Many-body Correlations Research Articles

Insight into the Density-Dependence of Pair Potentials for Predictive Coarse-Grained Models.

We investigate the temperature- and density-dependence of effective pair potentials for 1-site coarse-grained (CG) models of two industrial solvents, 1,4-dioxane and tetrahydrofuran. We observe that the calculated pair potentials are much more sensitive to density than to temperature. The generalized-Yvon-Born-Green framework reveals that this striking density-dependence reflects corresponding variations in the many-body correlations that determine the environment-mediated indirect contribution to the pair mean force. Moreover, we demonstrate, perhaps surprisingly, that this density-dependence is not important for accurately modeling the intermolecular structure. Accordingly, we adopt a density-independent interaction potential and transfer the density-dependence of the calculated pair potentials into a configuration-independent volume potential. Furthermore, we develop a single global potential that accurately models the intermolecular structure and pressure-volume equation of state across a very wide range of liquid state points. Consequently, this work provides fundamental insight into the density-dependence of effective pair potentials and also provides a significant step toward developing predictive CG models for efficiently modeling industrial solvents.

Development of a machine learning finite-range nonlocal density functional.

Kohn-Sham density functional theory has been the most popular method in electronic structure calculations. To fulfill the increasing accuracy requirements, new approximate functionals are needed to address key issues in existing approximations. It is well known that nonlocal components are crucial. Current nonlocal functionals mostly require orbital dependence such as in Hartree-Fock exchange and many-body perturbation correlation energy, which, however, leads to higher computational costs. Deviating from this pathway, we describe functional nonlocality in a new approach. By partitioning the total density to atom-centered local densities, a many-body expansion is proposed. This many-body expansion can be truncated at one-body contributions, if a base functional is used and an energy correction is approximated. The contribution from each atom-centered local density is a single finite-range nonlocal functional that is universal for all atoms. We then use machine learning to develop this universal atom-centered functional. Parameters in this functional are determined by fitting to data that are produced by high-level theories. Extensive tests on several different test sets, which include reaction energies, reaction barrier heights, and non-covalent interaction energies, show that the new functional, with only the density as the basic variable, can produce results comparable to the best-performing double-hybrid functionals, (for example, for the thermochemistry test set selected from the GMTKN55 database, BLYP based machine learning functional gives a weighted total mean absolute deviations of 3.33kcal/mol, while DSD-BLYP-D3(BJ) gives 3.28kcal/mol) with a lower computational cost. This opens a new pathway to nonlocal functional development and applications.

Quantum embedding for molecules using auxiliary particles - the ghost Gutzwiller Ansatz.

Strong/static electronic correlation mediates the emergence of remarkable phases of matter, and underlies the exceptional reactivity properties in transition metal-based catalysts. Modeling strongly correlated molecules and solids calls for multi-reference Ansätze, which explicitly capture the competition of energy scales characteristic of such systems. With the efficient computational screening of correlated solids in mind, the ghost Gutzwiller (gGut) Ansatz has been recently developed. This is a variational Ansatz which can be formulated as a self-consistent embedding approach, describing the system within a non-interacting, quasiparticle model, yet providing accurate spectra in both low and high energy regimes. Crucially, small fragments of the system are identified as responsible for the strong correlation, and are therefore enhanced by adding a set of auxiliary orbitals, the ghosts. These capture many-body correlations through one-body fluctuations and subsequent out-projection when computing physical observables. gGut has been shown to accurately describe multi-orbital lattice models at modest computational cost. In this work, we extend the gGut framework to strongly correlated molecules, for which it holds special promise. Indeed, despite the asymmetric embedding treatment, the quasiparticle Hamiltonian effectively describes all major sources of correlation in the molecule: strong correlation through the ghosts in the fragment, and dynamical correlation through the quasiparticle description of its environment. To adapt the gGut Ansatz for molecules, we address the fact that, unlike in the lattice model previously considered, electronic interactions in molecules are not local. Hence, we explore a hierarchy of approximations of increasing accuracy capturing interactions between fragments and environment, and within the environment, and discuss how these affect the embedding description of correlations in the whole molecule. We will compare the accuracy of the gGut model with established methods to capture strong correlation within active space formulations, and assess the realistic use of this novel approximation to the theoretical description of correlated molecular clusters.

Many-body correlations for nuclear physics across scales: from nuclei to quark-gluon plasmas to hadron distributions

It is an experimental fact that multi-particle correlations in the final states of high-energy nucleus-nucleus collisions are sensitive to collective correlations of nucleons in the wave functions of the colliding nuclei. Here, I show that this connection is more direct than it intuitively seems. With an energy deposition scheme inspired by high-energy quantum chromodynamics, and within a linearized description of initial-state fluctuations in the quark-gluon plasma, I exhibit relations between N-particle correlations in the final states of nuclear collisions and N-nucleon density distributions in the colliding nuclei. This result formally justifies the sensitivity of the outcome of high-energy collisions to features such as nuclear deformations. It paves the way, thus, to systematic studies of the impact of state-of-the-art nuclear interactions in such processes.

Potential energy surface and quantum dynamics calculation of SH2− (2A′) based on ab initio scaled external correlation correction

An accurate interatomic potential energy surface for ground state of SH2− is reported at the multireference configuration interaction level of theory using aug–cc–pVQZ basis set. The calculated ab initio energy points are utilized, after semi-empirically correcting the dynamical correlation by the many-body expansion-scaled external correlation method. To verify the accuracy of the potential energy surface, molecular reaction dynamics, including the relationship between reaction probability and collision energy, thermal rate constant, and integral scattering cross section are calculated by using the quantum time-dependent wave packet method. The final results show that our potential energy surface is accurate and the molecular reaction dynamics results are satisfactory, and the accurate potential energy surface and its dynamics results can also lay a foundation for the future experimental research of SH−-containing molecules.

Gaussian representation of coarse-grained interactions of liquids: Theory, parametrization, and transferability.

Coarse-grained (CG) interactions determined via bottom-up methodologies can faithfully reproduce the structural correlations observed in fine-grained (atomistic resolution) systems, yet they can suffer from limited extensibility due to complex many-body correlations. As part of an ongoing effort to understand and improve the applicability of bottom-up CG models, we propose an alternative approach to address both accuracy and transferability. Our main idea draws from classical perturbation theory to partition the hard sphere repulsive term from effective CG interactions. We then introduce Gaussian basis functions corresponding to the system's characteristic length by linking these Gaussian sub-interactions to the local particle densities at each coordination shell. The remaining perturbative long-range interaction can be treated as a collective solvation interaction, which we show exhibits a Gaussian form derived from integral equation theories. By applying this numerical parametrization protocol to CG liquid systems, our microscopic theory elucidates the emergence of Gaussian interactions in common phenomenological CG models. To facilitate transferability for these reduced descriptions, we further infer equations of state to determine the sub-interaction parameter as a function of the system variables. The reduced models exhibit excellent transferability across the thermodynamic state points. Furthermore, we propose a new strategy to design the cross-interactions between distinct CG sites in liquid mixtures. This involves combining each Gaussian in the proper radial domain, yielding accurate CG potentials of mean force and structural correlations for multi-component systems. Overall, our findings establish a solid foundation for constructing transferable bottom-up CG models of liquids with enhanced extensibility.

Nuclear Equation of State and many-body phase-space correlations in the Constrained Molecular Dynamics

Many-body correlations characterizing the Constrained Molecular Dynamics (CoMD) are analyzed in the case of finite and zero-range effective microscopic interactions. The study begins by analyzing the case of infinite nuclear matter at zero temperature. A comparison with the predictions in the mean-field (MF) limit corresponding to different effective masses, highlights non-negligible differences regarding the produced Equation of State (EoS). A procedure is illustrated to determine the necessary corrections of the effective interaction parameters in the CoMD model so to reproduce the chosen EoS. The specific model calculations, the general feature of the discussed correlations gives a wider meaning to the resulting differences, which are in fact strongly related both to the Pauli principle constraint and to the localization effects related to wave-packets dynamics. Moving on to finite systems, preliminary results are shown in relation to the reaction mechanisms in the N64i+48Ca system described by the CoMD model. Therefore, the topic covered illustrates the effects produced by the correlations of the CoMD dynamics on the EoS and on some observables commonly studied in heavy ion collisions.

Picosecond-Scale Ultrafast Many-Body Dynamics in an Ultracold Rydberg-Excited Atomic Mott Insulator.

We report the observation and control of ultrafast many-body dynamics of electrons in ultracold Rydberg-excited atoms, spatially ordered in a three-dimensional Mott insulator (MI) with unity filling in an optical lattice. By mapping out the time-domain Ramsey interferometry in the picosecond timescale, we can deduce entanglement growth indicating the emergence of many-body correlations via dipolar forces. We analyze our observations with different theoretical approaches and find that the semiclassical model breaks down, thus indicating that quantum fluctuations play a decisive role in the observed dynamics. Combining picosecond Rydberg excitation with MI lattice thus provides a platform for simulating nonequilibrium dynamics of strongly correlated systems in synthetic ultracold atomic crystals, such as in a metal-like quantum gas regime.

Soft pinning: Experimental validation of static correlations in supercooled molecular glass-forming liquids.

Enormous enhancement in the viscosity of a liquid near its glass transition is a hallmark of glass transition. Within a class of theoretical frameworks, it is connected to growing many-body static correlations near the transition, often called "amorphous ordering." At the same time, some theories do not invoke the existence of such a static length scale in the problem. Thus, proving the existence and possible estimation of the static length scales of amorphous order in different glass-forming liquids is very important to validate or falsify the predictions of these theories and unravel the true physics of glass formation. Experiments on molecular glass-forming liquids become pivotal in this scenario as the viscosity grows several folds (), and simulations or colloidal glass experiments fail to access these required long-time scales. Here we design an experiment to extract the static length scales in molecular liquids using dilute amounts of another large molecule as a pinning site. Results from dielectric relaxation experiments on supercooled Glycerol with different pinning concentrations of Sorbitol and Glucose, as well as the simulations on a few model glass-forming liquids with pinning sites, indicate the versatility of the proposed method, opening possible new avenues to study the physics of glass transition in other molecular liquids.

Exact results of dynamical structure factor of Lieb–Liniger model

The dynamical structure factor (DSF) represents a measure of dynamical density–density correlations in a quantum many-body system. Due to the complexity of many-body correlations and quantum fluctuations in a system of an infinitely large Hilbert space, such kind of dynamical correlations often impose a big theoretical challenge. For one-dimensional (1D) quantum many-body systems, qualitative predictions of dynamical response functions are usually carried out by using the Tomonaga–Luttinger liquid (TLL) theory. In this scenario, a precise evaluation of the DSF for a 1D quantum system with arbitrary interaction strength remains a formidable task. In this paper, we use the form factor approach based on algebraic Bethe ansatz theory to calculate precisely the DSF of Lieb–Liniger model with an arbitrary interaction strength at a large scale of particle number. We find that the DSF for a system as large as 2000 particles enables us to depict precisely its line-shape from which the power-law singularity with corresponding exponents in the vicinities of spectral thresholds naturally emerge. It should be noted that, the advantage of our algorithm promises an access to the threshold behavior of dynamical correlation functions, further confirming the validity of nonlinear TLL theory besides Kitanine et al (2012 J. Stat. Mech. P09001). Finally we discuss a comparison of results with the results from the ABACUS method by J-S Caux (2009 J. Math. Phys. 50 095214) as well as from the strongly coupling expansion by Brand and Cherny (2005 Phys. Rev. A 72 033619).

Efficient solutions of fermionic systems using artificial neural networks

In this study, we explore the similarities and differences between variational Monte Carlo techniques that employ conventional and artificial neural network representations of the ground-state wave function for fermionic systems. Our primary focus is on shallow neural network architectures, specifically the restricted Boltzmann machine, and we examine unsupervised learning algorithms that are appropriate for modeling complex many-body correlations. We assess the advantages and drawbacks of conventional and neural network wave functions by applying them to a range of circular quantum dot systems. Our findings, which include results for systems containing up to 90 electrons, emphasize the efficient implementation of these methods on both homogeneous and heterogeneous high-performance computing facilities.

Many-body correlations in one-dimensional optical lattices with alkaline-earth(-like) atoms

We explore the rich nature of correlations in the ground state of ultracold atoms trapped in state-dependent optical lattices. In particular, we consider interacting fermionic ytterbium or strontium atoms, realizing a two-orbital Hubbard model with two spin components. We analyze the model in one-dimensional setting with the experimentally relevant hierarchy of tunneling and interaction amplitudes by means of exact diagonalization and matrix product states approaches, and study the correlation functions in density, spin, and orbital sectors as functions of variable densities of atoms in the ground and metastable excited states. We show that in certain ranges of densities these atomic systems demonstrate strong density-wave, ferro- and antiferromagnetic, as well as antiferroorbital correlations.

Higher-order mean-field theory of chiral waveguide QED

Waveguide QED with cold atoms provides a potent platform for the study of non-equilibrium, many-body, and open-system quantum dynamics. Even with weak coupling and strong photon loss, the collective enhancement of light-atom interactions leads to strong correlations of photons arising in transmission, as shown in recent experiments. Here we apply an improved mean-field theory based on higher-order cumulant expansions to describe the experimentally relevant, but theoretically elusive, regime of weak coupling and strong driving of large ensembles. We determine the transmitted power, squeezing spectra and the degree of second-order coherence, and systematically check the convergence of the results by comparing expansions that truncate cumulants of few-particle correlations at increasing order. This reveals the important role of many-body and long-range correlations between atoms in steady state. Our approach allows to quantify the trade-off between anti-bunching and output power in previously inaccessible parameter regimes. Calculated squeezing spectra show good agreement with measured data, as we present here.

Implementing Jastrow-Gutzwiller operators on a quantum computer using the cascaded variational quantum eigensolver algorithm

A Jastrow-Gutzwiller operator adds many-body correlations to a quantum state. However, the operator is nonunitary, making it difficult to implement directly on a quantum computer. We present an implementation of the Jastrow-Gutzwiller operator using the cascaded variational quantum eigensolver algorithm. We demonstrate the method on IBM Q Lagos for a Hubbard model.

Emergent structural correlations in dense liquids.

The complete quantitative description of the structure of dense and supercooled liquids remains a notoriously difficult problem in statistical physics. Most studies to date focus solely on two-body structural correlations, and only a handful of papers have sought to consider additional three-body correlations. Here, we go beyond the state of the art by extracting many-body static structure factors from molecular dynamics simulations and by deriving accurate approximations up to the six-body structure factor via density functional theory. We find that supercooling manifestly increases four-body correlations, akin to the two- and three-body case. However, at small wave numbers, we observe that the four-point structure of a liquid drastically changes upon supercooling, both qualitatively and quantitatively, which is not the case in two-point structural correlations. This indicates that theories of the structure or dynamics of dense liquids should incorporate many-body correlations beyond the two-particle level to fully capture their intricate behavior.

Nuclear many-body effects on particle emission following muon capture on Si28 and Ca40

Background: Muon captures on nuclei have provided us with plenty of knowledge of nuclear properties. Recently, this reaction attracts attention in electronics, because charged particle emissions following muon capture on silicon become to trigger non-negligible soft errors in memory devices.Purpose: To date, there is no theoretical framework based on the nuclear structure that describes a muon capture reaction followed by particle emissions comprehensively. The purpose of this work is to develop a new method that considers the nuclear many-body correlation for the accurate understanding of the soft errors in memory devices.Method: We combined the second Tamm-Dancoff approximation that is used to estimate muon capture rates with the two-component exciton model, the model describing particle emission from the pre-equilibrium state. For particle evaporation from the compound state, the Hauser-Feshbach statistical models were applied. We chose $^{28}\mathrm{Si}$ and $^{40}\mathrm{Ca}$ to check the performance of the framework.Result: We paid attention to the muon capture rates, the particle emission spectra, and the multiplicities that have a close interrelation with each other. We found that the nuclear many-body correlations including two-particle two-hole excitations is a key to explaining them simultaneously.Conclusion: The present study showed that the combination of the microscopic approach of muon capture and the two-component exciton model of particle emission is an effective tool to describe particle emission following the muon captures, giving the nuclear structure information additionally. For a finer understanding of particle emission following muon capture and a validation of the present framework, further experimental studies on particle emission spectra are highly expected.

A finite element configuration interaction method for Wigner localization

The Wigner localization is an electron phase at low densities when the electrons are sharply localized around equilibrium positions. The simulation of the Wigner localization phenomenon requires careful treatment of the many-body correlations, as the electron-electron interaction dominates the system. This work proposes a numerical algorithm to study the electron ground states of the Wigner localized systems. The main features of our algorithm are three-fold: (i) a finite element discretization of the one-body space such that the sharp localization can be captured; (ii) a good initial state obtained by exploiting the strongly correlated limit; and (iii) a selected configuration interaction method by choosing the Slater determinants from (stochastic) gradients. Numerical experiments for some typical low-dimensional systems are provided to show the efficiency of our algorithm.

Extracting electronic many-body correlations from local measurements with artificial neural networks

The characterization of many-body correlations provides a powerful tool for analyzing correlated quantum materials. However, experimental extraction of quantum entanglement in correlated electronic systems remains an open problem in practice. In particular, the correlation entropy quantifies the strength of quantum correlations in interacting electronic systems, yet it requires measuring all the single-particle correlators of a macroscopic sample. To circumvent this bottleneck, we introduce a strategy to obtain the correlation entropy of electronic systems solely from a set of local measurements. We show that, by combining local particle-particle and density-density correlations with a neural-network algorithm, the correlation entropy can be predicted accurately. Specifically, we show that for a generalized interacting fermionic model, our algorithm yields an accurate prediction of the correlation entropy from a set of noisy local correlators. Our work shows that the correlation entropy in interacting electron systems can be reconstructed from local measurements, providing a starting point to experimentally extract many-body correlations with local probes.

Pulse overlap artifacts and double quantum coherence spectroscopy.

The double quantum coherence (DQC) signal in nonlinear spectroscopy gives information about the many-body correlation effects not easily available by other methods. The signal is short-lived, consequently, a significant part of it is generated during the pulse overlap. Since the signal is at two times the laser frequency, one may intuitively expect that the pulse overlap-related artifacts are filtered out by the Fourier transform. Here, we show that this is not the case. We perform explicit calculations of phase-modulated two-pulse experiments of a two-level system where the DQC is impossible. Still, we obtain a significant signal at the modulation frequency, which corresponds to the DQC, while the Fourier transform over the pulse delay shows a double frequency. We repeat the calculations with a three-level system where the true DQC signal occurs. We conclude that with realistic dephasing times, the pulse-overlap artifact can be significantly stronger than the DQC signal. Our results call for great care when analyzing such experiments. As a rule of thumb, we recommend that only delays larger than 1.5 times the pulse length should be used.

Entanglement at the interplay between single- and many-bodyness

The tensor network representation of the ground state of a Bethe chain is analytically obtained and studied in relation to its entanglement distribution. Block entanglement displays a maximum at the interplay between single- and many-bodyness. In systems of two fermions, tensor networks describing states with substantial many-body entropy cannot be written as a sequence of next-neighbor unitaries applied on an uncorrelated state, but need four-next-neighbor unitaries in addition. This differs from the idea that ground states can be obtained as a sequence of next-neighbor operations applied on an initial tensor network lacking many-body correlations. The work uncovers the transcendence of the notion of many-bodyness in the implementation of protocols based on matrix product states.