Many-body Effects Research Articles

ベイズ推定に基づく角度分解光電子スペクトルの網羅的解析

We review our recent study on the development of a quantitative data analysis technique for angle-resolved photoemission spectroscopy. The new method enables us to precisely disentangle one-particle band dispersion and many-body effects from ARPES data based on Bayesian inference.

A "short blanket" dilemma for a state-of-the-art neural network potential for water: Reproducing experimental properties or the physics of the underlying many-body interactions?

Deep neural network (DNN) potentials have recently gained popularity in computer simulations of a wide range of molecular systems, from liquids to materials. In this study, we explore the possibility of combining the computational efficiency of the DeePMD framework and the demonstrated accuracy of the MB-pol data-driven, many-body potential to train a DNN potential for large-scale simulations of water across its phase diagram. We find that the DNN potential is able to reliably reproduce the MB-pol results for liquid water, but provides a less accurate description of the vapor-liquid equilibrium properties. This shortcoming is traced back to the inability of the DNN potential to correctly represent many-body interactions. An attempt to explicitly include information about many-body effects results in a new DNN potential that exhibits the opposite performance, being able to correctly reproduce the MB-pol vapor-liquid equilibrium properties, but losing accuracy in the description of the liquid properties. These results suggest that DeePMD-based DNN potentials are not able to correctly "learn" and, consequently, represent many-body interactions, which implies that DNN potentials may have limited ability to predict the properties for state points that are not explicitly included in the training process. The computational efficiency of the DeePMD framework can still be exploited to train DNN potentials on data-driven many-body potentials, which can thus enable large-scale, "chemically accurate" simulations of various molecular systems, with the caveat that the target state points must have been adequately sampled by the reference data-driven many-body potential in order to guarantee a faithful representation of the associated properties.

Probing many-body effects in harmonic traps with twisted light

We explore the potential of twisted light, a structured beam carrying orbital angular momentum, as a tool to unveil many-body effects in parabolically confined systems. According to the generalized Kohn theorem, the dipole response of such a multiparticle system to a spatially homogeneous probe is indistinguishable from the response of a system of noninteracting particles. Twisted light however can excite internal degrees of freedom, resulting in the appearance of new peaks in the multipole spectrum which are not present when the probe is a plane wave. We also demonstrate the ability of the proposed twisted light probe to capture the transition of interacting fermions into a strongly correlated regime in a one-dimensional harmonic trap. We report that, by suitable choice of the probe's parameters, the transition into a strongly correlated phase manifests itself as an approaching and ultimate superposition of peaks in the second-order quadrupole response. These features are observed in exact calculations for two electrons and well reproduced in adiabatic time-dependent density-functional theory simulations.

Dissipative stabilization of dark quantum dimers via squeezed vacuum

Understanding the mechanism through which an open quantum system exchanges information with an environment is central to the creation and stabilization of quantum states. This theme has been explored recently, with attention mostly focused on system control or environment engineering. Here, we bring these ideas together to describe the many-body dynamics of an extended atomic array coupled to a squeezed vacuum. We show that fluctuations can drive the array into a pure dark state decoupled from the environment. The dark state is obtained for an even number of atoms and consists of maximally entangled atomic pairs, or dimers, that mimic the behavior of the squeezed field. Each pair displays reduced fluctuations in one polarization quadrature and amplified in another. This dissipation-induced stabilization relies on an efficient transfer of correlations between pairs of photons and atoms. It uncovers the mechanism through which squeezed light causes an atomic array to self-organize and illustrates the increasing importance of spatial correlations in modern quantum technologies where many-body effects play a central role.

Electronic and Optical Properties of Alkaline Earth Metal Fluoride Crystals with the Inclusion of Many-Body Effects: A Comparative Study on Rutile MgF2 and Cubic SrF2

We conducted a systematic investigation using state-of-the-art techniques on the electronic and optical properties of two crystals of alkaline earth metal fluorides, namely rutile MgF2 and cubic SrF2. For these two crystals of different symmetry, we present density functional theory (DFT), many-body perturbation theory (MBPT), and Bethe–Salpeter equation (BSE) calculations. We calculated a variety of properties, namely ground-state energies, band-energy gaps, and optical absorption spectra with the inclusion of excitonic effects. The quantities were obtained with a high degree of convergence regarding all bulk electronic and optical properties. Bulk rutile MgF2 has distinguished ground-state and excited-state properties with respect to the other cubic fluoride SrF2 and the other members of the alkaline earth metal fluoride family. The nature of the fundamental gaps and estimates of the self-energy and excitonic effects for the two compounds are presented and discussed in detail. Our results are in good accordance with the measurements and other theoretical–computational data. A comparison is made between the excitation and optical properties of bulk rutile MgF2, cubic SrF2, and the corresponding clusters, for which calculations have recently been published, confirming strong excitonic effects in finite-sized systems.

Exciton–Photon Interactions in Two-Dimensional Semiconductor Microcavities

Investigation of light–matter interactions in two-dimensional (2D) semiconductors is essential to understand many-body effects and explore their applications in photonics. 2D semiconductor microcavities can be formed by the integration of 2D semiconductor active media with planar Fabry–Perot resonant cavities. The emerging exciton–photon interactions between the strongly bound excitons in 2D semiconductors and the cavity photons allow exploring on the wealthy photonic and polaritonic physics of bosonic quasiparticles in the 2D limit. This Perspective focuses on recent advances in exciton–photon interactions of 2D semiconductor microcavities and their inspiring applications. First, we picture the research scope of 2D semiconductor microcavities, sort out the historical development from conventional semiconductor microcavities to the emerged 2D semiconductor microcavities, and illustrate mostly employed device structures. Second, we classify exciton–photon interactions in 2D semiconductor microcavities according to their coupling strengths. In the weak coupling regime, control of spontaneous emission and photon lasing are discussed together with the Purcell effect. In the strong coupling regime, we summarize experimental observations and theoretical predictions on Rabi splitting, Bose–Einstein condensation, polariton lasing, superfluidity, and superconductivity. Third, four types of leading-edge applications are outlined, including on-chip coherent light sources, microcavity-enhanced single-photon sources, topological photonics, and other nonlinear optics. Finally, we highlight the remaining challenges and future opportunities for fundamental physics of 2D semiconductor microcavities and their technological applications.

Robustness of electronic screening effects in electron spectroscopies: Example of V2O5

In bulk and low-dimensional extended systems, the screening of excitations by the electron cloud is a key feature governing spectroscopic properties. Widely used computational approaches, especially in the framework of many-body perturbation theory, such as the GW approximation and the resulting approximate Bethe-Salpeter equation, are explicitly formulated in terms of the screened Coulomb interaction. In the present work we explore the effect of screening in absorption and electron energy loss spectroscopy, concentrating on the effect of local distortions on the screening and elucidating the resulting changes in the various spectra. Using the layered bulk oxide V$_2$O$_5$ as prototype material, we show in which way local distortions affect the screening, and in which way changes in the screening impact electron energy loss and absorption spectra including excitons. We highlight cancellations that make many-body effects in the spectra very robust with respect to structural modifications, while the band structure undergoes significant changes and the nature of the excitations may also be affected. This yields insight concerning the structure-properties relations that are crucial for the use of V$_2$O$_5$ as energy storage material, and more generally, that may be used to optimize the analysis and the calculation of electronic spectra in complex materials.

Quantum simulation of weak-field light-matter interactions

Simulation of the interaction of light with matter, including at the few-photon level, is important for understanding the optical and optoelectronic properties of materials, and for modeling next-generation non-linear spectroscopies that use entangled light. At the few-photon level the quantum properties of the electromagnetic field must be accounted for with a quantized treatment of the field, and then such simulations quickly become intractable, especially if the matter subsystem must be modeled with a large number of degrees of freedom, as can be required to accurately capture many-body effects and quantum noise sources. Motivated by this we develop a quantum simulation framework for simulating such light-matter interactions on platforms with controllable bosonic degrees of freedom, such as vibrational modes in the trapped ion platform. The key innovation in our work is a scheme for simulating interactions with a continuum field using only a few discrete bosonic modes, which is enabled by a Green's function (response function) formalism. We develop the simulation approach, sketch how the simulation can be performed using trapped ions, and then illustrate the method with numerical examples. Our work expands the reach of quantum simulation to important light-matter interaction models and illustrates the advantages of extracting dynamical quantities such as response functions from quantum simulations.

Two-dimensional electronic spectroscopy of an ultracold gas.

Femtosecond coherent multidimensional spectroscopy is demonstrated for an ultracold gas. A setup for phase modulation spectroscopy is used to probe the 32S1/2-22P1/2,3/2 transition in an 800μK-cold sample of 7Li atoms confined in a magneto-optical trap. The observation of a double quantum coherence response, a signature of interparticle interactions, paves the way for detailed investigations of few- and many-body effects in ultracold gases using this technique. The experiment combines a frequency resolution of 3 GHz with a potential time resolution of 200 fs, which allows for high-resolution studies of ultracold atoms and molecules both in the frequency and in the time domain.

Sensitive dependence of the linewidth enhancement factor on electronic quantum effects in quantum cascade lasers

The linewidth enhancement factor (LEF) describes the coupling between amplitude and phase fluctuations in a semiconductor laser and has recently been shown to be a crucial component for frequency comb formation in addition to linewidth broadening. It necessarily arises from causality, as famously formulated by the Kramers–Kronig relation, in media with nontrivial dependence of the susceptibility on intensity variations. While thermal contributions are typically slow, and thus can often be excluded by suitably designing the dynamics of an experiment, the many quantum contributions are harder to separate. In order to understand and, ultimately, design the LEF to suitable values for frequency comb formation, soliton generation, or narrow laser linewidth, it is, therefore, important to systematically model all these effects. In this comprehensive work, we introduce a general scheme for computing the LEF, which we employ with a nonequilibrium Green's function model. This direct method, based on simulating the system response under varying optical intensity and extracting the dependence of the susceptibility to intensity fluctuations, can include all relevant electronic effects and predicts the LEF of an operating quantum cascade laser to be in the range of 0.1–1, depending on laser bias and frequency. We also confirm that many-body effects, off-resonant transitions, dispersive (Bloch) gain, counter-rotating terms, intensity-dependent transition energy, and precise subband distributions all significantly contribute and are important for accurate simulations of the LEF.

Investigation of local distortion effects on X-ray absorption of ferroelectric perovskites from first principles simulations.

Understanding the role of ferroelectric polarization in modulating the electronic and structural properties of crystals is critical for advancing these materials for overcoming various technological and scientific challenges. However, due to difficulties in performing experimental methods with the required resolution, or in interpreting the results of methods therein, the nanoscale morphology and response of these surfaces to external electric fields has not been properly elaborated. In this work we investigate the effect of ferroelectric polarization and local distortions in a BaTiO3 perovskite, using two widely used computational approaches which treat the many-body nature of X-ray excitations using different philosophies, namely the many-body, delta-self-consistent-field determinant (mb-ΔSCF) and the Bethe-Salpeter equation (BSE) approaches. We show that in agreement with our experiments, both approaches consistently predict higher excitations of the main peak in the O-K edge for the surface with upward polarization. However, the mb-ΔSCF approach mostly fails to capture the L2,3 separations at the Ti-L edge, due to the absence of spin-orbit coupling in Kohn-Sham density functional theory (KS-DFT) at the generalized gradient approximation level. On the other hand, and most promising, we show that application of the GW/BSE approach successfully reproduces the experimental XAS, both the relative peak intensities as well as the L2,3 separations at the Ti-L edges upon ferroelectric switching. Thus simulated XAS is shown to be a powerful method for capturing the nanoscale structure of complex materials, and we underscore the need for many-body perturbation approaches, with explicit consideration of core-hole and multiplet effects, for capturing the essential physics in these systems.

Thermal discrete dipole approximation for near-field radiative heat transfer in many-body systems with arbitrary nonreciprocal bodies

The theoretical study of many-body effects in the context of near-field radiative heat transfer (NFRHT) has already led to the prediction of a plethora of thermal radiation phenomena. Special attention has been paid to nonreciprocal systems in which the lack of the Lorentz reciprocity has been shown to give rise to unique physical effects. However, most of the theoretical work in this regard has been carried out with the help of approaches that consider either point-like particles or highly symmetric bodies (such as spheres), which are not easy to realize and explore experimentally. In this work we develop a many-body approach based on the thermal discrete dipole approximation (TDDA) that is able to describe the NFRHT between nonreciprocal objects of arbitrary size and shape. We illustrate the potential and the relevance of this approach with the analysis of two related phenomena, namely the existence of persistent thermal currents and the photon thermal Hall effect, in a system with several magneto-optical bodies. Our many-body TDDA approach paves the way for closing the gap between experiment and theory that is hindering the progress of the topic of NFRHT in many-body systems.

Optical conductivity of an anharmonic large polaron gas at weak coupling

In a polar solid, electrons or other charge carriers can interact with the phonons of the ionic lattice, leading to the formation of polaron quasiparticles. The optical conductivity and optical absorption spectrum of a material are affected by this electron-phonon coupling, most notably leading to an absorption peak in the midinfrared region. Recently, a model Hamiltonian for anharmonic electron-phonon coupling was derived [M. Houtput and J. Tempere, Phys. Rev. B 103, 184306 (2021)] that includes both the conventional Fr\"ohlich interaction as well as an interaction in which an electron interacts with two phonons simultaneously. In this article, we calculate and investigate the optical conductivity of the anharmonic large polaron gas, and we show that an additional characteristic absorption peak appears due to this one-electron--two-phonon interaction. We calculate a semianalytical expression for the optical conductivity $\ensuremath{\sigma}(\ensuremath{\omega})$ at finite temperatures and weak coupling using the Kubo formula. The electronic and phononic contributions can be split and treated separately, such that the many-body effects of the electron gas may be taken into account through the well-known dynamical structure factor $S(\mathbf{k},\ensuremath{\omega})$. From the resulting optical conductivity, we calculate the polaron effective mass, an estimate for the electron-phonon scattering times, and the optical absorption spectrum of the anharmonic polaron gas. It is shown that the effects are negligible for four common III-V semiconductors (BN, AlN, BP, AlP) in the zinc-blende structure, which justifies the commonly used harmonic approximation in these materials. We show that alongside the well-known polaron absorption peak at the phonon energy $\ensuremath{\hbar}{\ensuremath{\omega}}_{\text{LO}}$, the one-electron--two-phonon interaction leads to an additional absorption peak at $2\ensuremath{\hbar}{\ensuremath{\omega}}_{\text{LO}}$. We propose this absorption peak as an experimentally measurable indicator for non-negligible one-electron--two-phonon interaction in a material, since the height of this peak is proportional to the strength of this anharmonic interaction.

Orbital-Hybridization-Driven Charge Density Wave Transition in CsV3 Sb5 Kagome Superconductor.

Owing to its inherent non-trivial geometry, the unique structural motif of the recently discovered kagome topological superconductor AV3 Sb5 (A = K, Rb, Cs) is an ideal host of diverse topologically non-trivial phenomena, including giant anomalous Hall conductivity, topological charge order, charge density wave (CDW), and unconventional superconductivity. Despite possessing a normal-state CDW order in the form of topological chiral charge order and diverse superconducting gaps structures, it remains unclear how fundamental atomic-level properties and many-body effects including Fermi surface nesting, electron-phonon coupling, and orbital hybridization contribute to these symmetry-breaking phenomena. Here, the direct participation of the V3d-Sb5p orbital hybridization in mediating the CDW phase transition in CsV3 Sb5 is reported. The combination of temperature-dependent X-ray absorption and first-principles studies clearly indicates the inverse Star-of-David structure as the preferred reconstruction in the low-temperature CDW phase. The results highlight the critical role that Sb orbitals play and establish orbital hybridization as the direct mediator of the CDW states and structural transition dynamics in kagome unconventional superconductors. This is a significant step toward the fundamental understanding and control of the emerging correlated phases from the kagome lattice through the orbital interactions and provides promising approaches to novel regimes in unconventional orders and topology.

Full counting statistics in the many-body Hatano-Nelson model

We study non-hermitian many-body physics in the interacting Hatano-Nelson model with open boundary condition. The violation of reciprocity, resulting from an imaginary vector potential, induces the non-hermitian skin-effect and causes exponential localization for all single particle eigenfunctions in the non-interacting limit. Nevertheless, the density profile of the interacting system becomes only slightly tilted relative to the average filling. The Friedel oscillations exhibit a beating pattern due to the modification of the Fermi wavenumber. The probability distribution of particles over any finite interval is the normal distribution, whose mean scales with the imaginary vector potential and the variance is symmetric to the center of the chain. This is confirmed by several numerically exact methods even for relatively small systems. These features are expected to be generic not only for fermions, which naturally repel each other due to Pauli's exclusion principle, but for interacting bosons as well. Our findings indicate that many-body effects can significantly alter and conceal the single particle properties and the skin effect in non-hermitian systems.

Semiconductor Bloch equation analysis of optical Stark and Bloch-Siegert shifts in monolayer WSe2 and MoS2

We report on the theoretical and experimental investigation of valley-selective optical Stark and Bloch-Siegert shifts of exciton resonances in monolayers WSe$_2$ and MoS$_2$ induced by strong circularly polarized nonresonant optical fields. We predict and observe transient shifts of both 1sA and 1sB exciton transitions in the linear interaction regime. The theoretical description is based on semiconductor Bloch equations. The solutions of the equations are obtained with a modified perturbation technique, which takes into account many-body Coulomb interaction effects. These solutions allow to explain the polarization dependence of the shifts and calculate their values analytically. We found experimentally the limits of the applicability of the theoretical description by observing the transient exciton spectra change due to many-body effects at high field amplitudes of the driving wave.

A scheme for rapid evaluation of the intermolecular three-body polarization effect in water clusters.

The ability to accurately and rapidly evaluate the intermolecular many-body polarization effect of the water system is very important for computer simulations of biomolecule in aqueous. In this paper, a scheme is proposed based on the polarizable dipole-dipole interaction model and used to rapidly estimate the intermolecular many-body polarization effect in water clusters. We use a bond-dipole-based polarization function to evaluate the polarization energy. We regard two OH bonds of a water molecule as two bond-dipoles and set the permanent OH bond-dipole moment of a water molecule to be 1.51 Debye. We estimate the induced OH bond-dipole moment via a simple formula in which only one correction factor is needed. This scheme is then applied to tens of water clusters to calculate the three- and four-body interaction energies. The three-body interaction energies of 93 water clusters produced by our scheme are compared with those produced by the counterpoise-corrected CCSD(T)/aug-cc-pVDZ, MP2/aug-cc-pVDZ, M06-2X/jul-cc-pVTZ methods, by the AMOEBApro13, iAMOEBA, AMOEBA+, AMOEBA+(CF) methods, and by the MB-pol method. The four-body interaction energies of 47 water clusters yielded by our scheme are compared with those yielded by the counterpoise-corrected MP2/aug-cc-pVDZ and M06-2X/ jul-cc-pVTZ methods, by the AMOEBApro13, AMOEBA+, AMOEBA+(CF) methods, and by the MB-pol method. The comparison results show that the scheme proposed in this paper can reproduce the counterpoise-corrected CCSD(T)/aug-cc-pVDZ three-body interaction energies and reproduce the counterpoise-corrected MP2/aug-cc-pVDZ four-body interaction energies both accurately and efficiently. We anticipate the scheme proposed here can be useful for computer simulations of liquid water and aqueous solutions.

Geometrical patterning of receptor sites controls kinetics via many-body effects in bivalent systems

Geometrical patterning of receptor sites controls kinetics via many-body effects in bivalent systems

Flat-Band-Induced Many-Body Interactions and Exciton Complexes in a Layered Semiconductor.

Interactions among a collection of particles generate many-body effects in solids that result in striking modifications of material properties. The heavy carrier mass that yields strong interactions and gate control of carrier density over a wide range makes two-dimensional semiconductors an exciting playground to explore many-body physics. The family of III-VI metal monochalcogenides emerges as a new platform for this purpose because of its excellent optical properties and the flat valence band dispersion. In this work, we present a complete study of charge-tunable excitons in few-layer InSe by photoluminescence spectroscopy. From the optical spectra, we establish that free excitons in InSe are more likely to be captured by ionized donors leading to the formation of bound exciton complexes. Surprisingly, a pronounced red shift of the exciton energy accompanied by a decrease of the exciton binding energy upon hole-doping reveals a significant band gap renormalization induced by the presence of the Fermi reservoir.

Re-Evaluation of the Nuclear Magnetic Octupole Moment of 209Bi

We modified the Hfs92 code of the GRASP package in order to describe the magnetic octupole hyperfine interaction. To illustrate the utility of the modified code, we carried out state-of-the-art calculations of the electronic factors of the magnetic octupole hyperfine interaction constants for levels in the ground configuration of the Bi atom. The nuclear magnetic octupole moment of the 209Bi isotope was extracted by combining old measurements of the hyperfine structures of 6p34S3/2o [Hull, R.; Brink, G. Phys. Rev. A 1970, 1, 685] and 2P3/2o [Landman, D.A.; Lurio, A. Phys. Rev. A 1970, 1, 1330] using the atomic-beam magnetic-resonance technique with our theoretical electronic factors. The present extracted octupole moment was consistent with all the available values but the one obtained in the single-particle nuclear shell model approximation. This observation supports the previous finding that nuclear many-body effects, such as the core polarization, significantly contribute to the nuclear magnetic octupole moment in the case of 209Bi.