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Adam Burgess

Publications and source records attributed to Adam Burgess.

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Dynamics and spectra of open quantum systems coupled to anharmonic environments

In open quantum systems, the environment is typically modelled as a collection of harmonic oscillators, whereas realistic environments often exhibit unique non-Markovian effects due to the anharmonicity of the environment. Here we present a framework for modelling anharmonic environments in open quantum systems numerically exactly, in which, via a matching criterion, we map the anharmonic environment onto an effective harmonic one. This results in an effective spectral density that is a collection of shifted bare spectra arising from the non-equidistant energy gaps of the anharmonic environment, along with a unique zero-frequency term that effectively acts as static disorder on the system. This is due to the non-zero variance of the diagonal of the bath coupling operator. In tandem, we develop a framework for investigating the effects of environments comprising a few damped anharmonic modes where the matching criterion fails to work due to the non-Gaussianity of the environment. For both continuous and discrete damped anharmonic environments, this work investigates their unique influence on the system's dynamics, including enhanced non-Markovianity compared to a harmonic approximation, novel effects in the absorption spectrum, and the potential for anharmonic environments to enhance energy transport.

quant-ph

Tensor network methods for non-perturbative dynamics of open quantum systems

The description of open quantum system dynamics beyond the perturbative treatment (usually associated with Markovian master equations) is a computationally challenging task due to the unfavorable exponential scaling of memory kernels. Developed over recent decades in the context of quantum information and condensed matter, tensor networks provide both a new formalism and a toolbox for overcoming previous computational bottlenecks. This framework enables the formulation of non-perturbative, numerically exact methods for describing the dynamics of open quantum systems to controllable numerical accuracy. In this review, we present these methods and discuss their commonalities and differences to paint a comprehensive view of the field.

quant-ph

Scalable framework for quantum transport across large physical networks

Accurately modelling many-body quantum transport systems poses a challenge both conceptually and computationally due to the growth of the Hilbert space and the multi-scale nature of the geometries and couplings present in most naturally occurring networks. A compounding complexity of such systems is that the environment typically plays a key role in the transport dynamics. Utilising variational unitary transformations that displace environmental degrees of freedom allows for the deployment of a second-order master equation capable of capturing the dynamics of intermediate and strongly coupled systems, which are ubiquitous in microscopic energy transport systems. However, direct implementations of this approach suffer from fundamental scalability issues due to the complexity of the self-consistent equations required to solve for the variational parameters. Here, we present an efficient partitioning scheme that leverages the inherent multi-scale nature of natural energy transport networks. This enables scaling of the variational polaron framework to quantum energy transport systems, constituting hundreds to thousands of sites. Our work unlocks the physically motivated exploration of large transport networks, for example, those present within light-harvesting complexes and exciton transport in disordered semiconductors.

quant-ph

The Effect of Permanent Dipoles on Dark States in Molecular Dimers

Many organic molecules possess large permanent dipole moments that differ depending on the electronic state. These permanent dipoles influence both intermolecular coupling and interactions with the optical fields, yet they are often neglected in typical theoretical quantum optics treatments. Here, we investigate the optical properties and their effect on dark states of dimers possessing such permanent dipoles. We show that when monomers have excitation-dependent permanent dipoles, optical transitions between the bright and dark states of the dimer are enabled. We investigate how permanent dipoles allow for the existence of static driving terms between the ground and excited states of each monomer. In turn, these can cause the excited states of the monomers to couple indirectly to the zero excitation state of the dimer. This leads to interference between permanent and transition dipoles and can result in the formation of dark states that are entirely localised. Furthermore, dark states formed through indirect coupling exhibit enhanced robustness against energy level fluctuations, which may improve the efficiency of the design of photovoltaic devices.

quant-ph

Optical signatures of coherence in molecular dimers

We calculate experimentally measurable signatures of quantum correlations in a coupled molecular dimer that strongly interacts with its vibrational environment. We investigate intensity and mode-resolved photon coincidences for different relative orientations of such dimers, and observe spatio-temporal correlations for various configurations. We find that projective measurements can produce cooperative signatures even when emitters are arranged orthogonal to each other. To model effects of vibrational environments that are present in realistic experimental situations, we use the polaron framework. Further, we also account for the effects of finite instrument response, varying temperature, and presence of static disorder. We analyse the effect of disorder in both dimer orientation and measurement direction and find that photon coincidences remain well-resolvable using state-of-the-art detectors. This work enhances our understanding of cooperative emission from two coupled emitters and offers direction for future experiments on probing their coherent dynamics.

quant-ph

Enhancing energy transport utilising permanent molecular dipoles

We study exciton quantum transfer along a molecular chain whilst accounting for the effects of permanent dipoles that are induced by charge displacements in the molecular orbitals. These effects are typically neglected as they do not arise in atomic quantum optics; however, they can play an important role in molecular systems. We also consider novel collective photon-assisted transport and compare it against the scaling of phonon-assisted transport in chains featuring permanent dipoles, and determine a linear scaling with the number of dipoles, akin to single-excitation superradiance. We further demonstrate how permanent dipoles, dipoles can preferentially arrange energy eigenstates to support excitation transport. Finally, we show how permanent dipoles can enhance the ability of the molecular chain to support excitation transport compared to that of systems that do not possess permanent dipoles across a range of environmental and system configurations.

physics.chem-ph

Engineering dipole-dipole couplings for enhanced cooperative light-matter interactions

Cooperative optical effects are enabled and controlled by interactions between molecular dipoles, meaning that their mutual orientation is of paramount importance to, for example, superabsorbing light-harvesting antennas. Here we show how to move beyond the possibilities of simple geometric tailoring, demonstrating how a metallic sphere placed within a ring of parallel dipoles engineers an effective Hamiltonian that generates "guide-sliding" states within the ring system. This allows steady-state superabsorption in noisy room temperature environments, outperforming previous designs while being significantly simpler to implement. As exemplified by this showcase, our approach represents a powerful design paradigm for tailoring cooperative light-matter effects in molecular structures that extends beyond superabsorbing systems, to a huge array of quantum energy transport systems.

physics.optics

Optical polaron formation in quantum systems with permanent dipoles

Many optically active systems possess spatially asymmetric electron orbitals. These generate permanent dipole moments, which can be stronger than the corresponding transition dipole moments, significantly affecting the system dynamics and creating polarised Fock states of light. We derive a master equation for these systems by employing an optical polaron transformation that captures the photon mode polarisation induced by the permanent dipoles. This provides an intuitive framework to explore their influence on the system dynamics and emission spectrum. We find that permanent dipoles introduce multiple-photon processes and a photon sideband which causes substantial modifications to single-photon transition dipole processes. In the presence of an external drive, permanent dipoles lead to an additional process that we show can be exploited to optimise the decoherence and transition rates. We derive the emission spectrum of the system, highlighting experimentally detectable signatures of optical polarons, and measurements that can identify the parameters in the system Hamiltonian, the magnitude of the differences in the permanent dipoles, and the steady-state populations of the system.

quant-ph

Dynamical Decoherence and Memory Effects in Green Fluorescent Proteins by Dielectric Relaxation

In this article, we explore the dynamical decoherence of the chromophores within a green fluorescent protein when coupled to a finite-temperature dielectric environment. Such systems are of significant interest due to their anomalously long coherence lifetimes compared to other biomolecules. We work within the spin-boson model and employ the Hierarchical Equations of Motion formalism which allows for the accounting of the full non-perturbative and non-Markovian characteristics of the system dynamics. We analyse the level coherence of independent green fluorescent protein chromophores and the energy transfer dynamics in homo-dimer green fluorescent proteins, focusing on the effect of dielectric relaxation on the timescales of these systems. Using the Fluctuation-Dissipation theorem, we generate spectral densities from local electric susceptibility generated from Poisson's equation and employ a Debye dielectric model for the solvent environment. For different system architectures, we identify a number of very striking features in the dynamics of the chromophore induced by the dielectric relaxation of the environment, resulting in strong memory effects that extend the coherence lifetime of the system. Remarkably, the complex architecture of the green fluorescent protein, which includes a cavity-like structure around the atomic system, is well suited to preserving the coherences in the homo-dimer system. The system dynamics generate a dynamical correlation between the coherent energy transfer between its sub-systems and the entropy production, which can lead to transient reductions in entropy, a unique feature of the non-Markovian nature of the system-environment interaction.

physics.chem-ph

Quantum memory effects in atomic ensembles coupled to photonic cavities

In this article we explore the dynamics of many-body atomic systems symmetrically coupled to a single Lorentzian photonic cavity. Our study reveals interesting dynamical characteristics including non-zero steady states, superradiant decay, enhanced energy transfer and the ability to modulate oscillations in the atomic system by tuning environmental degrees of freedom. We also analyse a configuration consisting of a three-atom chain embedded in a photonic cavity. Similarly, we find a strong enhancement of the energy transfer rate between the two ends of the chain and identified specific initial conditions that lead to significantly reduced dissipation between the two atoms at the end of the chain. Another configuration of interest consists of two symmetrical detuned reservoirs with respect to the atomic system. In the single-atom case, we show that it is possible to enhance the decay rate of the system by modulating its reservoir detuning, while in the many-atom case, this results in dynamics akin to the on-resonant cavity. Finally, we examine the validity of rotating wave approximation through a direct comparison against the numerically exact hierarchical equations of motion approach. We find good agreement in the weak coupling regime while in the intermediate coupling regime, we identify qualitative similarities, but the rotating wave approximation becomes less reliable. In the moderate coupling regime, we find deviation of the steady states due to the formation of mixed photon atom states.

quant-ph

Quantum Reservoir Computing Implementations for Classical and Quantum Problems

Quantum reservoir computing has emerged as a promising paradigm within the field of quantum machine learning, harnessing the inherent properties of quantum systems to optimise and enhance information processing capabilities. Here, we explore the potential of quantum-inspired machine learning methodologies by leveraging the complex dynamics of quantum reservoirs to address computationally challenging tasks with enhanced efficiency and accuracy. To this end, we employ an open quantum system model comprising two-level atomic ensembles coupled to Lorentzian photonic cavities to construct a quantum physical reservoir computer layer for a recurrent neural network. We evaluate the effectiveness of this approach by applying it to a standard machine learning image-recognition problem and benchmarking its performance against a conventional neural network of similar architecture, but lacking the quantum physical reservoir computer layer. Remarkably, as the dataset size increases, the quantum physical reservoir computer outperforms the conventional neural network, requiring fewer training epochs and a smaller dataset to achieve comparable accuracy. Furthermore, we employ the quantum physical reservoir computing approach to model the dynamics of open quantum systems, focusing on atomic system ensembles interacting with a structured photonic reservoir associated with a photonic band-gap material. Our results reveal that the quantum reservoir computer provides equally powerful representations for quantum dynamical problems, maintaining effectiveness even under constraints of limited training data.

quant-ph

Non-Markovian Dynamics of a Single Excitation within Many-Body Dissipative Systems

We explore the dynamics of $N$ coupled atoms to a generic bosonic reservoir under specific system symmetries. In the regime of multiple atoms coupled to a single reservoir with identical couplings, we identify remarkable effects, notably that the initial configuration of the atomic excited state amplitudes strongly impacts the dynamics of the system and can even fully sever the system from its environment. Additionally, we find that steady state amplitudes of the excited states become independent of the choice of the reservoir. The framework introduced is applied to a structured photonic reservoir associated with a photonic crystal, where we show it reproduces previous theoretical and experimental results and it predicts superradiant behaviour within the single-excitation regime.

quant-ph