Abstract We present a quantum embedding methodology to resolve the Anderson impurity model in the context of dynamical mean-field theory, based on an extended exact diagonalization method. Our method provides a maximally localized quantum impurity model, where the non-local components of the correlation potential remain minimal. This comes at a large benefit, as the environment used in the quantum embedding approach is described by propagating correlated electrons and hence offers an exponentially increasing number of degrees of freedom for the embedding mapping, in contrast to traditional free-electron representation where the scaling is linear. We report that quantum impurity models with as few as 3 bath sites can reproduce both the Mott transition and the Kondo physics, thus opening a more accessible route to the description of time-dependent phenomena. Finally, we obtain excellent agreement for dynamical magnetic susceptibilities, poising this approach as a candidate to describe 2-particle excitations such as excitons in correlated systems. We expect that our approach will be highly beneficial for the implementation of embedding algorithms on quantum computers, as it allows for a fine description of the correlation in materials with a reduced number of required qubits.
Abstract We present a quantum embedding methodology to resolve the Anderson impurity model in the context of dynamical mean-field theory, based on an extended exact diagonalization method. Our method provides a maximally localized quantum impurity model, where the non-local components of the correlation potential remain minimal. This comes at a large benefit, as the environment used in the quantum embedding approach is described by propagating correlated electrons and hence offers an exponentially increasing number of degrees of freedom for the embedding mapping, in contrast to traditional free-electron representation where the scaling is linear. We report that quantum impurity models with as few as 3 bath sites can reproduce both the Mott transition and the Kondo physics, thus opening a more accessible route to the description of time-dependent phenomena. Finally, we obtain excellent agreement for dynamical magnetic susceptibilities, poising this approach as a candidate to describe 2-particle excitations such as excitons in correlated systems. We expect that our approach will be highly beneficial for the implementation of embedding algorithms on quantum computers, as it allows for a fine description of the correlation in materials with a reduced number of required qubits.
Quantum computing opens new avenues for modelling correlated materials, notoriously challenging to solve due to the presence of large electronic correlations. Quantum embedding approaches, such as the dynamical mean-field theory, provide corrections to first-principles calculations for strongly correlated materials, which are poorly described at lower levels of theory. Such embedding approaches are computationally demanding on classical computing architectures, and hence remain restricted to small systems, which limits the scope of applicability. Hitherto, implementations on quantum computers are limited by hardware constraints. Here, we derive a compact representation, where the number of quantum states is reduced for a given system, while retaining a high level of accuracy. We benchmark our method for archetypal quantum states of matter that emerge due to electronic correlations, such as Kondo and Mott physics, both at equilibrium and for quenched systems. We implement this approach on a quantum emulator demonstrating a reduction of the required number of qubits.
Quantum impurity models with strong electron correlations, such as the paradigmatic Anderson Impurity Model (AIM), are central to our understanding of a range of physical phenomena including local moment formation, Coulomb blockade and Kondo screening. They describe magnetic atoms and molecules on surfaces, quantum dot circuits, and correlated materials through dynamical mean field theory. The physics of such systems in strongly non-equilibrium conditions is particularly complex and challenging to capture, whereas Gaussian models of free fermions can be easily solved. Here we show that the time-evolving dynamics of the AIM after a quench can be described by a completely non-interacting version of the model, at the expense of coupling to additional static auxiliary degrees of freedom. Starting from the full solution of the quenched AIM using ED and DMRG, we study the properties of this mapping using numerical optimization, and uncover intriguing structure in the auxiliary system. The method allows us to understand interacting non-equilibrium dynamics through the simpler lens of an effective non-interacting system of larger dimension.
Quantum computers (QC) could harbor the potential to significantly advance materials simulations, particularly at the atomistic scale involving strongly correlated fermionic systems, where an accurate description of quantum many-body effects scales unfavorably with size. While a full-scale treatment of condensed matter systems with currently available noisy quantum computers remains elusive, quantum embedding schemes like dynamical mean-field theory (DMFT) allow the mapping of an effective, reduced subspace Hamiltonian to available devices to improve the accuracy of ab initio calculations such as density functional theory (DFT). Here, we report on the development of a hybrid quantum-classical DFT + DMFT simulation framework which relies on a quantum impurity solver based on the Lehmann representation of the impurity Green’s function. Hardware experiments with up to 14 qubits on the IBM Quantum system are conducted, using advanced error mitigation methods and a novel calibration scheme for an improved zero-noise extrapolation to effectively reduce adverse effects from inherent noise on current quantum devices. We showcase the utility of our quantum DFT + DMFT workflow by assessing the correlation effects on the electronic structure of a real material, Ca 2 CuO 2 Cl 2 , which is mapped to an effective single-band Hubbard Hamiltonian and the subsequently derived Anderson impurity model solved with up to 6 bath sites on available quantum hardware. Further, we carefully benchmark our quantum results with respect to exact reference solutions and experimental spectroscopy measurements. While challenges remain to scale our approach to larger, multi-orbital and multi-site systems with more bath sites, the present work marks an important milestone towards achieving utility-scale quantum computation in materials simulation.
We present a numerical method for the study of correlated quantum impurity problems out of equilibrium, which is particularly suited to address steady-state properties within dynamical mean field theory. The approach, recently introduced by Arrigoni et al. [Phys. Rev. Lett. 110, 086403 (2013)], is based upon a mapping of the original impurity problem onto an auxiliary open quantum system, consisting of the interacting impurity coupled to bath sites as well as to a Markovian environment. The dynamics of the auxiliary system is governed by a Lindblad master equation whose parameters are used to optimize the mapping. The accuracy of the results can be readily estimated and systematically improved by increasing the number of auxiliary bath sites, or by introducing a linear correction. Here, we focus on a detailed discussion of the proposed approach including technical remarks. To solve for the Green's functions of the auxiliary impurity problem, a non-Hermitian Lanczos diagonalization is applied. As a benchmark, results for the steady-state current-voltage characteristics of the single-impurity Anderson model are presented. Furthermore, the bias dependence of the single-particle spectral function and the splitting of the Kondo resonance are discussed. In its present form, the method is fast, efficient, and features a controlled accuracy.
Abstract We propose a minimal effective impurity model that captures the phenomenology of the Mott–Hubbard metal–insulator transition of the half-filled Hubbard model on the Bethe lattice in infinite dimensions as observed by dynamical mean field theory (DMFT). This involves extending the standard Anderson impurity model Hamiltonian to include an explicit Kondo coupling J, as well as a local on-site correlation Ub on the conduction bath site connected directly to the impurity. For the case of attractive local bath correlations ( U b < 0 ), the extended Anderson impurity model (e-SIAM) sheds new light on several aspects of the DMFT phase diagram. For example, the T = 0 metal-to-insulator quantum phase transition (QPT) is preceded by an excited state QPT (ESQPT) where the local moment eigenstates are emergent in the low-lying spectrum. Long-ranged fluctuations are observed near both the QPT and ESQPT, suggesting that they are the origin of the quantum critical scaling observed recently at high temperatures in DMFT simulations. The T = 0 gapless excitations at the quantum critical point display particle-hole interconversion processes, and exhibit power-law behaviour in self-energies and two-particle correlations. These are signatures of non-Fermi liquid behaviour that emerge from the partial breakdown of the Kondo screening.
An essential role for the description of correlated quantum many-particle systems is played by impurity problems. These consist of a small number of localized orbitals, where the electrons are subject to a Coulomb-interaction, coupled to noninteracting bath degrees of freedom. Impurity models are used for the description of magnetic impurities in metals, of quantum points in nanostructures, and in the context of the dynamical mean field theory (DMFT). For their solution a large number of numerical methods exists. We mention here quantum Monte Carlo methods, the numerical renormalization group, or the exact diagonalization method. In this thesis we introduce a new approach to impurity problems, which is based on the functional renormalization group (fRG). In contrast to the methods mentioned above this approach is approximative, but it can be applied with comparatively lower numerical effort. The aim of this thesis is to examine the advantages and limits of this method. An important role in this connection is played by the single impurity Anderson model (SIAM), which is already understood very well with other methods and is seen as a prototype for models with strong local correlations. The spin fluctuations of this model are governed by the so-called Kondo energy scale and a central question of this thesis is whether this scale can be reproduced with our approach. We begin with a short introduction to the Green's function formalism for correlated quantum many particle systems. Then the fRG flow equations for the one-particle irreducible vertex functions are deduced, and several approximation schemes are discussed. In chapter 4 we introduce the fRG scheme used in this thesis. At first the SIAM is mapped to a semi-infinite chain, in which the interacting orbital is given by the first site of this chain. The system is then subdivided into two parts. The first part, which is called 'core', consists of the interacting orbital and the first L bath sites. The remaining bath sites form the second part. At the beginning both parts are decoupled from each other such that the core can be solved exactly. Starting with this exact solution the coupling between the core and the remaining bath sites is switched on slowly in a renormalization group flow. This way it is possible to calculate the one-particle and two-particle correlation functions on the correlated site. We call this flow scheme 'hybridization flow'. The flow equations are formulated in an effective theory on the first bath site outside the core, which turns out to be advantageous compared to other implementations of the hybridization flow. In chapter 5 this hybridization flow method is applied to the SIAM with semi-elliptic bath density of states. We discuss the differences which arise for different core-sizes (L = 0,1,2,3) and for different truncations of the fRG flow equations. In the cases L=0 and L=2 the local Fermi liquid properties of the SIAM and the associated Kondo scale can not be reproduced in both approximation schemes. For the core sizes L=1 and L=3 the ground state of the core is already a spin singlet state in the beginning of the flow and the Fermi liquid properties are reproduced. The Kondo energy scale, which determines the width of the central quasi-particle peak and the size of the local spin-susceptibility, is however not accurately resolved. This is partly due to the finite temperature used in our implementation such that for larger interaction strength the temperature is above the Kondo energy scale. The application of the hybridization flow method to quantum impurity problems in the context of the DMFT is discussed in chapter 6. In this approach lattice models with a local interaction, like the Hubbard model, are mapped to an effective impurity problem for a single lattice site embedded in a dynamical mean field representing the influence of the other electrons. This scheme is exact in infinitely many dimensions and a nonperturbative approximation method for finite-dimensional systems. In particular the Mott metal-insulator transition in the Hubbard model is successfully described by this method. One class of quantities, which is easily accessible from the hybridization flow scheme, is given by the local two-particle correlation functions. These play an essential role in non-local extensions of the DMFT. Therefore we mainly focus on these quantities. At first we apply our flow scheme to the Hubbard model on the Bethe lattice in infinite dimensions and calculate the local one-particle irreducible vertex functions in the insulating and the metallic phase in good agreement with previous calculations, which use the exact diagonalization method as impurity solver. After this we extend our flow scheme to a cluster DMFT method, which includes short-range antiferromagnetic correlations and calculate again the local and non-local vertex functions for the two-dimensional Hubbard model. We compare these to the results of the single-site DMFT.