The theoretical description of materials' properties driven out of equilibrium has important consequences in various fields such as semiconductor spintronics, nonlinear optics, and continuous and discrete quantum information science and technology. The coupling of a quantum many-body system to an external bath can dramatically modify its dynamics compared to that of closed systems; new phenomena like relaxation and decoherence appear as a consequence of the non-unitary evolution of the quantum system. In addition, electron-electron correlations must be properly accounted for in order to go beyond a simple one-electron or mean-field description of the electronic system. Here, we discuss a first-principles methodology based on the evolution of the electronic density matrix capable of treating electron-environment interactions and electron-electron correlations at the same level of description. The effect of the environment is separated into a coherent contribution, like the coupling to applied external electromagnetic fields, and an incoherent contribution, like the interaction with lattice vibrations or the thermal background of radiation. Electron-electron interactions are included using the nonequilibrium Green's function plus the generalized Kadanoff-Baym ansatz. The obtained non-Markovian coupled set of equations reduces to the ordinary Lindblad quantum master equation form in the Markovian limit.
The theoretical description of materials' properties driven out of equilibrium has important consequences in various fields such as semiconductor spintronics, nonlinear optics, and continuous and discrete quantum information science and technology. The coupling of a quantum many-body system to an external bath can dramatically modify its dynamics compared to that of closed systems; new phenomena like relaxation and decoherence appear as a consequence of the non-unitary evolution of the quantum system. In addition, electron-electron correlations must be properly accounted for in order to go beyond a simple one-electron or mean-field description of the electronic system. Here, we discuss a first-principles methodology based on the evolution of the electronic density matrix capable of treating electron-environment interactions and electron-electron correlations at the same level of description. The effect of the environment is separated into a coherent contribution, like the coupling to applied external electromagnetic fields, and an incoherent contribution, like the interaction with lattice vibrations or the thermal background of radiation. Electron-electron interactions are included using the nonequilibrium Green's function plus the generalized Kadanoff-Baym ansatz. The obtained non-Markovian coupled set of equations reduces to the ordinary Lindblad quantum master equation form in the Markovian limit.
The quantum dynamics of many-electron spin systems is investigated using a reduced-density-matrix description. Applications of interest include trapped atomic systems in optical lattices, semiconductor quantum dots, and vacancy defect centers in solids. Complimentary time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are self-consistently developed. The general non-perturbative and non-Markovian formulations provide a fundamental framework for systematic evaluations of corrections to the standard Born (lowest-order-perturbation) and Markov (short-memory-time) approximations. Particular attention is given to decoherence and relaxation processes, together with spectral-line broadening phenomena, that are induced by interactions of many-electron spin systems with photons, phonons, nuclear spins, external electric, magnetic, and electromagnetic fields. Within the framework of a quantum-open-systems (reduced-density-operator) approach, these processes are treated either as coherent interactions or as environmental interactions. The environmental interactions are incorporated by means of the general expressions that are derived for the time-domain and frequency-domain Liouville-space self-energy operators, for which the tetradic-matrix elements are explicitly evaluated in the diagonal-resolvent, lowest-order, and Markov (short-memory time) approximations.
Quantum systems are inherently open to their environment and thus they evolve under the influence of dissipation, decoherence and driving from external fields. This poses a significant theoretical challenge: how to track the dynamics of the system of interest while tracing out environmental degrees of freedom. Markovian master equations offer a longstanding solution to this problem, where under a series of assumptions the reduced density matrix of the system can be obtained. These flexible approaches provide a conceptually and numerically simple framework for describing complex many-body systems. However, the assumptions enforced by Markovian master equations create a gap in the availability of generic, simple, and analytical techniques capable of treating open quantum systems beyond the regimes of standard Markovian master equations. In this thesis, we introduce three studies addressing three regimes that are inaccessible to standard Markovian master equations and investigate their consequences in quantum thermodynamics-inspired applications. We begin by developing a Markovian embedding technique to tackle non-Markovian dynamics induced by the long correlation times of a qubit coupled to a structured environment. Subsequently, we propose an "effective" Hamiltonian theory enabling the study of equilibrium properties of strong coupling to a thermal reservoir through a dressed version of the Gibbs state. This framework can also be applied to address problems of equilibration, transport, quantum thermal machines, and quantum dynamics. Lastly, we showcase the importance of including non-secular terms in the quantum master equation, which results in a drastic separation of timescales leading to rich metastable dynamics. We apply this quantum master equation approach to temperature sensing in a nonequilibrium setting offering an alternative to standard equilibrium probes. Overall, this thesis contributes novel theoretical techniques for tackling open quantum systems beyond standard approximations with applications in quantum thermodynamics.
An open quantum system is a quantum system that interacts with some environment whose degrees of freedom have been coarse grained away. This model describes non-equilibrium processes more general than scattering-matrix formulations. Furthermore, the microscopically-derived environment provides a model of noise, dissipation and decoherence far more general than Markovian (white noise) models. The latter are fully characterized by Lindblad equations and can be motivated phenomenologically. Non-Markovian processes consistently account for backreaction with the environment and can incorporate effects such as finite temperature and spatial correlations. We consider linear systems with bilinear coupling to the environment, or quantum Brownian motion, and nonlinear systems with weak coupling to the environment. For linear systems we provide exact solutions with analytical results for a variety of spectral densities. Furthermore, we point out an important mathematical subtlety which led to incorrect master-equation coefficients in earlier derivations, given nonlocal dissipation. For nonlinear systems we provide perturbative solutions by translating the formalism of canonical perturbation theory into the context of master equations. It is shown that unavoidable degeneracy causes an unfortunate reduction in accuracy between perturbative master equations and their solutions. We also extend the famous theorem of Lindblad, Gorini, Kossakowski and Sudarshan on completely positivity to non-Markovian master equations. Our application is primarily to model atoms interacting via a common electromagnetic field. The electromagnetic field contains correlations in both space and time, which are related to its relativistic (photon-mediated) nature. As such, atoms residing in the same field experience different environmental effects depending upon their relative position and orientation. Our more accurate solutions were necessary to assess sudden death of entanglement at zero temperature. In contrast to previous claims, we found that all initial states of two-level atoms undergo finite-time disentanglement. We were also able to access regimes which cannot be described by Lindblad equations and other simpler methods, such as near resonance. Finally we revisit the infamous Abraham-Lorentz force, wherein a single particle in motion experiences backreaction from the electromagnetic field. This leads to a number of well-known problems including pre-acceleration and runaway solutions. We found a more a more-suitable open-system treatment of the nonrelativistic particle to be perfectly causal and dissipative without any extraneous requirements for finite size of the particle, weak coupling to the field, etc..
Open quantum systems have drawn attention over decades due to its applicability in the foundation of theoretical physics, e.g. statistical mechanics, quantum mechanics and condensed matter physics. The dynamics of open quantum systems has been described as separate entities from their surrounding environment that consists of a very large number of modes, somehow coupled to the mode of the system. Even though the exact solution of the dynamical behavior of the system is impossible to calculate, we obtain a tentative solution using the crucial Markov approximation. The input-output formalism of the quantum Langevin equation (QLE) has been considered as a useful tool which provides a semi-classical description of the dynamics of the system, whereas the master equation provides a complete picture of the dynamics of the system expressed in terms of density matrix. While studying the dynamics of nonlinear system/environment coupling using QLE, we see, for a small value of external field, that the steady state system field does not change much from the steady state field obtained in the absence of nonlinear dissipation. However, in a case where a stronger external field is applied, we see that the deviation becomes substantial from the solution of linear system. We also see that the nonlinear coupling introduces significant difference in the cavity fluctuation spectrum. The description, therefore, provides a potential explanation of parametric effects in terms of nonlinear dissipation phenomena associated with the nonlinear coupling. Even though the theories developed in the context of open quantum systems have proven to be powerful tools, they do not provide a satisfactory platform to be implemented on non-linear Hamiltonians. We often approximate it by linearizing over nonlinear steady state field amplitude, and therefore, the interesting effects are often overlooked. The limitation of the analytics provokes us to simulate open quantum dynamics numerically. The numerical method consists of transformation of the environmental degrees of freedom to a one-dimensional many-body chain, and the computational technique includes numerical diagonalization and renormalization process. The time-adaptive density matrix renormalisation group (t-DMRG) is known as one of the most powerful techniques for the simulation of strongly-correlated many-body quantum systems. In this thesis, along with the theoretical modeling, we implement DMRG numerical scheme for the simulation of canonical S/B model by mapping it to one-dimensional harmonic chain with nearest neighbor interactions, and use the method to investigate the dynamics of the free dissipative system. The thermalization of open quantum systems is also studied by generating minimally entangled typical thermal states (METTS) through imaginary time evolution, and real-time evolving an empty system in the presence of the thermal bath. Further, we simulate coherently driven free dissipative Kerr nonlinear system numerically using Euler's method by solving Heisenberg equation of motion and t-DMRG algorithm, and demonstrate how the numerical results are analogous to classical bistability. By comparing with analytics, we see that the DMRG numerics is analogous to the quantum-mechanical exact solution obtained by mapping the equation of motion of the density matrix of the system to a Fokker-Plank equation. The comparison between two different numerical techniques shows that the semi-classical Euler's method determines the dynamics of the system field of one among two coherent branches, whereas DMRG numerics gives the superposition of both of them. Hence, DMRG-determined time dynamics undergoes generating non-classical states. Our approach of dealing with nonlinearity represents an important contribution in the developments of technique to study the dynamical and steady-state behavior of open quantum systems, which is a fundamental aspect of quantum physics.
This work establishes a strongly correlated system-and-bath dynamics theory, the many-dissipaton density operators formalism. It puts forward a quasi-particle picture for environmental influences. This picture unifies the physical descriptions and algebraic treatments on three distinct classes of quantum environments, electron bath, phonon bath, and two-level spin or exciton bath, as their participating in quantum dissipation processes. Dynamical variables for theoretical description are no longer just the reduced density matrix for system, but remarkably also those for quasi-particles of bath. The present theoretical formalism offers efficient and accurate means for the study of steady-state (nonequilibrium and equilibrium) and real-time dynamical properties of both systems and hybridizing environments. It further provides universal evaluations, exact in principle, on various correlation functions, including even those of environmental degrees of freedom in coupling with systems. Induced environmental dynamics could be reflected directly in experimentally measurable quantities, such as Fano resonances and quantum transport current shot noise statistics.
In this work, we lay down the ab initio many-body quantum theory of electrons and phonons in equilibrium as well as in steady-state or time-varying settings.Our focus is on the harmonic approximation, but the developed tools can readily incorporate anharmonic effects.We begin by showing the necessity of determining the ab initio Hamiltonian in a self-consistent manner to ensure the existence of an equilibrium state.We then identify the correct partitioning into a "noninteracting" and an "interacting" part to carry out diagrammatic expansions in terms of dressed propagators and screened interactions.The final outcome is the finite-temperature nonequilibrium extension of the Hedin equations, showcasing the emergence of the coupling between electrons and coherent phonons through the time-local Ehrenfest diagram.The Hedin equations have limited practical utility for real-time simulations of systems driven out of equilibrium by external fields.To overcome this limitation, we leverage the versatility of the diagrammatic approach to generate a closed system of differential equations for the dressed propagators and nuclear displacements.These are the Kadanoff-Baym equations for electrons and phonons.The formalism naturally merges with the theory of conserving approximations, which guarantee the satisfaction of the continuity equation and the conservation of total energy during time evolution.As an example, we show that the popular Born-Oppenheimer approximation is not conserving whereas its dynamical extension is conserving, provided that the electrons are treated in the Fan-Migdal approximation with a dynamically screened electronphonon coupling.We also derive the formal solution of the Kadanoff-Baym equations for nonequilibrium steady states, which is useful for studies in photovoltaics and optoelectronics.Interestingly, the expansion of the phononic Green's function around the quasiphonon energies points to a correlation-induced splitting of the phonon dispersion in materials with no time-reversal invariance.