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Chris Gustin

Publications and source records attributed to Chris Gustin.

At least 19 recordsLinked to original sources

Quantum Optical Soliton Dynamics Beyond Linearization: An Open-System Approach

We introduce two approaches to modeling the quantum dynamics of optical $\chi^{(3)}$ solitons. Taking an open-system viewpoint, we project the underlying quantum field into system (soliton) and residual reservoir components. The reservoir is treated as either (i) a discrete ``Lanczos supermode'' (LSM) expansion which localizes dynamics to a few-supermode basis, or (ii) a non-local environment which can be traced out by deriving a Markovian master equation (ME). Using these methods, we analyze and identify the quantum structure of both the soliton's stability and its hierarchy of perturbations. Through numerical simulations, we confirm both methods effectively capture quantum-induced soliton phase shifts in a concise few-mode (single-mode for ME) basis, and the LSM approach also captures photon loss which arises from non-Markovian dispersive couplings. As neither method is limited to the linearized regime, our approaches provide powerful computational tools to analyze complex non-Gaussian quantum dynamics of solitons where other commonly-used methods fail, providing insight into such non-perturbative regimes. We also investigate radiation that occurs in the presence of higher-order dispersion with ultrashort pulses, deriving a ME that predicts photon loss consistent with classical theory, but find that both classical and ME theory dramatically underestimate the actual amount of dissipation, which we explain in terms of dispersive coupling-induced soliton broadening.

quant-ph

Dissipation in the Broadband and Ultrastrong Coupling Regimes of Cavity Quantum Electrodynamics: An Ab Initio Quantized Quasinormal Mode Approach

Phenomenological approaches to photon loss have long been the workhorse of cavity-QED, but prove inadequate in the presence of sufficiently broadband light-matter interactions. We present a rigorous and ab initio derivation of a quantum master equation for a quantized optical cavity mode coupled to a dipole, using a quasinormal mode (QNM) quantization procedure for plasmonic and dielectric open-system cavity-QED, which is valid in broadband light-matter interaction regimes, including ultrastrong coupling (USC). The theory supports general three-dimensional resonators with arbitrary dispersion and loss, and thus can be applied to a wide range of open cavities. Our ab initio and gauge-invariant approach fully recovers the recent result of Phys. Rev. Lett. 134, 123601 (2025) for the spectral density of a quantized cavity with a single dipole, exhibits a dissipative classical-quantum correspondence for bosonic Hopfield model systems, and reveals important departures from previous heuristic assumptions about system-bath coupling. We identify a new criterion for what we term the "broadband" dissipative regime of cavity-QED, where phenomenological models require corrections in accordance with the intrinsic and spatially-dependent complex phase of the QNM, and also shed light on fundamental limits to single-mode models in extreme coupling regimes. Using plasmonic and dielectric cavity examples, we show validity ranges of our QNM master equation and spectral USC calculations, and discuss prospects for near-term experimental observation of broadband dissipative effects.

quant-ph

Gauge invariance of the natural lineshape and dissipative dynamics of a two-level atom

The calculation of the natural lineshape of an excited two-level atom (TLA) has long been known to be gauge-dependent, with certain experiments in better agreement with the lineshape calculated with the dipole gauge. We show that by using a Coulomb gauge Hamiltonian truncated in a manner consistent with the gauge principle, the correct output spectrum can be obtained. For TLAs undergoing dynamics arising from additional Hamiltonian couplings, we also show that the master equation is gauge-invariant under the same conditions of validity as the Born-Markov approximation, despite different gauges having different spectral densities. These results highlight the importance of using correctly truncated gauge-invariant Hamiltonians in input-output theory for accurate frequency-dependent spectra, even in weak coupling regimes.

quant-ph

What is the spectral density of the reservoir for a lossy quantized cavity?

By considering a two-level system weakly coupled to a single lossy three-dimensional cavity mode, and using a quasinormal mode expansion for the photonic medium, we show that the frequency-dependence of the quantum coupling interaction between the cavity and its photonic reservoir can not be simply constructed to be independent of the cavity contents. For the single quantum dipole case, we identify the correct form of the local spectral density, revealing a surprising gauge-dependent $\sim \omega^{\pm 1} prefactor scaling, as well as a spatially-dependent correction. We thus establish the correct quantum form for the cavity-reservoir interaction, which so far has only been worked out rigorously for simple 1D geometries, and show its significant impact on broadband strong coupling.

quant-ph

Using system-reservoir methods to derive effective field theories for broadband nonlinear quantum optics: a case study on cascaded quadratic nonlinearities

In broadband quantum optical systems, nonlinear interactions among a large number of frequency components induce complex dynamics that may defy heuristic analysis. In this work we introduce a perturbative framework for factoring out reservoir degrees of freedom and establishing a concise effective model (effective field theory) for the remaining system. Our approach combines approximate diagonalization of judiciously partitioned subsystems with master equation techniques. We consider cascaded optical $χ^{(2)}$ (quadratic) nonlinearities as an example and show that the dynamics can be construed (to leading order) as self-phase modulations of dressed fundamental modes plus cross-phase modulations of dressed fundamental and second-harmonic modes. We then formally eliminate the second-harmonic degrees of freedom and identify emergent features of the fundamental wave dynamics, such as two-photon loss channels, and examine conditions for accuracy of the reduced model in dispersive and dissipative parameter regimes. Our results highlight the utility of system-reservoir methods for deriving accurate, intuitive reduced models for complex dynamics in broadband nonlinear quantum photonics.

quant-ph

Reconciling quantum and classical spectral theories of ultrastrong coupling: Role of cavity bath coupling and gauge corrections

Focusing on the widely adopted Hopfield model with cavity dissipation, we show how the linear spectrum of an ultrastrongly coupled cavity and a dipole can be described either classically or quantum mechanically, but only when the quantum model includes (i) corrections to maintain gauge invariance, and (ii) a specific type of cavity bath coupling. We also show the impact of this bath model on the quantum Rabi model, which has no classical analogue in ultrastrong coupling.

quant-ph

Dynamic resonance fluorescence in solid-state cavity quantum electrodynamics

The coherent interaction between a two-level system and electromagnetic fields serves as a foundation for fundamental quantum physics and modern photonic quantum technology. A profound example is resonance fluorescence, where the non-classical photon emission appears in the form of a Mollow-triplet when a two-level system is continuously driven by a resonant laser. Pushing resonance fluorescence from a static to dynamic regime by using short optical pulses generates on-demand emissions of highly coherent single photons. Further increasing the driving strength in the dynamical regime enables the pursuit of exotic non-classical light emission in photon number superposition, photon number entanglement, and photon bundle states. However, the long-sought-after spectrum beyond the Mollow-triplet, a characteristic of dynamic resonance fluorescence under strong driving strength, has not been observed yet. Here we report the direct observation and systematic investigations of dynamic resonance fluorescence spectra beyond the Mollow-triplet in a solid-state cavity quantum electrodynamic system. The dynamic resonance fluorescence spectra with up to five pairs of side peaks, excitation detuning induced spectral asymmetry, and cavity filtering effect are observed and quantitatively modeled by a full quantum model with phonon scattering included. Time-resolved measurements further reveal that the multiple side peaks originate from interference of the emission associated with different temporal positions of the excitation pulses. Our work facilitates the generation of a variety of exotic quantum states of light with dynamic driving of two-level systems.

quant-ph

Gauge-invariant theory of truncated quantum light-matter interactions in arbitrary media

The loss of gauge invariance in models of light-matter interaction which arises from material and photonic space truncation can pose significant challenges to conventional quantum optical models when matter and light strongly hybridize. In structured photonic environments, necessary in practice to achieve strong light-matter coupling, a rigorous model of field quantization within the medium is also needed. Here, we use the framework of macroscopic QED by quantizing the fields in an arbitrary material system, with a spatially-dependent dispersive and absorptive dielectric, starting from a fundamental light-matter action. We truncate the material and mode degrees of freedom while respecting the gauge principle by imposing a partial gauge fixing constraint during canonical quantization, which admits a large number of gauges including the Coulomb and multipolar gauges. We also consider gauge conditions with explicit time-dependence, enabling us to unambiguously introduce phenomenologically time-dependent light-matter interactions in any gauge. Our results allow one to derive rigorous models of ultrastrong light-matter interactions in structured photonic environments with no gauge ambiguity. Results for two-level systems and the dipole approximation are discussed, as well as how to go beyond the dipole approximation for effective single-particle models. By comparing with the limiting case of an inhomogeneous dielectric, where dispersion and absorption can be neglected and the fields can be expanded in terms of the generalized transverse eigenfunctions of the dielectric, we show how lossy systems can introduce an additional gauge ambiguity, which we resolve and predict to have fundamental implications for open quantum system models. Finally, we show how observables in mode-truncated systems can be calculated without ambiguity by using a simple gauge-invariant photodetection model.

quant-ph

Gauge-Independent Emission Spectra and Quantum Correlations in the Ultrastrong Coupling Regime of Open System Cavity-QED

A quantum dipole interacting with an optical cavity is one of the key models in cavity quantum electrodynamics (cavity-QED). To treat this system theoretically, the typical approach is to truncate the dipole to two levels. However, it has been shown that in the ultrastrong-coupling regime, this truncation naively destroys gauge invariance. By truncating in a manner consistent with the gauge principle, we introduce master equations {for open systems} to compute gauge-invariant emission spectra, photon flux rates, and quantum correlation functions which show significant disagreement with previous results obtained using the standard quantum Rabi model. Explicit examples are shown using both the dipole gauge and the Coulomb gauge.

quant-ph

Using the Autler-Townes and ac Stark effects to optically tune the frequency of indistinguishable single-photons from an on-demand source

We describe how a coherent optical drive that is near-resonant with the upper rungs of a three-level ladder system, in conjunction with a short pulse excitation, can be used to provide a frequency-tunable source of on-demand single photons. Using an intuitive master equation model, we identify two distinct regimes of device operation: (i) for a resonant drive, the source operates using the Autler-Townes effect, and (ii) for an off-resonant drive, the source exploits the ac Stark effect. The former regime allows for a large frequency tuning range but coherence suffers from timing jitter effects, while the latter allows for high indistinguishability and efficiency, but with a restricted tuning bandwidth due to high required drive strengths and detunings. We show how both these negative effects can be mitigated by using an optical cavity to increase the collection rate of the desired photons. We apply our general theory to semiconductor quantum dots, which have proven to be excellent single-photon sources, and find that scattering of acoustic phonons leads to excitation-induced dephasing and increased population of the higher energy level which limits the bandwidth of frequency tuning achievable while retaining high indistinguishability. Despite this, for realistic cavity and quantum dot parameters, indistinguishabilities of over $90\%$ are achievable for energy shifts of up to hundreds of $μ$eV, and near-unity indistinguishabilities for energy shifts up to tens of $μ$eV. Additionally, we clarify the often-overlooked differences between an idealized Hong-Ou-Mandel two-photon interference experiment and its usual implementation with an unbalanced Mach-Zehnder interferometer, pointing out the subtle differences in the single-photon visibility associated with these different setups.

quant-ph

Nonlinear Quantum Behavior of Ultrashort-Pulse Optical Parametric Oscillators

The quantum features of ultrashort-pulse optical parametric oscillators (OPOs) are investigated theoretically in the nonlinear regime near and above threshold. Viewing the pulsed OPO as a multimode open quantum system, we rigorously derive a general input-output model that features nonlinear coupling among many cavity (i.e., system) signal modes and a broadband single-pass (i.e., reservoir) pump field. Under appropriate assumptions, our model produces a Lindblad master equation with multimode nonlinear Lindblad operators describing two-photon dissipation and a multimode four-wave-mixing Hamiltonian describing a broadband, dispersive optical cascade, which we show is required to preserve causality. To simplify the multimode complexity of the model, we employ a supermode decomposition to perform numerical simulations in the regime where the pulsed supermodes experience strong single-photon nonlinearity. We find that the quantum nonlinear dynamics induces pump depletion as well as corrections to the below-threshold squeezing spectrum predicted by linearized models. We also observe the formation of non-Gaussian states with Wigner-function negativity and show that the multimode interactions with the pump, both dissipative and dispersive, can act as effective decoherence channels. Finally, we briefly discuss some experimental considerations for potentially observing such quantum nonlinear phenomena with ultrashort-pulse OPOs on nonlinear nanophotonic platforms.

quant-ph

All-optical Tuning of Indistinguishable Single-Photons Generated in Three-level Quantum Systems

Resonance fluorescence of two-level quantum systems has emerged as a powerful tool in quantum information processing. Extension of this approach to higher-level systems provides new opportunities for quantum optics applications. Here we introduce a coherent driving scheme of a three-level ladder system utilizing Autler-Townes and ac Stark effects by resonant excitation with two laser fields. We propose theoretically and demonstrate experimentally the feasibility of this approach towards all-optical spectral tuning of quantum dot-based single-photon sources and investigate photon indistinguishability and purity levels. Our tuning technique allows for fast optical control of the quantum emitter spectrum which paves the way towards temporal and spectral shaping of the single photons, formation of topological Floquet states or generation of high-dimensional frequency-encoded quantum states of light.

quant-ph

Regimes of Cavity-QED under Incoherent Excitation: From Weak to Deep Strong Coupling

The prototypical system constituted by a two-level atom interacting with a quantized single-mode electromagnetic field is described by the quantum Rabi model (QRM). The QRM is potentially valid at any light-matter interaction regime, ranging from the weak (where the decay rates exceeds the coupling rate) to the deep strong coupling (where the interaction rate exceeds the bare transition frequencies of the subsystems). However, when reaching the ultrastrong coupling regime, several theoretical issues may prevent the correct description of the observable dynamics of such a system: (i) the standard quantum optics master equation fails to correctly describe the interaction of this system with the reservoirs; (ii) the correct output photon rate is no longer proportional to the intracavity photon number; and (iii) the appears to violate gauge invariance. Here, we study the photon flux emission rate of this system under the incoherent excitation of the two-level atom for any light-matter interaction strength, and consider different effective temperatures. The dependence of the emission spectra on the coupling strength is the result of the interplay between energy levels, matrix elements of the observables, and the density of states of the reservoirs. Within this approach, we also study the occurence of light-matter decoupling in the deep strong coupling regime, and show how all of the obtained results are gauge invariant.

quant-ph

High-resolution spectroscopy of a quantum dot driven bichromatically by two strong coherent fields

We present spectroscopic experiments and theory of a quantum dot driven bichromatically by two strong coherent lasers. In particular, we explore the regime where the drive strengths are substantial enough to merit a general non-perturbative analysis, resulting in a rich higher-order Floquet dressed-state energy structure. We show high resolution spectroscopy measurements with a variety of laser detunings performed on a single InGaAs quantum dot, with the resulting features well explained with a time-dependent quantum master equation and Floquet analysis. Notably, driving the quantum dot resonance and one of the subsequent Mollow triplet sidepeaks, we observe the disappearance and subsequent reappearance of the central transition and transition resonant with detuned-laser at high detuned-laser pump strengths and additional higher-order effects, e.g. emission triplets at higher harmonics and signatures of higher order Floquet states. For a similar excitation condition but with an off-resonant primary laser, we observe similar spectral features but with an enhanced inherent spectral asymmetry.

quant-ph

Efficient Pulse-Excitation Techniques for Single Photon Sources from Quantum Dots in Cavities

We present rigorous and intuitive master equation models to study on-demand single photon sources from pulse-excited quantum dots coupled to cavities. We consider three methods of source excitation: resonant pi-pulse, off-resonant phonon-assisted inversion, and two-photon excitation of a biexciton-exciton cascade, and investigate the effect of the pulse excitation process on the quantum indistinguishability, efficiency, and purity of emitted photons. By explicitly modelling the time-dependent pulsed excitation process in a manner which captures non-Markovian effects associated with coupling to photon and phonon reservoirs, we find that photons of near-unity indistinguishability can be emitted with over 90% efficiency for all these schemes, with the off-resonant schemes not necessarily requiring polarization filtering due to the frequency separation of the excitation pulse, and allowing for very high single photon purities. Furthermore, the off-resonant methods are shown to be robust over certain parameter regimes, with less stringent requirements on the excitation pulse duration in particular. We also derive a semi-analytical simplification of our master equation for the off-resonant drive, which gives insight into the important role that exciton-phonon decoupling for a strong drive plays in the off-resonant phonon-assisted inversion process

quant-ph

Theory and experiments of coherent photon coupling in semiconductor nanowire waveguides with quantum dot molecules

We present a quantum optics theory, numerical calculations, and experiments on coupled quantumdots in semiconductor nanowire waveguides. We first present an analytical Green function theory tocompute the emitted spectra of two coupled quantum dots, treated as point dipoles, fully accountingfor retardation effects, and demonstrate the signatures of coherent and incoherent coupling througha pronounced splitting of the uncoupled quantum dot resonances and modified spectral broadening.In the weak excitation regime, the classical Green functions used in models are verified and justifiedthrough full 3D solutions of Maxwell equations for nanowire waveguides, specifically using finite-difference time-domain techniques, showing how both waveguide modes and near-field evanescentmode coupling is important. The theory exploits an ensemble-based quantum description, and andan intuitive eigenmode-expansion based Maxwell theory. We then demonstrate how the molecularresonances (in the presence of coupling) take on the form of bright and dark (or quasi-dark) reso-nances, and study how these depend on the excitation and detection conditions. To go beyond theweak excitation regime, we also introduce a quantum master equation approach to model the non-linear spectra from an increasing incoherent pump field, which shows the role of the pump field onthe oscillator strengths and broadening of the molecular resonances, with and without pure dephas-ing. Next, we present experimental photoluminescence spectra for spatially-separated quantum dotmolecules (InAsP) in InP nanowires, which show clear signatures of pronounced splittings, thoughthey also highlight additional mechanisms that are not accounted for in the dipole-dipole couplingmodel. Two different approaches are taken to control the spatial separation of the quantum dotmolecules, and we discuss the advantages and disadvantages of each.

physics.optics

Theory and limits of on-demand single photon sources using plasmonic resonators: a quantized quasinormal mode approach

Quantum emitters coupled to plasmonic resonators are known to allow enhanced broadband Purcell factors, and such systems have been recently suggested as possible candidates for on-demand single photon sources, with fast operation speeds. However, a true single photon source has strict requirements of high efficiency (brightness) and quantum indistinguishability of the emitted photons, which can be quantified through two-photon interference experiments. To help address this problem, we employ and extend a recently developed quantized quasinormal mode approach, which rigorously quantizes arbitrarily lossy open system modes, to compute the key parameters that accurately quantify the figures of merit for plasmon-based single photon sources. We also present a quantized input-output theory to quantify the radiative and nonradiative quantum efficiencies. We exemplify the theory using a nanoplasmonic dimer resonator made up of two gold nanorods, which yields large Purcell factors and good radiative output beta factors. Considering an optically pulsed excitation scheme, we explore the key roles of pulse duration and pure dephasing on the single photon properties, and show that ultrashort pulses (sub-ps) are generally required for such structures, even for low temperature operation. We also quantify the role of the nonradiative beta factor both for single photon and two-photon emission processes. Our general approach can be applied to a wide variety of plasmon systems, including metal-dielectrics, and cavity-waveguide systems, without recourse to phenomenological quantization schemes.

quant-ph

Pulsed excitation dynamics in quantum dot-cavity systems: limits to optimizing the fidelity of on-demand single photon sources

A quantum dot coupled to an optical cavity has recently proven to be an excellent source of on-demand single photons. Typically, applications require simultaneous high efficiency of the source and quantum indistinguishability of the extracted photons. While much progress has been made both in suppressing background sources of decoherence and utilizing cavity-quantum electrodynamics to overcome fundamental limitations set by the intrinsic exciton-phonon scattering inherent in the solid-state platform, the role of the excitation pulse has been often neglected. We investigate quantitatively the factors associated with pulsed excitation that can limit simultaneous efficiency and indistinguishability, including excitation of multiple excitons, multi-photons, and pump-induced dephasing, and find for realistic single photon sources that these effects cause degradation of the source figures-of-merit comparable to that of phonon scattering. We also develop rigorous open quantum system polaron master equation models of quantum dot dynamics under a time-dependent drive which incorporate non-Markovian effects of both photon and phonon reservoirs, and explicitly show how coupling to a high Q-factor cavity suppresses multi-photon emission in a way not predicted by commonly employed models. We then use our findings to summarize the criteria that can be used for single photon source optimization.

quant-ph