Perfect Chirality with Imperfect Polarization.

Unidirectional (chiral) emission of light from a circular dipole emitter into a waveguide is only possible at points of perfect circular polarization (C points), with elliptical polarizations yielding a lower directional contrast. However, there is no need to restrict engineered systems to circular dipoles, and with an appropriate choice of dipole unidirectional emission is possible for any elliptical polarization. Using elliptical dipoles, rather than circular, typically increases the size of the area suitable for chiral interactions (in an exemplary mode by a factor ∼30), while simultaneously increasing coupling efficiencies. We propose illustrative schemes to engineer the necessary elliptical transitions in both atomic systems and quantum dots.

Phonon-Induced Optical Dephasing in Single Organic Molecules.

We present a joint experiment-theory analysis of the temperature-dependent emission spectra, zero-phonon linewidth, and second-order correlation function of light emitted from a single organic molecule. We observe spectra with a zero-phonon line together with several additional sharp peaks, broad phonon sidebands, and a strongly temperature dependent homogeneous broadening. Our model includes both localized vibrational modes of the molecule and a thermal phonon bath, which we include nonperturbatively, and is able to capture all observed features. For resonant driving we measure Rabi oscillations that become increasingly damped with temperature, which our model naturally reproduces. Our results constitute an essential characterization of the photon coherence of molecules, paving the way to their use in future quantum information applications.

Photon Statistics of Filtered Resonance Fluorescence.

Spectral filtering of resonance fluorescence is widely employed to improve single photon purity and indistinguishability by removing unwanted backgrounds. For filter bandwidths approaching the emitter linewidth, complex behavior is predicted due to preferential transmission of components with differing photon statistics. We probe this regime using a Purcell-enhanced quantum dot in both weak and strong excitation limits, finding excellent agreement with an extended sensor theory model. By changing only the filter width, the photon statistics can be transformed between antibunched, bunched, or Poissonian. Our results verify that strong antibunching and a subnatural linewidth cannot simultaneously be observed, providing new insight into the nature of coherent scattering.

Light Scattering from Solid-State Quantum Emitters: Beyond the Atomic Picture.

Coherent scattering of light by a single quantum emitter is a fundamental process at the heart of many proposed quantum technologies. Unlike atomic systems, solid-state emitters couple to their host lattice by phonons. Using a quantum dot in an optical nanocavity, we resolve these interactions in both time and frequency domains, going beyond the atomic picture to develop a comprehensive model of light scattering from solid-state emitters. We find that even in the presence of a low-Q cavity with high Purcell enhancement, phonon coupling leads to a sideband that is completely insensitive to excitation conditions and to a nonmonotonic relationship between laser detuning and coherent fraction, both of which are major deviations from atomlike behavior.

Probing Electron-Phonon Interaction through Two-Photon Interference in Resonantly Driven Semiconductor Quantum Dots.

We investigate the temperature dependence of photon coherence properties through two-photon interference (TPI) measurements from a single quantum dot (QD) under resonant excitation. We show that the loss of indistinguishability is related only to the electron-phonon coupling and is not affected by spectral diffusion. Through these measurements and a complementary microscopic theory, we identify two independent separate decoherence processes, both of which are associated with phonons. Below 10 K, we find that the relaxation of the vibrational lattice is the dominant contribution to the loss of TPI visibility. This process is non-Markovian in nature and corresponds to real phonon transitions resulting in a broad phonon sideband in the QD emission spectra. Above 10 K, virtual phonon transitions to higher lying excited states in the QD become the dominant dephasing mechanism, this leads to a broadening of the zero phonon line, and a corresponding rapid decay in the visibility. The microscopic theory we develop provides analytic expressions for the dephasing rates for both virtual phonon scattering and non-Markovian lattice relaxation.

A broadband tapered nanocavity for efficient nonclassical light emission.

We present the design of a tapered nanocavity, obtained by sandwiching a photonic wire section between a planar gold reflector and a few-period Bragg mirror integrated into the tapered wire. Thanks to its ultrasmall mode volume (0.71 λ3/n3), this hybrid nanocavity largely enhances the spontaneous emission rate of an embedded quantum dot (Purcell factor: 6), while offering a wide operation bandwidth (full-width half-maximum: 20 nm). In addition, the top tapered section shapes the cavity far-field emission into a very directive output beam, with a Gaussian spatial profile. For realistic taper dimensions, a total outcoupling efficiency to a Gaussian beam of 0.8 is predicted. Envisioned applications include bright sources of non-classical states of light, such as widely tunable sources of indistinguishable single photons and polarization-entangled photon pairs.

Error distributions on large entangled states with non-Markovian dynamics.

We investigate the distribution of errors on a computationally useful entangled state generated via the repeated emission from an emitter undergoing strongly non-Markovian evolution. For emitter-environment coupling of pure-dephasing form, we show that the probability that a particular patten of errors occurs has a bound of Markovian form, and thus, accuracy threshold theorems based on Markovian models should be just as effective. Beyond the pure-dephasing assumption, though complicated error structures can arise, they can still be qualitatively bounded by a Markovian error model.

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.

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.

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.

Vibrational enhancement of quadrature squeezing and phase sensitivity in resonance fluorescence.

Vibrational environments are commonly considered to be detrimental to the optical emission properties of solid-state and molecular systems, limiting their performance within quantum information protocols. Given that such environments arise naturally it is important to ask whether they can instead be turned to our advantage. Here we show that vibrational interactions can be harnessed within resonance fluorescence to generate optical states with a higher degree of quadrature squeezing than in isolated atomic systems. Considering the example of a driven quantum dot coupled to phonons, we demonstrate that it is feasible to surpass the maximum level of squeezing theoretically obtainable in an isolated atomic system and indeed come close to saturating the fundamental upper bound on squeezing from a two-level emitter. We analyse the performance of these vibrationally-enhanced squeezed states in a phase estimation protocol, finding that for the same photon flux, they can outperform the single mode squeezed vacuum state.

Modelling exciton-phonon interactions in optically driven quantum dots.

We provide a self-contained review of master equation approaches to modelling phonon effects in optically driven self-assembled quantum dots. Coupling of the (quasi) two-level excitonic system to phonons leads to dissipation and dephasing, the rates of which depend on the excitation conditions, intrinsic properties of the QD sample, and its temperature. We describe several techniques, which include weak-coupling master equations that are perturbative in the exciton-phonon coupling, as well as those based on the polaron transformation that can remain valid for strong phonon interactions. We additionally consider the role of phonons in altering the optical emission characteristics of quantum dot devices, outlining how we must modify standard quantum optics treatments to account for the presence of the solid-state environment.