Nanodevices exploiting quantum effects are critically important elements of future quantum technologies (QT), but their real-world performance is strongly limited by decoherence arising from local `environmental' interactions. Compounding this, as devices become more complex, i.e. contain multiple functional units, the `local' environments begin to overlap, creating the possibility of environmentally mediated decoherence phenomena on new time-and-length scales. Such complex and inherently non-Markovian dynamics could present a challenge for scaling up QT, but – on the other hand – the ability of environments to transfer `signals' and energy might also enable sophisticated spatiotemporal coordination of inter-component processes, as is suggested to happen in biological nanomachines, like enzymes and photosynthetic proteins. Exploiting numerically exact many body methods (tensor networks) we study a fully quantum model that allows us to explore how propagating environmental dynamics can instigate and direct the evolution of spatially remote, non-interacting quantum systems. We demonstrate how energy dissipated into the environment can be remotely harvested to create transient excited/reactive states, and also identify how reorganisation triggered by system excitation can qualitatively and reversibly alter the `downstream' kinetics of a `functional' quantum system. With access to complete system-environment wave functions, we elucidate the microscopic processes underlying these phenomena, providing new insight into how they could be exploited for energy efficient quantum devices.
Nanodevices exploiting quantum effects are critically important elements of future quantum technologies (QT), but their real-world performance is strongly limited by decoherence arising from local environmental' interactions. Compounding this, as devices become more complex, i.e. contain multiple functional units, the local' environments begin to overlap, creating the possibility of environmentally mediated decoherence phenomena on new time-and-length scales. Such complex and inherently non-Markovian dynamics could present a challenge for scaling up QT, but – on the other hand – the ability of environments to transfer signals' and energy might also enable sophisticated spatiotemporal coordination of inter-component processes, as is suggested to happen in biological nanomachines, like enzymes and photosynthetic proteins. Exploiting numerically exact many body methods (tensor networks) we study a fully quantum model that allows us to explore how propagating environmental dynamics can instigate and direct the evolution of spatially remote, non-interacting quantum systems. We demonstrate how energy dissipated into the environment can be remotely harvested to create transient excited/reactive states, and also identify how reorganisation triggered by system excitation can qualitatively and reversibly alter the downstream' kinetics of a `functional' quantum system. With access to complete system-environment wave functions, we elucidate the microscopic processes underlying these phenomena, providing new insight into how they could be exploited for energy efficient quantum devices.
A better understanding of dissipation is crucial for understanding real-world quantum systems. Indeed, all quantum systems experience interactions with an (often) uncontrollable outside environment that can lead to a decay of excited state populations and a loss of quantum coherences. The study of dissipation is timely as the development of next-generation nanoscale quantum technologies is on its way, and the existence of non-trivial quantum effects in biological systems is being seriously investigated. However, descriptions of dissipation in quantum systems are reduced (most of the time) to time-local approaches and (everywhere) to space-local independent environments. These simplifying assumptions do render analytic and numerical calculations possible, yet they get rid of a breadth of physical processes that can alter radically the quantum systems' dynamics. In this thesis, building on a numerically exact tensor networks method, we developed a technique able to handle spatio-temporal correlations between a quantum system and bosonic (i.e. vibrational, electromagnetic, magnons, etc.) environments. With this method we studied the signalling process - a form of information backflow - in quantum systems, and uncovered how it can induce non-trivial dynamics, and be leveraged to populate otherwise inaccessible excited states. We also evidenced the ability of 'non-local' environment reorganisation, induced by system-environment interactions, to radically change the nature of the thermodynamically favoured system ground state. The new phenomenology of physical processes, resulting from considering quantum systems interacting with a common environment, has important consequences for the design of nanodevices as it gives access to new control, sensing and cross-talk mechanisms. In another vein, these results might also give us a new framework to study and interpret (quantum?) effects in the biological realm.
Strong coupling between a quantum system and its many-body environment is becoming an increasingly important topic for many branches of physics. Numerous systems of experimental and technological relevance demonstrate strong system-environment coupling, leading to complex dynamical behaviour. This thesis is concerned with two particular examples of such systems, namely quantum dots (QDs) and excitonic energy transfer (EET) in molecular systems. Traditional quantum optics treatments are often insufficient to describe the transient, steady state, and optical properties of QDs due to system-environment correlations. In contrast, we present a modified theory of quantum optics capable of capturing the influence of a thermal environment on the behaviour of QDs. Using this framework we demonstrate a striking departure of the emission spectra and photon measurement statistics of a classically driven QD when compared to an analogous atomic system. Furthermore, in contradiction to accepted notions of decoherence and dissipation, we show that the interaction between a QD and its thermal environment induces non-classical light-matter correlations in an otherwise semi-classical regime of cavity quantum electrodynamics. Away from QDs, we develop the reaction coordinate (RC) formalism to describe the dynamics of a system coupled to a low frequency environment — a regime important to EET systems. We do so by identifying and incorporating important environmental degrees of freedom into an enlarged system Hamiltonian. Uniquely, this approach gives insight directly into the dynamical evolution of the environment and correlations accumulated between the system and environment. Furthermore, it is demonstrated that these corre- lations persist into the steady state, generating non-canonical equilibrium states of the system and environment. We then apply the RC model to describe EET in a molecular dimer, highlighting the effect that under- and over-damped environments have on the excitation dynamics. In doing so, we show interactions between the dimer and a structured environment can significantly enhance the energy transfer rate.
All real-world quantum systems interact with their surrounding environment to some extent. No matter how weak the coupling that prevents the system from being isolated, the evolution of an open quantum system is eventually plagued by non-unitary features, such as decoherence and dissipation. Decoherence is a quantum effect where the system loses its ability to exhibit coherent behavior. Nowadays, decoherence stands as a serious obstacle in quantum information processing. As the manipulation of quantum coherence in experiments has progressed, the need to better understand, control, and utilize dissipative non-equilibrium dynamics of quantum systems has grown in importance. This has ranged from fundamental questions associated with the quantum-to-classical transition and quantum thermodynamics innovation in quantum optics and cavity/circuit quantum electrodynamics. Current studies of many-body dynamics, ultracold atoms in optical lattices, trapped ions, superconducting systems, nanoelectro-mechanical systems, and quantum fields under the influence of external conditions offer new challenges to address questions regarding quantum systems far from equilibrium. On the theoretical side, quantum trajectory-based methods could be the key to both quantum nanodevice design and exploration of new regimes of quantum mechanics and quantum measurement, as well as applications to various quantum technologies.
The simulation of open quantum dynamics is a critical tool for understanding how the non-classical properties of matter might be functionalised in future devices. However, unlocking the enormous potential of molecular quantum processes is highly challenging due to the very strong and non-Markovian coupling of 'environmental' molecular vibrations to the electronic 'system' degrees of freedom. Here, we present an advanced but general computational strategy that allows tensor network methods to effectively compute the non-perturbative, real-time dynamics of exponentially large vibronic wave functions of real molecules. We demonstrate how ab initio modelling, machine learning and entanglement analysis can enable simulations which provide real-time insight and direct visualisation of dissipative photophysics, and illustrate this with an example based on the ultrafast process known as singlet fission.
Tracing out the environmental degrees of freedom is a necessary procedure when simulating open quantum systems. While being an essential step in deriving a tractable master equation it represents a loss of information. In situations where there is strong interplay between the system and environmental degrees of freedom this loss makes understanding the dynamics challenging. These dynamics, when viewed in isolation, have no time-local description: they are non-Markovian and memory effects induce complex features that are difficult to interpret. To address this problem, we here show how to use system correlations, calculated by any method, to infer any correlation function of a Gaussian environment, so long as the coupling between system and environment is linear. This not only allows reconstruction of the full dynamics of both system and environment, but also opens avenues into studying the effect of a system on its environment. In order to obtain accurate bath dynamics, we exploit a numerically exact approach to simulating the system dynamics, which is based on the construction and contraction of a tensor network that represents the process tensor of this open quantum system. Using this we are able to find any system correlation function exactly. To demonstrate the applicability of our method we show how heat moves between different modes of a bosonic bath when coupled to a two-level system that is subject to an off-resonant drive.
All real-world quantum systems interact with their surrounding environment to some extent. No matter how weak the coupling that prevents the system from being isolated, the evolution of an open quantum system is eventually plagued by non-unitary features, such as decoherence and dissipation. Decoherence is a quantum effect where the system loses its ability to exhibit coherent behavior. Nowadays, decoherence stands as a serious obstacle in quantum information processing. As the manipulation of quantum coherence in experiments has progressed, the need to better understand, control, and utilize dissipative non-equilibrium dynamics of quantum systems has grown in importance. This has ranged from fundamental questions associated with the quantum-to-classical transition and quantum thermodynamics innovation in quantum optics and cavity/circuit quantum electrodynamics. Current studies of many-body dynamics, ultracold atoms in optical lattices, trapped ions, superconducting systems, nanoelectro-mechanical systems, and quantum fields under the influence of external conditions offer new challenges to address questions regarding quantum systems far from equilibrium. On the theoretical side, quantum trajectory-based methods could be the key to both quantum nanodevice design and exploration of new regimes of quantum mechanics and quantum measurement, as well as applications to various quantum technologies.