-state by showing that it leads to predictions in excellent agreement with those derived from a nonperturbative Bethe-ansatz technique. Finally, recasting our ansatz in the form of a generalized polaron transformation, we are able to explore the dissipative two-state dynamics beyond weak system-environment coupling within an efficient time-local master equation formalism.

Two-photon interference from a quantum dot microcavity: Persistent pure dephasing and suppression of time jitter

We demonstrate the emission of highly indistinguishable photons from a quasi-resonantly pumped coupled quantum dot--microcavity system operating in the regime of cavity quantum electrodynamics. Changing the sample temperature allows us to vary the quantum dot--cavity detuning, and on spectral resonance we observe a three-fold improvement in the Hong--Ou--Mandel interference visibility, reaching values in excess of 80\%. Our measurements off-resonance allow us to investigate varying Purcell enhancements, and to probe the dephasing environment at different temperatures and energy scales. By comparison with our microscopic model, we are able to identify pure-dephasing and not time-jitter as the dominating source of imperfections in our system.