We describe a powerful and intuitive technique for modeling light-matter interactions in classical and quantum nanoplasmonics. Our approach uses a quasinormal mode expansion of the Green function within a metal nanoresonator of arbitrary shape, toget
her with a Dyson equation, to derive an expression for the spontaneous decay rate and far field propagator from dipole oscillators outside resonators. For a single quasinormal mode, at field positions outside the quasi-static coupling regime, we give a closed form solution for the Purcell factor and generalized effective mode volume. We augment this with an analytic expression for the divergent LDOS very near the metal surface, which allows us to derive a simple and highly accurate expression for the electric field outside the metal resonator at distances from a few nanometers to infinity. This intuitive formalism provides an enormous simplification over full numerical calculations and fixes several pending problems in quasinormal mode theory.
We present a theoretical study of the resonance fluorescence spectra of an optically driven quantum dot placed near a single metal nanoparticle. The metallic reservoir coupling is calculated for an 8-nm metal nanoparticle using a time-convolutionless
master equation approach where the exact photon reservoir function is included using Green function theory. By exciting the system coherently near the nanoparticle dipole mode, we show that the driven Mollow spectrum becomes highly asymmetric due to internal coupling effects with higher-order plasmons. We also highlight regimes of resonance squeezing and broadening as well as spectral reshaping through light propagation. Our master equation technique can be applied to any arbitrary material system, including lossy inhomogeneous structures, where mode expansion techniques are known to break down.
Charge-neutral excitons in semiconductor quantum dots have a small finite energy separation caused by the anisotropic exchange splitting. Coherent excitation of neutral excitons will generally excite both exciton components, unless the excitation is
parallel to one of the dipole axes. We present a polaron master equation model to describe two-exciton pumping using a coherent continuous wave pump field in the presence of a realistic anisotropic exchange splitting. We predict a five-peak incoherent spectrum, thus generalizing the Mollow triplet to become a Mollow quintuplet. We experimentally confirm such spectral quintuplets for In(Ga)As quantum dots and obtain very good agreement with theory.
We investigate pump-induced exciton inversion in a quantum-dot cavity system with continuous wave drive. Using a polaron-based master equation, we demonstrate excited-state populations above 0.9 for an InAs dot at a phonon bath temperature of 4K. In
an exciton-driven system, the dominant mechanism is incoherent excitation from the phonon bath. For cavity driving, the mechanism is phonon-mediated switching between ground- and excited-state branches of the ladder of photon states, as quantum trajectory simulations clearly show. The exciton inversion as a function of detuning is found to be qualitatively different for exciton and cavity driving, primarily due to cavity filtering. The master equation approach allows us to include important radiative and non-radiative decay processes on the zero phonon line, provides a clear underlying dynamic in terms of photon and phonon scattering, and admits simple analytical approximations that help to explain the physics.
We present a semiconductor master equation technique to study the input/output characteristics of coherent photon transport in a semiconductor waveguide-cavity system containing a single quantum dot. We use this approach to investigate the effects of
photon propagation and anharmonic cavity-QED for various dot-cavity interaction strengths, including weakly-coupled, intermediately-coupled, and strongly-coupled regimes. We demonstrate that for mean photon numbers much less than 0.1, the commonly adopted weak excitation (single quantum) approximation breaks down, even in the weak coupling regime. As a measure of the anharmonic multiphoton-correlations, we compute the Fano factor and the correlation error associated with making a semiclassical approximation. We also explore the role of electron--acoustic-phonon scattering and find that phonon-mediated scattering plays a qualitatively important role on the light propagation characteristics. As an application of the theory, we simulate a conditional phase gate at a phonon bath temperature of $20 $K in the strong coupling regime.
We present an off-resonant excitation scheme that realizes pronounced stationary inversion in a two level system. The created inversion exploits a cavity-assisted two photon resonance to enhance the multi-photon regime of nonlinear cavity QED and sur
vives even in a semiconductor environment, where the cavity decay rate is comparable to the cavity-dot coupling rate. Exciton populations of greater than 0.75 are obtained in the presence of realistic decay and pure dephasing. Quantum trajectory simulations and quantum master equation calculations help elucidate the underlying physics and delineate the limitations of a simplified rate equation model. Experimental signatures of inversion and multi-photon cavity QED are predicted in the fluorescence intensity and second-order correlation function measured as a function of drive power.
We present a medium-dependent quantum optics approach to describe the influence of electron-acoustic phonon coupling on the emission spectra of a strongly coupled quantum-dot cavity system. Using a canonical Hamiltonian for light quantization and a p
hoton Green function formalism, phonons are included to all orders through the dot polarizability function obtained within the independent Boson model. We derive simple user-friendly analytical expressions for the linear quantum light spectrum, including the influence from both exciton and cavity-emission decay channels. In the regime of semiconductor cavity-QED, we study cavity emission for various exciton-cavity detunings and demonstrate rich spectral asymmetries as well as cavity-mode suppression and enhancement effects. Our technique is nonperturbative, and non-Markovian, and can be applied to study photon emission from a wide range of semiconductor quantum dot structures, including waveguides and coupled cavity arrays. We compare our theory directly to recent and apparently puzzling experimental data for a single site-controlled quantum dot in a photonic crystal cavity and show good agreement as a function of cavity-dot detuning and as a function of temperature.
