In this thesis we present an investigation of the influence of quantum correlations on a quantum system’s dynamical behaviour. Our focus is specifically on the time dependence of quantum spins in an environment of itinerant electrons. This is an archetype for strong correlation physics, whose dynamical onset is the central correlation effect investigated in this work. We derive an analytic result for the time evolution of a single localised quantum spin in weak contact with conduction electrons. This result is obtained from a detailed analysis of the pole structure of the Nakajima-Zwanzig equation for the reduced density matrix in Laplace space. We provide a description of the full time range, from very short times in which a novel result for non-Markovian behaviour is obtained, to long times in which we recover the well-known exponential decay expressions. For the short times we show how the non-Markovian memory effects of the spin’s dynamics arise from the backaction of coherent electronic particle-hole fluctuations. As an application of the fast dynamics we propose a cooling protocol going beyond the paradigm of thermodynamic cycles. The protocol relies on a rapid pump scheme with a repeated reinitialisation of the fast quantum coherent dynamics, with each repetition carrying away a small amount of heat from the electronic environment. This protocol is temperature independent and designed to circumvent a natural bottleneck in standard demagnetisation cooling due to long relaxation times at low temperatures. Finally we extend the dynamics to a pair of localised spins coupled through the same electronic environment, using a self-consistent projection operator framework. In contrast to the conventional RKKY coupling we derive a set of coupled equations including the temporal and spatial correlations. This set becomes finite through a meticulous identification of the electronic fluctuations responsible for the coupled dynamics, allowing for a numerical solution.
In this thesis we present an investigation of the influence of quantum correlations on a quantum system’s dynamical behaviour. Our focus is specifically on the time dependence of quantum spins in an environment of itinerant electrons. This is an archetype for strong correlation physics, whose dynamical onset is the central correlation effect investigated in this work. We derive an analytic result for the time evolution of a single localised quantum spin in weak contact with conduction electrons. This result is obtained from a detailed analysis of the pole structure of the Nakajima-Zwanzig equation for the reduced density matrix in Laplace space. We provide a description of the full time range, from very short times in which a novel result for non-Markovian behaviour is obtained, to long times in which we recover the well-known exponential decay expressions. For the short times we show how the non-Markovian memory effects of the spin’s dynamics arise from the backaction of coherent electronic particle-hole fluctuations. As an application of the fast dynamics we propose a cooling protocol going beyond the paradigm of thermodynamic cycles. The protocol relies on a rapid pump scheme with a repeated reinitialisation of the fast quantum coherent dynamics, with each repetition carrying away a small amount of heat from the electronic environment. This protocol is temperature independent and designed to circumvent a natural bottleneck in standard demagnetisation cooling due to long relaxation times at low temperatures. Finally we extend the dynamics to a pair of localised spins coupled through the same electronic environment, using a self-consistent projection operator framework. In contrast to the conventional RKKY coupling we derive a set of coupled equations including the temporal and spatial correlations. This set becomes finite through a meticulous identification of the electronic fluctuations responsible for the coupled dynamics, allowing for a numerical solution.
We provide a versatile analytical framework for calculating the dynamics of a spin system in contact with a fermionic bath beyond the Markov approximation. The approach is based on a second-order expansion of the Nakajima-Zwanzig master equation but systematically includes all quantum coherent memory effects leading to non-Markovian dynamics. Our results describe, for the free induction decay, the full time range from the non-Markovian dynamics at short times, to the well-known exponential thermal decay at long times. We provide full analytic results for the entire time range using a bath of itinerant electrons as an archetype for universal quantum fluctuations. Furthermore, we propose a quantum thermodynamic scheme to employ the temperature insensitivity of the non-Markovian decay to transport heat out of the electron system and thus, by repeated reinitialization of a cluster of spins, to efficiently cool the electrons at very low temperatures.
The theory of open quantum systems represents one of the major developments of quantum mechanics over the last 50 years. Its central object of study is constituted by quantum systems that cannot be regarded as fully isolated, but instead interact with additional degrees of freedom, giving rise to irreversible phenomena such as dissipation and decoherence. The tools provided by this framework are nowadays of paramount importance across many active areas of research, including quantum computation, thermodynamics, metrology and biology. In this thesis, we investigate three main topics within the field. The first contribution concerns the microscopic derivation of the evolution equations, socalled quantum master equations, for open systems which are also subject to external driving fields. Standard techniques developed for time-independent Hamiltonians encounter several difficulties in the time-dependent case, largely restricting their applicability to specific instances, such as periodic or adiabatic drivings. In contrast, a core result of the derivation presented in the thesis is that, when the environment is sufficiently Markovian (essentially, memoryless), the non-adiabatic contributions to the driving field can be neglected in a controlled fashion, yielding an accurate master equation with time-dependent generator, capable of correctly reproducing the open dynamics even for strong drivings. This result is further supported by benchmarks against numerically exact simulations. The second contribution addresses the long-time behavior of general types of (Markovian) quantum master equations, including those of the form introduced above. While this problem has been extensively analyzed in the time-independent setting, virtually no results are known for time-dependent generators. In particular, we establish the foundations of a general theory of relaxation, that is, convergence towards an asymptotic trajectory in the long-time limit, independently of the initial state. The main results include a theorem guaranteeing sufficient conditions for relaxation and the derivation of a rate function governing the convergence to the asymptotic trajectory. The analysis is further extended to a simple non-Markovian case. Moreover, we treat in detail the specific master equation derived in the first part, connecting the aforementioned relaxation property directly to the underlying microscopic dynamics. The third contribution investigates chirality-induced spin selectivity (CISS) effects from the perspective of open quantum systems. Although the majority of theoretical studies aiming to model CISS are based on a coherent description of the spin dynamics, such effects have been observed also for electrons subject to incoherent transport across molecular networks. In this regard, we provide a rigorous ab initio derivation of the microscopic Hamiltonian describing the electronic transport, incorporating electron spin effects and contributions stemming from the nuclear vibrations. Within this result, we critically revise a master equation approach aiming to explain the origin of CISS effects observed in photosynthetic complexes. Taken together, these contributions offer fresh insights and original results on the interplay between driving fields and dissipation, relaxation phenomena, and electronic spin transport in the presence of incoherent dynamics. More broadly, these results provide new theoretical tools with several potential applications in quantum technologies, from modeling of control pulses in noisy environments to quantum reservoir engineering, and contribute to a deeper understanding of the role of quantum effects in biological systems.
This thesis focuses on the study of dissipative quantum impurity models. Quantum impurity models describe a localized quantum system, known as the impurity, that interacts with a large quantum bath, enabling the exploration of essential phenomena such as the Kondo effect in magnetic impurities and the transport properties in quantum dots. An intriguing extension of these models is the exploration of the interplay between strong correlations and dissipation. Dissipation, often described by the Lindblad master equation in its Markovian limit, introduces challenges and opportunities as it interacts with coherent many-body effects. In this thesis, we want to investigate the non-equilibrium dynamics of quantum impurity systems influenced by both strong correlations and dissipation across four main parts. We begin by developing numerical methods, specifically a diagrammatic Monte Carlo technique, to analyze the real-time dynamics of dissipative quantum impurity models. Our findings demonstrate that local Markovian dissipation enhances the convergence of Monte Carlo sampling by constraining the process to a reduced subspace of diagrams. This effectively mitigates the sign problem and facilitates the exploration of longer time scales compared to conventional unitary approaches. In the second part, we derive a self-consistent dynamical map using the Non-Crossing Approximation to study the long-term behavior of dissipative quantum impurity models. This method effectively resums diagrams into a self-consistent Dyson equation, capturing essential non-Markovian environmental effects, including the Kondo effect. In a third part, we examine the relationship between Kondo physics and Markovian dissipation by investigating an interacting quantum dot coupled to a metallic bath under continuous charge monitoring. We identify a crossover from Kondo screening to the Quantum Zeno effect, effectively described by a non-Hermitian Kondo model in the weak dissipation regime. Finally, the last part explores the effects of particle losses on the Kondo effect and the Kondo-Zeno crossover. Preliminary results indicate that while single-particle losses reduce many-body effects, two-body losses introduce intriguing phenomena, such as spin decay and hints of the Kondo-Zeno crossover, along with an unusual spectral function exhibiting a low-frequency lineshape.
In strongly correlated materials, quantum fluctuations taking place at the level of atomic sites play a central role. These local processes are captured nonperturbatively in dynamical mean field theory (DMFT). Nonlocal mechanisms, however, are also suspected to be essential for the proper description of some of these materials, including the well-known high-temperature cuprate superconductors and the more exotic systems of atoms adsorbed on semiconducting surfaces.In this thesis, the effect of nonlocal, potentially long-range fluctuations beyond the DMFT framework is investigated from two angles.First, long-ranged interactions in adatom systems, computed from first principles within the constrained random-phase approximation (cRPA), are treated within the extended DMFT (EDMFT) framework and its combination with the diagrammatic GW method (GW +EDMFT). They are shown to explain some material trends observed in these compounds. In addition, thanks to the spatial and temporal information delivered by GW+EDMFT, they solve existing puzzles raised by different experimental conclusions drawn from different probes.Second, a new approach to the Hubbard model including nonlocal correlation effects is proposed. Formally based on the local expansion of the triply-irreducible functional, this approach, dubbed TRILEX, approximates the renormalized three-leg electron-boson vertex by a local but frequency-dependent vertex computed from an impurity model with retarded density-density and spin-spin interactions. This local vertex is used to construct frequency- and momentum-dependent self-energies capturing nonlocal correlation effects. By construction, this method reconciles two theoretical pictures of cuprate superconductors, namely the spin fluctuation theory at weak interaction strengths and the doped-Mott-insulator picture at strong coupling.This novel approach is applied to the single-band Hubbard model. It is shown to reduce to DMFT at strong coupling and high temperatures, and to fluctuation-exchange theories at weak coupling, while substantial deviations from both limits are observed at intermediate coupling. There, upon doping, antiferromagnetic spin fluctuations are observed to lead to a momentum-differentiated spectral intensity on the Fermi surface, which is reminiscent of the formation of Fermi arcs in photoemission measurements on cuprate superconductors.These two methodological developments are intrinsically linked to algorithmic aspects which are reviewed in the last part of this work. In particular, an open-source library dedicated to massively parallel computations in the field of quantum many-body physics, TRIQS, is presented, with a focus on error estimation through the binning and jackknife methods. The hybridization-expansion continuous-time quantum Monte-Carlo algorithm in the segment picture -- central to the TRILEX method -- and its state-of-the-art implementation are explained. Finally, as a further illustration, a new lightweight method relying on this algorithm and designed for realistic systems, the combined screened-exchange and dynamical DMFT method (SEx+DDMFT), is presented together with an application to the BaCo2As2 compound.
Strongly correlated electron systems show a rich variety of astonishing physical phenomena. However, the strong interactions make the theoretical description of these systems a highly non-trivial task. Even the simplest models cannot be solved exactly, and one has to reside to approximative solutions, which often cover only certain aspects of the physics contained in these models. In recent years progress has been made in the theoretical description of correlated lattice systems through the mapping of lattice models onto effective impurity models. The most prominent example is the mapping of the Hubbard model onto an effective single impurity Anderson model (SIAM). Within this description both models feature the prominent Kondo effect, which leads to the emergence of low energy quasiparticles. The occurrence of such excitations is a result of the dynamical screening of local magnetic moments and the corresponding formation of a low temperature Fermi liquid phase. On the other hand these theories usually fail in the description of non Fermi liquid behavior, which is for example observed in the normal state of high temperature superconductors and some Heavy-Fermion systems. Strong nonlocal fluctuations drive the dynamics of these systems. In the theoretical treatment, due to the mapping of the lattice problem to an effective single impurity problem, these fluctuations are not adequately described.\\\\ In this thesis a new self-consistent approach for the inclusion of spatial correlations is presented for the Hubbard model. In contrast to existing quantum cluster theories in this field, the approach allows for the simultaneous description of short and long range pair correlations. Due to the intimate connection of this new lattice theory with the two impurity Anderson model (TIAM) a thorough numerical investigation of the TIAM is undertaken in this thesis. The competition of the Kondo effect with the RKKY interactions is studied in great detail. Furthermore two new solvers for the TIAM are introduced, which extend existing non crossing approximations for the SIAM.
The dynamics of an open quantum system is non-Markovian when memory effect is non-negligible. The quantum memory effect is a very complex issue and presently there is no universally accepted method to quantify it. By examining the memory kernel of the Nakajima-Zwanzig master equation, we study the memory effect in a theoretical model consisting of a spin coupled to an environment of an Ising spin chain subject to a transverse field. We find that it can be dictated by either the time correlation in the environment, or the system-environment correlation, depending on the strength of the transverse field and the state of the environment. We analyze the information loss to the environment and backflow from it, and discover that the information flow is not always a reliable indicator for the nature of the dynamics.