Ground State Correlations Research Articles

Monte Carlo methods in the manifold of Hartree-Fock-Bogoliubov wave functions.

We explore the possibility of implementing random walks in the manifold of Hartree-Fock-Bogoliubov wave functions. The goal is to extend state-of-the-art quantum Monte Carlo approaches, in particular the constrained-path auxiliary-field quantum Monte Carlo technique, to systems where finite pairing order parameters or complex pairing mechanisms, e.g., Fulde-Ferrell-Larkin-Ovchinnikov pairing or triplet pairing, may be expected. Leveraging the flexibility to define a vacuum state tailored to the physical problem, we discuss a method to use imaginary-time evolution of Hartree-Fock-Bogoliubov states to compute ground state correlations, extending beyond situations spanned by current formalisms. Illustrative examples are provided.

Quantum Algorithms for the Variational Optimization of Correlated Electronic States with Stochastic Reconfiguration and the Linear Method.

Solving the electronic Schrodinger equation for strongly correlated ground states is a long-standing challenge. We present quantum algorithms for the variational optimization of wave functions correlated by products of unitary operators, such as Local Unitary Cluster Jastrow (LUCJ) ansatzes, using stochastic reconfiguration (SR) and the linear method (LM). While an implementation on classical computing hardware would require exponentially growing compute cost, the cost (number of circuits and shots) of our quantum algorithms is polynomial in system size. We find that classical simulations of optimization with the linear method consistently find lower energy solutions than with the L-BFGS-B optimizer across the dissociation curves of the notoriously difficult N2 and C2 dimers; LUCJ predictions of the ground-state energies deviate from exact diagonalization by 1 kcal/mol or less at all points on the potential energy curve. While we do characterize the effect of shot noise on the LM optimization, these noiseless results highlight the critical but often overlooked role that optimization techniques must play in attacking the electronic structure problem (on both classical and quantum hardware), for which even mean-field optimization is formally NP hard. We also discuss the challenge of obtaining smooth curves in these strongly correlated regimes, and propose a number of quantum-friendly solutions ranging from symmetry-projected ansatz forms to a symmetry-constrained optimization algorithm.

Exploiting Non-Abelian Point-Group Symmetry to Estimate the Exact Ground-State Correlation Energy of Benzene in a Polarized Split-Valence Triple-Zeta Basis Set.

Local electronic-structure methods in quantum chemistry operate on the ability to compress electron correlations more efficiently in a basis of spatially localized molecular orbitals than in a parent set of canonical orbitals. However, many typical choices of localized orbitals tend to be related by selected, near-exact symmetry operations whenever a molecule belongs to a point group, a feature which remains largely unexploited in most local correlation methods. The present Letter demonstrates how to leverage a recent unitary protocol for enforcing symmetry properties among localized orbitals to yield a high-accuracy estimate of the exact ground-state correlation energy of benzene (D6h) in correlation-consistent polarized basis sets of both double- and triple-ζ quality. Through an initial application to many-body expanded full configuration interaction (MBE-FCI) theory, we show how molecular point-group symmetry can lead to computational savings that are inversely proportional to the order of the point group in a manner generally applicable to the acceleration of modern local correlation methods.

Beyond Electrons: Correlation and Self-Energy in Multicomponent Density Functional Theory.

Post-Kohn-Sham methods are used to evaluate the ground-state correlation energy and the orbital self-energy of systems consisting of multiple flavors of different fermions. Starting from multicomponent density functional theory, suitable ways to arrive at the corresponding multicomponent random-phase approximation and the multicomponent Green's function approximation, including relativistic effects, are outlined. Given the importance of both of this methods in the development of modern Kohn-Sham density functional approximations, this work will provide a foundation to design advanced multicomponent density functional approximations. Additionally, the quasiparticle energies are needed to study light-matter interactions with the Bethe-Salpeter equation.

Coexistence of Interacting Charge Density Waves in a Layered Semiconductor.

Coexisting orders are key features of strongly correlated materials and underlie many intriguing phenomena from unconventional superconductivity to topological orders. Here, we report the coexistence of two interacting charge-density-wave (CDW) orders in EuTe_{4}, a layered crystal that has drawn considerable attention owing to its anomalous thermal hysteresis and a semiconducting CDW state despite the absence of perfect Fermi surface nesting. By accessing unoccupied conduction bands with time- and angle-resolved photoemission measurements, we find that monolayers and bilayers of Te in the unit cell host different CDWs that are associated with distinct energy gaps. The two gaps display dichotomous evolutions following photoexcitation, where the larger bilayer CDW gap exhibits less renormalization and faster recovery. Surprisingly, the CDW in the Te monolayer displays an additional momentum-dependent gap renormalization that cannot be captured by density-functional theory calculations. This phenomenon is attributed to interlayer interactions between the two CDW orders, which account for the semiconducting nature of the equilibrium state. Our findings not only offer microscopic insights into the correlated ground state of EuTe_{4} but also provide a general nonequilibrium approach to understand coexisting, layer-dependent orders in a complex system.

Imaging moiré excited states with photocurrent tunnelling microscopy.

Moiré superlattices provide a highly tuneable and versatile platform to explore novel quantum phases and exotic excited states ranging from correlated insulators to moiré excitons. Scanning tunnelling microscopy has played a key role in probing microscopic behaviours of the moiré correlated ground states at the atomic scale. However, imaging of quantum excited states in moiré heterostructures remains an outstanding challenge. Here we develop a photocurrent tunnelling microscopy technique that combines laser excitation and scanning tunnelling spectroscopy to directly visualize the electron and hole distribution within the photoexcited moiré exciton in twisted bilayer WS2. The tunnelling photocurrent alternates between positive and negative polarities at different locations within a single moiré unit cell. This alternating photocurrent originates from the in-plane charge transfer moiré exciton in twisted bilayer WS2, predicted by our GW-Bethe-Salpeter equation calculations, that emerges from the competition between the electron-hole Coulomb interaction and the moiré potential landscape. Our technique enables the exploration of photoexcited non-equilibrium moiré phenomena at the atomic scale.

Spin skyrmion gaps as signatures of strong-coupling insulators in magic-angle twisted bilayer graphene

The flat electronic bands in magic-angle twisted bilayer graphene (MATBG) host a variety of correlated insulating ground states, many of which are predicted to support charged excitations with topologically non-trivial spin and/or valley skyrmion textures. However, it has remained challenging to experimentally address their ground state order and excitations, both because some of the proposed states do not couple directly to experimental probes, and because they are highly sensitive to spatial inhomogeneities in real samples. Here, using a scanning single-electron transistor, we observe thermodynamic gaps at even integer moiré filling factors at low magnetic fields. We find evidence of a field-tuned crossover from charged spin skyrmions to bare particle-like excitations, suggesting that the underlying ground state belongs to the manifold of strong-coupling insulators. From the spatial dependence of these states and the chemical potential variation within the flat bands, we infer a link between the stability of the correlated ground states and local twist angle and strain. Our work advances the microscopic understanding of the correlated insulators in MATBG and their unconventional excitations.

Controlling qubit-oscillator systems using linear parameter sweeps

We investigate the dynamics of a qubit-oscillator system under the influence of a linear sweep of system parameters. We consider two main cases. In the first case, we consider sweeping the parameters between the regime of a weakly correlated ground state and the regime of a strongly correlated ground state, a situation that can be viewed as a finite-duration quench between two phases of matter: the normal phase and the superradiant phase. Excitations are created as a result of this quench. We investigate the dependence of the excitation probabilities on the various parameters. We find a qualitative asymmetry in the dynamics between the cases of a normal-to-superradiant and superradiant-to-normal quench. The second case of parameter sweeps that we investigate is the problem of a Landau–Zener sweep in the qubit bias term for a qubit coupled to a harmonic oscillator. We analyze a theoretical formula based on the assumption that the dynamics can be decomposed into a sequence of independent Landau–Zener transitions. In addition to establishing the conditions of validity for the theoretical formula, we find that under suitable conditions, deterministic and robust multi-photon state preparation is possible in this system.

A Regularized Second-Order Correlation Method from Green's Function Theory.

We present a scalable single-particle framework to treat electronic correlation in molecules and materials motivated by Green's function theory. We derive a size-extensive Brillouin-Wigner perturbation theory from the single-particle Green's function by introducing the Goldstone self-energy. This new ground state correlation energy, referred to as Quasi-Particle MP2 theory (QPMP2), avoids the characteristic divergences present in both second-order Møller-Plesset perturbation theory and Coupled Cluster Singles and Doubles within the strongly correlated regime. We show that the exact ground state energy and properties of the Hubbard dimer are reproduced by QPMP2 and demonstrate the advantages of the approach for larger Hubbard models where the metal-to-insulator transition is qualitatively reproduced, contrasting with the complete failure of traditional methods. We apply this formalism to characteristic strongly correlated molecular systems and show that QPMP2 provides an efficient, size-consistent regularization of MP2.

Nuclear ground state correlations

The paper discusses ground state correlations (GSC) in nuclei, which are especially clearly manifested when using the formalism of quantum Green’s functions (FG) and Feynman diagrams. In addition to one-particleone-hole GSC, which appear in the well known random phase approximation method (RPA), there exist and give a noticeable quantitative contribution THE GSCs resulting from the use of configurations that are more complex than in RPA. Namely, configurations containing phonons and configurations containing only three quasiparticles, respectively, the GSC-phon and GSC3. This last case of GSC3 is considered in detail in the present paper. It is shown that GSC3 make a significant quantitative contribution IN THE problems related to the explanation of some characteristics of low-lying excited states (phonons) and transitions between them in even-even nuclei.

Competition between antiferromagnetism and superconductivity in a doped Hubbard model with anisotropic interaction

The competition between antiferromagnetism and superconductivity is one of the central questions in the research of strong correlated systems. In this work, we utilize a double layer model containing Hubbard interaction and interlayer Heisenberg interaction to reveal their competitions. This model is free of sign problem at certain conditions, and we perform projector quantum Monte Carlo simulations to extract the ground state correlations of magnetism and superconductivity. Our results shows that the superconductivity emerges when the antiferromagnetism is suppressed by tuning the filling or the anisotropy of the interlayer Heisenberg interaction. This model can be seen as an analogue of unconventional superconductors and may help us to understand the transition from an antiferromagnetic insulator to a superconductor.

Ground-state and spectral properties of the doped one-dimensional optical Hubbard-Su-Schrieffer-Heeger model

We present a density matrix renormalization group study of the doped one-dimensional (1D) Hubbard-Su-Schrieffer-Heeger (Hubbard-SSH) model, where the atomic displacements linearly modulate the nearest-neighbor hopping integrals. Focusing on an optical variant of the model in the strongly correlated limit relevant for cuprate spin chains, we examine how the SSH interaction modifies the model's ground- and excited-state properties. The SSH coupling weakly renormalizes the model's single- and two-particle response functions for electron-phonon $(e\text{\ensuremath{-}}\mathrm{ph})$ coupling strengths below a parameter-dependent critical value ${g}_{\mathrm{c}}$. For larger $e\text{\ensuremath{-}}\mathrm{ph}$ coupling, the sign of the effective hopping integrals changes for a subset of orbitals, which drives a lattice dimerization distinct from the standard nesting-driven picture in 1D. The spectral weight of the one- and two-particle dynamical response functions are dramatically rearranged across this transition, with significant changes in the ground-state correlations. We argue that this dimerization results from the breakdown of the linear approximation for the $e\text{\ensuremath{-}}\mathrm{ph}$ coupling and thus signals a fundamental limitation of the linear SSH interaction. Our results have consequences for our understanding of how SSH-like interactions can enter the physics of strongly correlated quantum materials, including the recently synthesized doped cuprate spin chains.

Nuclear Ground State Correlations

Nuclear Ground State Correlations

Even-odd effects in the J1−J2 SU(N) Heisenberg spin chain

The zero-temperature phase diagram of the ${J}_{1}\text{\ensuremath{-}}{J}_{2}\phantom{\rule{4pt}{0ex}}\mathrm{SU}(N)$ antiferromagnetic Heisenberg spin chain is investigated by means of complementary field theory and numerical approaches for general $N$. A fully gapped $\mathrm{SU}(N)$ valence bond solid made of $N$ sites is formed above a critical value of ${J}_{2}/{J}_{1}$ for all $N$. We find that the extension of this $N$-merized phase for larger values of ${J}_{2}$ strongly depends on the parity of $N$. For even $N$, the phase smoothly interpolates to the large ${J}_{2}$ regime where the model can be viewed as a zigzag $\mathrm{SU}(N)$ two-leg spin ladder. The phase exhibits both a $N$-merized ground state and incommensurate spin-spin correlations. In stark contrast to the even case, we show that the $N$-merized phase with odd $N$ has only a finite extent with no incommensuration. A gapless phase in the $\mathrm{SU}{(N)}_{1}$ universality class is stabilized for larger ${J}_{2}$ that stems from the existence of a massless renormalization group flow from $\mathrm{SU}{(N)}_{2}$ to $\mathrm{SU}{(N)}_{1}$ conformal field theories when $N$ is odd.

Fractional topology in interacting one-dimensional superconductors

We investigate the topological phases of two one-dimensional (1D) interacting superconducting wires and propose topological markers directly measurable from ground-state correlation functions. These quantities remain powerful tools in the presence of couplings and interactions. We show with the density matrix renormalization group that the double critical Ising (DCI) phase of two interacting Kitaev chains is a fractional topological phase with gapless Majorana modes in the bulk, and a one-half topological invariant per wire. Using both numerics and quantum field theoretical methods, we show that the phase diagram remains stable in the presence of an interwire hopping amplitude ${t}_{\ensuremath{\perp}}$ at length scales below $\ensuremath{\sim}1/{t}_{\ensuremath{\perp}}$. A large interwire hopping amplitude results in the emergence of two integer topological phases, stable also at large interactions. They host one edge mode per boundary shared between both wires. At large interactions, the two wires are described by Mott physics, with the ${t}_{\ensuremath{\perp}}$ hopping amplitude resulting in a paramagnetic order.

Multipartite information of free fermions on Hamming graphs

We investigate multipartite information and entanglement measures in the ground state of a free-fermion model defined on a Hamming graph. Using the known diagonalization of the adjacency matrix, we solve the model and construct the ground-state correlation matrix. Moreover, we find all the eigenvalues of the chopped correlation matrix when the subsystem consists of n disjoint Hamming subgraphs embedded in a larger one. These results allow us to find an exact formula for the entanglement entropy of disjoint graphs, as well as for the mutual and tripartite information. We use the exact formulas for these measures to extract their asymptotic behavior in two distinct thermodynamic limits, and find excellent match with the numerical calculations. In particular, we find that the entanglement entropy admits a logarithmic violation of the area law which decreases the amount of entanglement compared to the area law scaling.

Electronic Excited States in Extreme Limits via Ensemble Density Functionals.

Density functional theory (DFT) has greatly expanded our ability to affordably compute and understand electronic ground states, by replacing intractable abinitio calculations by models based on paradigmatic physics from high- and low-density limits. But, a comparable treatment of excited states lags behind. Here, we solve this outstanding problem by employing a generalization of density functional theory to ensemble states (EDFT). We thus address important paradigmatic cases of all electronic systems in strongly (low-density) and weakly (high-density) correlated regimes. We show that the high-density limit connects to recent, exactly solvable EDFT results. The low-density limit reveals an unnoticed and most unexpected result-density functionals for strictly correlated ground states can be reused directly for excited states. Nontrivial dependence on excitation structure only shows up at third leading order. Overall, our results provide foundations for effective models of excited states that interpolate between exact low- and high-density limits, which we illustrate on the cases of singlet-singlet excitations in H_{2} and a ring of quantum wells.

Long-Range Free Fermions: Lieb-Robinson Bound, Clustering Properties, and Topological Phases.

We consider free fermions living on lattices in arbitrary dimensions, where hopping amplitudes follow a power-law decay with respect to the distance. We focus on the regime where this power is larger than the spatial dimension (i.e., where the single particle energies are guaranteed to be bounded) for which we provide a comprehensive series of fundamental constraints on their equilibrium and nonequilibrium properties. First, we derive a Lieb-Robinson bound which is optimal in the spatial tail. This bound then implies a clustering property with essentially the same power law for the Green's function, whenever its variable lies outside the energy spectrum. The widely believed (but yet unproven in this regime) clustering property for the ground-state correlation function follows as a corollary among other implications. Finally, we discuss the impact of these results on topological phases in long-range free-fermion systems: they justify the equivalence between Hamiltonian and state-based definitions and the extension of the short-range phase classification to systems with decay power larger than the spatial dimension. Additionally, we argue that all the short-range topological phases are unified whenever this power is allowed to be smaller.

Spin disorder in a stacking polytype of a layered magnet

Strongly correlated ground states and exotic quasiparticle excitations in low-dimensional systems are central research topics in the solid-state research community. The present work develops a layered material and explores the physical properties. Single crystals of $3R\text{\ensuremath{-}}{\mathrm{Na}}_{2}\mathrm{MnTe}{\mathrm{O}}_{6}$ were synthesized via a flux method. Single-crystal x-ray diffraction and transmission electron microscopy reveal a crystal structure with ABC-type stacking and an $R\text{\ensuremath{-}}3$ space group, which establishes this material as a stacking polytype to previously reported $2H\text{\ensuremath{-}}{\mathrm{Na}}_{2}\mathrm{MnTe}{\mathrm{O}}_{6}$. Magnetic- and heat-capacity measurements demonstrate dominant antiferromagnetic interactions, the absence of long-range magnetic order down to 0.5 K, and field-dependent short-range magnetic correlations. A structural transition at $\ensuremath{\sim}23$ K observed in dielectric measurements may be related to displacements of the Na positions. Our results demonstrate that $3R\text{\ensuremath{-}}{\mathrm{Na}}_{2}\mathrm{MnTe}{\mathrm{O}}_{6}$ displays low-dimensional magnetism, disordered structure and spins, and the system displays a rich structure variety.

A highly correlated topological bubble phase of composite fermions

Strong interactions and topology drive a wide variety of correlated ground states. Some of the most interesting of these ground states, such as fractional quantum Hall states and fractional Chern insulators, have fractionally charged quasiparticles. Correlations in these phases are captured by the binding of electrons and vortices into emergent particles called composite fermions. Composite fermion quasiparticles are randomly localized at high levels of disorder and may exhibit charge order when there is not too much disorder in the system. However, more complex correlations are predicted when composite fermion quasiparticles cluster into a bubble, and then these bubbles order on a lattice. Such a highly correlated ground state is termed the bubble phase of composite fermions. Here we report the observation of such a bubble phase of composite fermions, evidenced by the re-entrance of the fractional quantum Hall effect. We associate this re-entrance with a bubble phase with two composite fermion quasiparticles per bubble. Our results demonstrate the existence of a new class of strongly correlated topological phases driven by clustering and charge ordering of emergent quasiparticles. Composite fermions emerge in the fractional quantum Hall effect. Now, it has been shown that these objects can group into bubbles and that these can order into a lattice.