One-particle Green Function Research Articles

Quantum Algorithm for Imaginary-Time Green's Functions.

Green's function methods lead to ab initio, systematically improvable simulations of molecules and materials while providing access to multiple experimentally observable properties such as the density of states and the spectral function. The calculation of the exact one-particle Green's function remains a significant challenge for classical computers and was attempted only on very small systems. Here, we present a hybrid quantum-classical algorithm to calculate the imaginary-time one-particle Green's function. The proposed algorithm combines the variational quantum eigensolver and the quantum subspace expansion methods to calculate Green's function in Lehmann's representation. We demonstrate the validity of this algorithm by simulating H2 and H4 on quantum simulators and on IBM's quantum devices.

Four-gluon vertex from lattice QCD

A lattice QCD calculation for the four-gluon one-particle irreducible Green function in the Landau gauge is discussed. Results for some of the associated form factors are reported for kinematical configurations with a single momentum scale. Our results show that the computation of this Green function requires large statistical ensembles with 10 K or larger number of gauge configurations. The simulations considered herein have a clear Monte Carlo signal for momenta up to ∼1 GeV. The form factors show an hierarchy, with the form factor associated with the tree level Feynman rule being dominant and essentially constant for the range of momenta accessed. The remaining form factors seem to increase as the momentum decreases, suggesting that a possible log divergence may occur. The computed form factors are, at least, in qualitative agreement with the results obtained with continuum approaches to this vertex, when available. Published by the American Physical Society 2024

Algebraic Diagrammatic Construction Theory for Simulating Charged Excited States and Photoelectron Spectra.

Charged excitations are electronic transitions that involve a change in the total charge of a molecule or material. Understanding the properties and reactivity of charged species requires insights from theoretical calculations that can accurately describe orbital relaxation and electron correlation effects in open-shell electronic states. In this Review, we describe the current state of algebraic diagrammatic construction (ADC) theory for simulating charged excitations and its recent developments. We start with a short overview of ADC formalism for the one-particle Green's function, including its single- and multireference formulations and extension to periodic systems. Next, we focus on the capabilities of ADC methods and discuss recent findings about their accuracy for calculating a wide range of excited-state properties. We conclude our Review by outlining possible directions for future developments of this theoretical approach.

One-particle Green's functions from the quantum equation of motion algorithm

Many-body Green's functions encode all the properties and excitations of interacting electrons. While these are challenging to be evaluated accurately on a classical computer, recent efforts have been directed towards finding quantum algorithms that may provide a quantum advantage for this task, exploiting architectures that will become available in the near future. In this work we introduce a novel near-term quantum algorithm for computing one-particle Green's functions via their Lehmann representation. The method is based on a generalization of the quantum equation of motion algorithm that gives access to the charged excitations of the system. We demonstrate the validity of the present proposal by computing the Green's function of a two-site Fermi-Hubbard model on a IBM quantum processor.

Intralayer charge-transfer moiré excitons in van der Waals superlattices.

Moiré patterns of transition metal dichalcogenide heterobilayers have proved to be an ideal platform on which to host unusual correlated electronic phases, emerging magnetism and correlated exciton physics. Whereas the existence of new moiré excitonic states is established1-4 through optical measurements, the microscopic nature of these states is still poorly understood, often relying on empirically fit models. Here, combining large-scale first-principles GW (where G and W denote the one-particle Green's function and the screened Coulomb interaction, respectively) plus Bethe-Salpeter calculations and micro-reflection spectroscopy, we identify the nature of the exciton resonances in WSe2/WS2 moiré superlattices, discovering a rich set of moiré excitons that cannot be captured by prevailing continuum models. Our calculations show moiré excitons with distinct characters, including modulated Wannier excitons and previously unidentified intralayer charge-transfer excitons. Signatures of these distinct excitonic characters are confirmed experimentally by the unique carrier-density and magnetic-field dependences of different moiré exciton resonances. Our study highlights the highly non-trivial exciton states that can emerge in transition metal dichalcogenide moiré superlattices, and suggests new ways of tuning many-body physics in moiré systems by engineering excited-states with specific spatial characters.

Algebraic equation of motion approach for solving the Anderson model

Based on the algebraic equation of motion (AEOM) approach, we have studied the single-impurity Anderson model by analytically solving the AEOM of the f-electron one-particle Green function in the Kondo limit. The related spectral function satisfies the sum rule and shows that there is a well-known three-peak structure at zero temperature. In the low energy limit, we obtain the analytical formula of the Kondo temperature that is the same as the exact solution in form except for a prefactor. We also show that the shape of the Kondo resonance is the Lorentzian form and the corresponding weight is proportional to the spin-flip correlation function.

Cumulant methods for electron-phonon problems. I. Perturbative expansions

In this work we investigate the ability of the cumulant expansion (CE) to capture one-particle spectral information in electron-phonon coupled systems at both zero and finite temperatures. In particular, we present a comprehensive study of the second- and fourth-order CE for the one-dimensional Holstein model as compared with numerically exact methods. We investigate both finite sized systems as well as the approach to the thermodynamic limit, drawing distinctions and connections between the behavior of systems in and away from the thermodynamic limit that enable a greater understanding of the ability of the CE to capture real-frequency information across the full range of wave vectors. We find that for zero electronic momentum, the spectral function is well described by the second-order CE at low and high temperatures. However, for non-zero electronic momenta, the CE is only accurate at high temperature. We analyze the fourth-order cumulant, and find that while it improves the description of the short-time dynamics encoded in the one-particle Green's function, it can introduce divergences in the time domain as well as unphysical negative spectral weight in the spectral function. When well-behaved, the fourth-order CE does provide notable accurate corrections to the second-order CE. Finally, we use our results to comment on the use of the CE as a tool for calculating transport behavior in the realistic ab initio modeling of materials.

Time-dependent exchange-correlation potential in lieu of self-energy

It is shown that the equation of motion of the one-particle Green function of an interacting many-electron system is governed by a multiplicative time-dependent exchange-correlation potential, which is the Coulomb potential of a time-dependent exchange-correlation hole. This exchange-correlation hole fulfills a sum rule, a generalization of the well-known sum rule of the static exchange-correlation hole. It is envisaged that the proposed formalism may provide an alternative route for calculating the Green function by finding a suitable approximation for the exchange-correlation hole or potential based on, e.g., a local-density approximation.

Non-Markovian transients in transport across chiral quantum wires using space–time non-equilibrium Green functions

We study a system of two non-interacting quantum wires with fermions of opposite chirality with a point contact junction at the origin across which tunneling can take place when an arbitrary time-dependent bias between the wires is applied. We obtain the exact dynamical non-equilibrium Green function by solving Dyson’s equation analytically. Both the space–time dependent two and four-point functions are written down in a closed form in terms of simple functions of position and time. This allows us to obtain, among other things, the I–V characteristics for an arbitrary time-dependent bias. Our method is a superior alternative to competing approaches to non-equilibrium as we are able to account for transient phenomena as well as the steady state. We study the approach to steady state by computing the time evolution of the equal-time one-particle Green function. Our method can be easily applied to the problem of a double barrier contact whose internal properties can be adjusted to induce resonant tunneling leading to a conductance maximum. We then consider the case of a finite bandwidth in the point contact and calculate the non-equilibrium transport properties which exhibit non-Markovian behaviour. When a subsequently constant bias is suddenly switched on, the current shows a transient build up before approaching its steady state value in contrast to the infinite bandwidth case. This transient property is consistent with numerical simulations of lattice systems using time-dependent density matrix renormalization group suggesting thereby that this transient build up is merely due to the presence of a short distance cutoff in the problem description and not on the other details.

Diffusion-controlled annihilation reactions in 2D and 3D nanostructures

An analytical consideration of bimolecular reactions in nanostructures is presented. As a mathematical model, the two-particle Green's function approach for the diffusion problem with the Neumann boundary condition is proposed. Also, the special cases, when the solutions can be reduced to the simpler one-particle Green's function, are analysed. Despite such diffusion equations are almost always analytically intractable, Green's function technique allows to build an analytical expression for the distance-dependent annihilation rate. The observed model can describe non-spin-selective annihilation reactions and spin-selective annihilation reactions such as triplet–triplet annihilation (TTA) of excitons or quenching of triplets by doublet centers. Based on this model, the distance-dependent annihilation rates were calculated for circular (2D system) and spherical (3D system) nanostructures. As illustrations of this method, we show that the annihilation rate can be enhanced in circular and spherical nanostructures.

Fluctuations analysis of spin susceptibility: Néel ordering revisited in dynamical mean field theory

In this paper, we revisit the antiferromagnetic (AF) phase diagram of the single-band three-dimensional half-filled Hubbard model on a simple cubic lattice studied within the dynamical mean field theory (DMFT). Although this problem has been investigated extensively in the literature, a comprehensive understanding of the impact of the different one- and, in particular, two-particle local correlation functions of DMFT on the AF transition temperature is still missing. We have, hence, performed a fluctuation analysis of ${T}_{N}$ with respect to different local bosonic fluctuations (charge, spin, particle-particle) contained in the two-particle vertex of DMFT. Our results indicate that, beyond weak coupling, the screening of the DMFT vertex by local fluctuations leads to an enhancement of ${T}_{N}$ with respect to a random phase approximation (RPA) like calculation where this vertex is replaced by the bare interaction. The overall suppression of ${T}_{N}$ in DMFT with respect to RPA is then solely due to the incoherence introduced by the DMFT self-energy in the one-particle Green's functions. This illustrates the Janus-faced role of the local moment formation in the DMFT solution of the Hubbard model, which leads to completely opposite effects in the one- and two-particle correlation functions.

Self-energy method for time-dependent spectral functions of the Anderson impurity model within the time-dependent numerical renormalization group approach

The self-energy method for quantum impurity models expresses the correlation part of the self-energy in terms of the ratio of two Green's functions and allows for a more accurate calculation of equilibrium spectral functions than is possible directly from the one-particle Green's function [Bulla et al., J. Phys.: Condens. Matter 10, 8365 (1998)], for example, within the numerical renormalization group method. In addition, the self-energy itself is a central quantity required in the dynamical mean field theory of strongly correlated lattice models. Here, we show how to generalize the self-energy method to the time-dependent situation for the prototype model of strong correlations, the Anderson impurity model. We use the equation of motion method to obtain closed expressions for the local Green's function in terms of a time-dependent correlation self-energy, with the latter being given as a ratio of a one-particle time-dependent Green's function and a higher-order correlation function. We benchmark this self-energy approach to time-dependent spectral functions against the direct approach within the time-dependent numerical renormalization group method. The self-energy approach improves the accuracy of time-dependent spectral function calculations, and the closed-form expressions for the Green's function allow for a clear picture of the time-evolution of spectral features at the different characteristic time-scales. The self-energy approach is of potential interest also for other quantum impurity solvers for real-time evolution, including time-dependent density matrix renormalization group and continuous-time quantum Monte Carlo techniques.

Evaluation of two-particle properties within finite-temperature self-consistent one-particle Green's function methods: Theory and application to GW and GF2.

One-particle Green's function methods can model molecular and solid spectra at zero or non-zero temperatures. One-particle Green's functions directly provide electronic energies and one-particle properties, such as dipole moment. However, the evaluation of two-particle properties, such as ⟨S2⟩ and ⟨N2⟩, can be challenging because they require a solution of the computationally expensive Bethe-Salpeter equation to find two-particle Green's functions. We demonstrate that the solution of the Bethe-Salpeter equation can be completely avoided. Applying the thermodynamic Hellmann-Feynman theorem to self-consistent one-particle Green's function methods, we derive expressions for two-particle density matrices in a general case and provide explicit expressions for GF2 and GW methods. Such density matrices can be decomposed into an antisymmetrized product of correlated one-electron density matrices and the two-particle electronic cumulant of the density matrix. Cumulant expressions reveal a deviation from ensemble representability for GW, explaining its known deficiencies. We analyze the temperature dependence of ⟨S2⟩ and ⟨N2⟩ for a set of small closed-shell systems. Interestingly, both GF2 and GW show a non-zero spin contamination and a non-zero fluctuation of the number of particles for closed-shell systems at the zero-temperature limit.

Anomalous fractional quantum Hall effect and multi-valued Hamiltonians

We discuss anomalous fractional quantum Hall effect that exists without external magnetic field. We propose that excitations in such systems may be described effectively by non-interacting particles with the Hamiltonians defined on the Brillouin zone with a branch cut. Hall conductivity of such a system is expressed through the one-particle Green function. We demonstrate that for the Hamiltonians of the proposed type this expression takes fractional values times Klitzing constant. Possible relation of the proposed construction with degeneracy of ground state is discussed as well.

Electronic Structure and Conductivity of a Disordered A1 – xBx Binary Alloy in the Cluster Approach for the Hubbard Model

We propose a method for calculating the electronic band structure of disordered systems with strong electron correlations. Various approaches to the description of electrical conductivity of disordered systems are considered. Calculations are based on determining the one-particle Green function of the system, which is averaged over different configurations of a cluster, on the Boltzmann formalism, and the Kubo linear response theory. As the basic model, we use the Hubbard model for an A1 – xBx binary alloy.

Nonequilibrium dynamics of the anyonic Tonks-Girardeau gas at finite temperature

We derive an exact description of the nonequilibrium dynamics at finite temperature for the anyonic Tonks-Girardeau gas, extending the results of Atas et al. [Phys. Rev. A 95, 043622 (2017)] to the case of arbitrary statistics. The one-particle reduced density matrix is expressed as the Fredholm minor of an integral operator, with the kernel being the one-particle Green's function of free fermions at finite temperature and the statistics parameter determining the constant in front of the integral operator. We show that the numerical evaluation of this representation using Nystr\"om's method significantly outperforms the other approaches present in the literature when there are no analytical expressions for the overlaps of the wave functions. We illustrate the distinctive features and novel phenomena present in the dynamics of anyonic systems in two experimentally relevant scenarios: the quantum Newton's cradle setting and the breathing oscillations initiated by a sudden change of the trap frequency.

Nonlinear response in the cumulant expansion for core-level photoemission

Most currently used approximations for the one-particle Green's function G in the framework of many-body perturbation theory, such as Hedin's GW approximation or the cumulant GW+C approach, are based on a linear response approximation for the screened interaction W. The extent to which such a hypothesis is valid and ways to go beyond have been explored only very little. Here we show how to derive a cumulant Green's function beyond linear-response from the equation of motion of the Green's function in a functional derivative formulation. The results can be written in a compact form, which opens the possibility to calculate the corrections in a first principles framework using time-dependent density functional theory. In order to illustrate the potential importance of the corrections, numerical results are presented for a model system with a core level and two valence orbitals.

Natural orbitals renormalization group approach to a Kondo singlet

A magnetic impurity embedded in a metal host is collectively screened by a cloud of conduction electrons to form a Kondo singlet below a characteristic energy scale $T_K$, the Kondo temperature, through the mechanism of the Kondo effect. We have reinvestigated the Kondo singlet by means of the newly developed natural orbitals renormalization group (NORG) method. We find that, in the framework of natural orbitals formalism, the Kondo screening mechanism becomes transparent and simple, while the intrinsic structure of Kondo singlet is clearly resolved. For a single impurity Kondo system, there exits a single active natural orbital which screens the magnetic impurity dominantly. In the perspective of entanglement, the magnetic impurity is entangled dominantly with the active natural orbital, i.e., the subsystem formed by the active natural orbital and the magnetic impurity basically disentangles from the remaining system. We have also studied the structures of the active natural orbital respectively projected into real space and momentum space. Moreover, the dynamical properties, represented by one-particle Green's functions defined at impurity site with active natural orbital, were obtained by using correction vector method. In order to clarify the spatial extension of the Kondo screening cloud, the concept of Kondo correlation energy was introduced. With this concept we obtain a characteristic length scale beyond which the Kondo screening cloud is hardly detected in experiment. Our numerical results indicate that this characteristic length scale usually is just a few nanometers, which interprets why it is difficult to detect the Kondo screening cloud experimentally in a metal host.

Effect of Crystal Field on the Electronic Structure of the Two-Band Hubbard Model with Spin Crossover

We consider the change in the electronic structure of the two-band Hubbard model in the regime of strong electron correlations with spin crossover upon the passage through the crossover point depending on the crystal field growth. An abrupt semimetal–insulator–semimetal transition is detected during the passage through the spin crossover point in the absence of the spin–orbit interaction, which is accompanied by a jumpwise redistribution of the partial spectral weight between the poles of the Green function of Fermi quasiparticles. The role of the spin–orbit interaction and the change in the surface topology of surface of one-particle Green function zeros are considered.

Methods of electron transport in ab initio theory of spin stiffness

We present an ab initio theory of the spin-wave stiffness tensor for ordered and disordered itinerant ferromagnets with pair exchange interactions derived from a method of infinitesimal spin rotations. The resulting formula bears an explicit form of a linear-response coefficient which involves one-particle Green's functions and effective velocity operators encountered in a recent theory of electron transport. Application of this approach to ideal metal crystals yields more reliable values of the spin stiffness than traditional ill-convergent real-space lattice summations. The formalism can also be combined with the coherent potential approximation for an effective-medium treatment of random alloys, which leads naturally to an inclusion of disorder-induced vertex corrections to the spin stiffness. The calculated concentration dependence of the spin-wave stiffness of random fcc Ni-Fe alloys can be ascribed to a variation of the reciprocal value of alloy magnetization. Calculations for random iron-rich bcc Fe-Al alloys reveal that their spin-wave stiffness is strongly reduced owing to the atomic ordering; this effect takes place due to weakly coupled local magnetic moments of Fe atoms surrounded by a reduced number of Fe nearest neighbors.