Publications

For molecules and solids, we developed efficient MPI-parallel algorithms for evaluating the second-order exchange term with bare, statically screened, and dynamically screened interactions. We employ the resulting term in a fully self-consistent manner together with scGW, resulting in the following vertex-corrected scGW schemes: scGWSOX, scGWSOSEX, scGW2SOSEX, and scG3W2theories. We show that for the vertex evaluation, the reduction of scaling by tensor hypercontraction (THC) has two limiting execution regimes. We used the resulting code to perform the largest (by the number of orbitals) fully self-consistent calculations with the SOX term. We demonstrate that our procedure allows for a reliable evaluation of even small energy differences. Utilizing a broken-symmetry approach, we explore the influence of the SOX term on the effective magnetic exchange couplings. We show that the treatment of SOX has a significant impact on the obtained values of the effective exchange constants, which we explain through a self-energy dependence on an effective dielectric constant. We confirm this explanation by analyzing natural orbitals and local changes in charge transfer quantifying superexchange. Our analysis explains the structure of weak electron correlation responsible for the modulation of superexchange in both molecules and solids. Finally, for solids, we evaluate Neel temperatures utilizing the high-temperature expansion and compare the results obtained with experimental measurements.

We study the formation of ferromagnetic and magnetic polaron states in weakly doped heterobilayer transition metal dichalcogenides in the

The recent observation of superconductivity in the vicinity of insulating or Fermi surface reconstructed metallic states has established twisted bilayers of WSe

Magic angle twisted bilayer graphene (MATBG) presents a fascinating platform for investigating the effects of electron interactions in topological flat bands. The Bistritzer-MacDonald (BM) model provides a simplified quantitative description of the flat bands. Introducing long-range Coulomb interactions leads to an interacting BM (IBM) Hamiltonian, a momentum-space continuum description which offers a very natural starting point for many-body studies of MATBG. Accurate and reliable many-body computations in the IBM model are challenging, however, and have been limited mostly to special fillings, or smaller lattice sizes. We employ state-of-the-art auxiliary-field quantum Monte Carlo (AFQMC) method to study the IBM model, which constrains the sign problem to enable accurate treatment of large system sizes. We determine ground-state properties and quantify errors compared to mean-field theory calculations. Our calculations identify correlated metal states and their competition with the insulating Kramers inter-valley coherent state at both half-filling and charge neutrality. Additionally, we investigate one- and three-quarter fillings, and examine the effect of many-body corrections beyond single Slater determinant solutions. We discuss the effect that details of the IBM Hamiltonian have on the results, including different forms of double-counting corrections, and the need to establish and precisely specify many-body Hamiltonians to allow more direct and quantitative comparisons with experiments in MATBG.

We show how to use diagrammatic techniques to compute the weak-coupling perturbation series of the self-consistent solution to a Dynamical Mean Field Theory (DMFT) problem. This approach constitutes an alternative to using diagrammatic techniques directly as an impurity solver. It allows one to bypass the need of multiple perturbative series resummations within the DMFT self-consistency loop. It can be applied at or out of equilibrium, with any diagrammatic formalism, such as real times, imaginary times, or Matsubara frequencies formalisms. As a proof of principle, we illustrate our method with the half-filled Hubbard model on the Bethe lattice in the DMFT approximation, using Quantum Quasi-Monte Carlo (QQMC) to obtain the impurity perturbation series on the real time axis.

Characterizing complex many-body phases of matter has been a central question in quantum physics for decades. Numerical methods built around approximations of the renormalization group (RG) flow equations have offered reliable and systematically improvable answers to the initial question -- what simple physics drives quantum order and disorder? The flow equations are a very high dimensional set of coupled nonlinear equations whose solution is the two particle vertex function, a function of three continuous momenta that describes particle-particle scattering and encodes much of the low energy physics including whether the system exhibits various forms of long ranged order. In this work, we take a simple and interpretable data-driven approach to the open question of compressing the two-particle vertex. We use PCA and an autoencoder neural network to derive compact, low-dimensional representations of underlying physics for the case of interacting fermions on a lattice. We quantify errors in the representations by multiple metrics and show that a simple linear PCA offers more physical insight and better out-of-distribution (zero-shot) generalization than the nominally more expressive nonlinear models. Even with a modest number of principal components (10 - 20), we find excellent reconstruction of vertex functions across the phase diagram. This result suggests that many other many-body functions may be similarly compressible, potentially allowing for efficient computation of observables. Finally, we identify principal component subspaces that are shared between known phases, offering new physical insight.

Despite recent numerical evidence, one of the fundamental theoretical mysteries of polaritonic chemistry is how and if collective strong coupling can induce local changes of the electronic structure to modify chemical properties. Here we present non-perturbative analytic results for a model system consisting of an ensemble of N harmonic molecules under vibrational strong coupling (VSC) that alters our present understanding of this fundamental question. By applying the cavity Born-Oppenheimer partitioning on the Pauli-Fierz Hamiltonian in dipole approximation, the dressed many-molecule problem can be solved self-consistently and analytically in the dilute limit. We discover that the electronic molecular polarizabilities are modified even in the case of vanishingly small single-molecule couplings. Consequently, this non-perturbative local polarization mechanism persists even in the large-N limit. In contrast, a perturbative calculation of the polarizabilities leads to a qualitatively erroneous scaling behavior with vanishing effects in the large-N limit. Nevertheless, the exact (self-consistent) polarizabilities can be determined from single-molecule strong coupling simulations instead. Our fundamental theoretical observations demonstrate that hitherto existing collective-scaling arguments are insufficient for polaritonic chemistry and they pave the way for refined single- (or few-) molecule strong-coupling ab-initio simulations of chemical systems under collective strong coupling.

Due to the large-period superlattices emerging in moiré two-dimensional (2D) materials, electronic states in such systems exhibit low energy flat bands that can be used to simulate strongly correlated physics in a highly tunable setup. While many investigations have thus far focused on moiré flat bands and emergent correlated electron physics in triangular, honeycomb and quasi-one-dimensional lattices, tunable moiré realizations of square lattices subject to strong correlations remain elusive. Here we propose a feasible scheme to construct moire square lattice systems by twisting two layers of 2D materials in a rectangular lattice by 90 degrees. We demonstrate such scheme with twisted Ge/SnX (X=S,Se) moiré superlattices and theoretical calculate their electronic structures from first principles. We show that the lowest conduction flat band in these systems can be described by a square lattice Hubbard model with parameters which can be controlled by varying the choice of host materials, number of layers, and external electric fields. In particular, twisted double bilayer GeSe realizes a square lattice Hubbard model with strong frustration due to the next nearest neighbour hopping that could lead to unconventional superconductivity, in close analogy to the Hubbard model for copper-oxygen planes of cuprate high-temperature superconductors. The basic concept of using 90-degree twisted 2D materials with rectangular unit cell to realize the square lattice Hubbard model works in general and therefore we establish those systems as tunable platforms to simulate correlation physics in such a geometries.

We theoretically study dynamical excitonic condensates occurring in bilayers with an imposed chemical potential difference and in photodoped semiconductors. We show that optical spectroscopy can experimentally identify phase-trapped and phase-delocalized dynamical regimes of condensation. In the weak-bias regime, the trapped dynamics of the order parameter's phase lead to an in-gap absorption line at a frequency almost independent of the bias voltage, while for larger biases, the frequency of the spectral feature increases approximately linearly with bias. In both cases there is a pronounced second harmonic response. Close to the transition between the trapped and freely oscillating states, we find a strong response upon application of a weak electric probe field and compare the results to those found in a minimal model description for the dynamics of the order parameter's phase and analyze the limitations of the latter.

While superconductors are conventionally established by attractive interactions, higher-temperature mechanisms for emergent electronic pairing from strong repulsive electron-electron interactions remain under considerable scrutiny. Here, we establish a strong-coupling mechanism for intertwined superconductivity and magnetic order from purely repulsive interactions in a Kondo-like bilayer system, composed of a two-dimensional Mott insulator coupled to a layer of weakly-interacting itinerant electrons. Combining large scale DMRG and Monte Carlo simulations, we find that superconductivity persists and coexists with magnetism over a wide range of interlayer couplings. We classify the resulting rich phase diagram and find 2-rung antiferromagnetic and 4-rung antiferromagnetic order in one-dimensional systems along with a phase separation regime, while finding that superconductivity coexists with either antiferromagnetic or ferromagnetic order in two dimensions. Remarkably, the model permits a rigorous strong-coupling analysis via localized spins coupled to charge-2e bosons through Kugel-Khomskii interactions, capturing the pairing mechanism in the presence of magnetism due to emergent attractive interactions. Our numerical analysis reveals that pairing remains robust well beyond the strong-coupling regime, establishing a new mechanism for superconductivity in coupled weakly- and strongly-interacting electron systems, relevant for infinite-layer nickelates and superconductivity in moire multilayer heterostructures.