Bethe-Salpeter Research Articles

Contact interaction treatment of V→Pγ for light-quark mesons

The V→Pγ and η(η′)→γγ decays are evaluated within a Dyson-Schwinger and Bethe-Salpeter equations framework (here V={ρ±,K⋆±,ϕ} and P={π±,K±,η,η′}). The so-called impulse approximation (IA) is employed in the computation of the decay constants involved and decay widths, and so in the estimation of the associated charge and interaction radii. For their part, the required propagators and vertices stem from a contact interaction model, embedded within a beyond rainbow-ladder (RL) truncation that accounts for the typical ladder exchanges, quark anomalous magnetic moment, as well as the non-Abelian anomaly. While the examined transitions produce decay widths plainly compatible with the available experimental data, those processes involving the η−η′ mesons highlight the incompleteness of the IA when considering beyond RL effects in the interaction kernels. Published by the American Physical Society 2024

Optical properties of rutile TiO[formula omitted] with Zr, Mo, Zn, Cd impurities

To explore quasiparticle (QP) energy gaps and photoabsorption spectra of rutile TiO2 with nonmagnetic transition metal (Zr, Mo, Zn, Cd) impurities, we conducted a Γ-point only GW ＋ Bethe–Salpeter equation (BSE) calculation on a 72 (or 71) atom supercell. Our findings reveal that Zn and Cd impurities must coexist, at least partly, with oxygen vacancies to maintain charge neutrality. Among the systems considered, Mo, Zn, or Cd doped rutile TiO2 may exhibit optical absorption and catalytic activity under visible light. The resulting QP energy gaps (ΔɛQP) and photoabsorption energies (PAEs) are fairly in good agreement with both experimental and theoretical data currently available. The necessary conditions for the applicability of the Γ-point only approach in the GW ＋ BSE framework were found to be: (1) The Γ-point only GW calculation should reproduce a reasonable band gap. (2) The “superficial” exciton binding energy (the diagonal element of Wvc;vc−2Xvc;vc between v= VBM and c= CBM, where W and X are the direct and exchange terms of the BSE matrix elements, respectively) must be positive or marginally negative. (3) The “real” exciton binding energy (ΔɛQP− the lowest PAE) should be positive, even if it is exceptionally small.

Embedded Many‐Body Green's Function Methods for Electronic Excitations in Complex Molecular Systems

ABSTRACTMany‐body Green's function theory in the GW approximation with the Bethe–Salpeter equation (BSE) provides a powerful framework for the first‐principles calculations of single‐particle and electron–hole excitations in perfect crystals and molecules alike. Application to complex molecular systems, for example, solvated dyes, molecular aggregates, thin films, interfaces, or macromolecules, is particularly challenging as they contain a prohibitively large number of atoms. Exploiting the often localized nature of excitation in such disordered systems, several methods have recently been developed in which GW‐BSE is applied to a smaller, tractable region of interest that is embedded into an environment described with a lower‐level method. Here, we review the various strategies proposed for such embedded many‐body Green's functions approaches, including quantum–quantum and quantum–classical embeddings, and focus in particular on how they include environment screening effects either intrinsically in the screened Coulomb interaction in the GW and BSE steps or via extrinsic electrostatic couplings.

Tuning the optical absorption and exciton bound states of germanene by chemical functionalization

We present a comprehensive study of buckled honeycomb germanene functionalized with alternately bonded side groups hydroxyl (–H), methyl (–CH3) and trifluoro methyl (–CF3). By means of most modern theoretical and computational methods we determine the atomic geometries versus the functionalizing groups. The quasiparticle excitation effects on the electronic structure are taken into account by means of exchange-correlation treatment within the GW framework. The Bethe–Salpeter equation is solved ab initio to derive optical spectra including excitonic and quasiparticle effects. Band edge excitons are investigated in detail. The binding properties are compared with those resulting from model studies. The functionalization leads to significantly modified band structures compared with pristine germanene. The Dirac bands near the K point are destroyed and direct gaps appear at the \\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\Gamma$$\\end{document} point. Together with the many-body effects, quasiparticle gaps of 2.3, 1.8 or 1.0 eV result for –H, –CH3 and –CF3 functionalization. Totally different absorption spectra are found for in-plane and out-of-plane light polarization. Strongly bound excitons are visible below the quasiparticle band edge with binding energies of about 0.5, 0.4 or 0.3 eV. The nature of these band-gap excitons is investigated via their wave function, the contribution of various interband combinations and the dipole selection rules.

Consequences of the Pb-S Bond Formation for Lead Halide Perovskites.

Lead halide perovskites are structurally not stable due to their ionic bonds. Using sulfur agents in the crystal growth improves the stability and performance of the photovoltaic and light-emitting devices. In this theoretical work, we use a small toy S-radical in place of A cation in the bulk of lead iodide perovskite, and highlight the significance of the Pb-S covalent-double-bond formation for: the charge redistribution on the neighboring bonds that also turn to be covalent, phase transformation to a stable non-perovskite structure, and superior optoelectronic properties. The chemical analysis was performed with the Quantum Theory of Atoms In Molecules (QTAIM) and Non-Covalent Interactions (NCI) index. Excitonic properties were obtained from the solution of ab initio Bethe-Salpeter equation. Presence of the spin-orbit coupling triggers an interplay between the Frenkel and charge-transfer multiexcitons, switching between the photovoltaic and laser applications. Multiexcitons obey the exciton-fission preconditions.

Probing axion-like particles in leptonic decays of heavy mesons

Abstract We study the possibility to find the axion-like particles (ALPs) through the leptonic decays of heavy mesons. The Standard Model (SM) predictions of the branching ratios of the leptonic decays of heavy mesons are less than corresponding experimental upper limits. This provides some space for the existence of decay channels where the ALP is one of the products. Three scenarios are considered: first, the ALP is only coupled to one single charged fermion, namely, the quark, the antiquark, or the charged lepton; second, the ALP is only coupled to quark and antiquark with the same strength; third, the ALP is coupled to all the charged fermions with the same strength. The constraints of the coupling strength in different scenarios are obtained by comparing the experimental data of the branching ratios of leptonic decays of $B^-$, $D^+$, and $D_s^+$ mesons with the theoretical predictions which are achieved by using the Bethe-Salpeter (BS) method. These constraints are further applied to predict the upper limits of the leptonic decay processes of the $B_c^-$ meson in which the ALP participates.Content from this work may be used under the terms of the Creative Commons Attribution 3.0 licence. Any further distribution of this work must maintain attribution to the author(s) and the title of the work, journal citation and DOI. Article funded by SCOAP3 and published under licence by Chinese Physical Society and the Institute of High Energy Physics of the Chinese Academy of Science and the Institute of Modern Physics of the Chinese Academy of Sciences and IOP Publishing Ltd.

Optical Gaps of Ionic Materials from GW/BSE-in-DFT and CC2-in-DFT.

This work presents a density functional theory (DFT)-based embedding technique for the calculation of optical gaps in ionic solids. The approach partitions the supercell of the ionic solid and embeds a small molecule-like cluster in a periodic environment using a cluster-in-periodic embedding method. The environment is treated with DFT, and its influence on the cluster is captured by a DFT-based embedding potential. The optical gap is estimated as the lowest singlet excitation energy of the embedded cluster, obtained using a wave function theory method: second-order approximate coupled-cluster singles and doubles (CC2), and a many-body perturbation theory method: GW approximation combined with the Bethe-Salpeter equation (GW/BSE). The calculated excitation energies are benchmarked against the periodic GW/BSE values, equation-of-motion coupled-cluster singles and doubles (EOM-CCSD) results, and experiments. Both CC2-in-DFT and GW/BSE-in-DFT deliver excitation energies that are in good agreement with experimental values for several ionic solids (MgO, CaO, LiF, NaF, KF, and LiCl) while incurring negligible computational costs. Notably, GW/BSE-in-DFT exhibits remarkable accuracy with a mean absolute error (MAE) of just 0.38 eV with respect to experiments, demonstrating the effectiveness of the embedding strategy. In addition, the versatility of the method is highlighted by investigating the optical gap of a 2D MgCl2 system and the excitation energy of an oxygen vacancy in MgO, with results in good agreement with reported values.

Topological features of trajectories of virtual photons and their effective interaction under multiple scattering in a system of conductive nanoparticles

It is shown that in conditions of strong light localization in a system of Rayleigh's resonance scatterers, effective photon–photon interaction appears. This interaction is associated with neither nonlinearity of medium nor nonlocal interaction of polarization-entangled photon pairs. It is related to complex topology of photon trajectories due to multiple scattering. Because of this interaction, acts of simultaneous elastic scattering of pair of photons in the considered system cease to be independent processes. The differential cross section of this cooperative process contains only an extra degree of small Rayleigh's factor in comparison with the classical scattering cross section of a single photon. This opens up the possibility of control of light fluxes by means of alternative low-intensity light fluxes without using slow optoelectronic converters. Light localization that provides the effective photon–photon interaction is considered in the framework of a new formalism different from traditional one. Equation of the Bethe–Salpeter for two-photon propagator is resolved directly in coordinate representation without traditional reducing of this equation to some transport equation. This allows in a new light to look on reason of weak light localization and to show that weak localization is one of consequences of strong localization.

(J/ψ,J/ψ), and (ηc,ηc) production through two intermediate photons in electron-positron annihilation at B-factories

We study the processes, e−e+→γ⁎γ⁎→J/ψ+J/ψ, and e−e+→γ⁎γ⁎→ηc+ηc at s=10.6 GeV in the framework of 4×4 Bethe-Salpeter equation. For J/ψ+J/ψ production, the dominant contribution is through fragmentation process, while for ηc+ηc production, the quark rearrangement diagrams contribute. Our results of cross section for J/ψ+J/ψ and ψ(2S)+ψ(2S) are compatible with the experimental upper limits set by Belle Collaboration, while in the absence of experimental data for ηc(1S)+ηc(1S), and ηc(2S)+ηc(2S) production, we have given theoretical prediction of their cross sections, and compared with NRQCD prediction.

Possible molecules of triple-heavy pentaquarks within the extended local hidden gauge formalism

In this study, we explore the interactions between mesons and baryons in the open heavy sectors to identify potential triple-heavy molecular pentaquarks. We derive the meson-baryon interaction potentials using the vector meson exchange mechanism within the extended local hidden gauge formalism. The scattering amplitudes are computed by solving the coupled-channel Bethe-Salpeter equation, revealing several bound systems. By analyzing the poles of these amplitudes in the complex plane, we determine the masses and widths of these bound states. Additionally, we evaluate the couplings and compositeness of different channels within each bound system to assess their molecular characteristics. Our predictions include 4 Ωccc-like states, 4 Ωbbb-like states, 14 Ωbcc-like states, and 10 Ωbbc-like states, which could be targets for future experimental investigations. Published by the American Physical Society 2024

Lyapunov exponent as a signature of dissipative many-body quantum chaos

A distinct feature of Hermitian quantum chaotic dynamics is the exponential increase of certain out-of-time-order correlation (OTOC) functions around the Ehrenfest time with a rate given by a Lyapunov exponent. Physically, the OTOCs describe the growth of quantum uncertainty that crucially depends on the nature of the quantum motion. Here, we employ the OTOC in order to provide a precise definition of dissipative quantum chaos. For this purpose, we compute analytically the Lyapunov exponent for the vectorized formulation of the large-q limit of a q-body Sachdev-Ye-Kitaev model coupled to a Markovian bath. These analytic results are confirmed by an explicit numerical calculation of the Lyapunov exponent for several values of q≥4 based on the solutions of the Schwinger-Dyson and Bethe-Salpeter equations. We show that the Lyapunov exponent decreases monotonically as the coupling to the bath increases and eventually becomes negative at a critical value of the coupling signaling a transition to a dynamics which is no longer quantum chaotic. Therefore, a positive Lyapunov exponent is a defining feature of dissipative many-body quantum chaos. The observation of the breaking of the exponential growth for sufficiently strong coupling suggests that dissipative quantum chaos may require in certain cases a sufficiently weak coupling to the environment. Published by the American Physical Society 2024

Kinetic energy and speed powers vn of a heavy quark inside S wave and P wave heavy-light mesons

The average values of the powers of |q→|n¯≡qn and |v→|n¯≡vn are commonly used physical quantities, where q→ and v→ are the three-dimensional momentum and velocity of a quark inside a meson, respectively. For example, the average kinetic energy μπ2=q2 is an important quantity in the heavy quark effective theory, and the expansion of vn is commonly used in the nonrelativistic quantum chromodynamics. In this paper, based on the instantaneous Bethe-Salpeter equation method, we calculate the average values qn and vn (n=1, 2, 3, 4) of a heavy quark inside S wave and P wave heavy-light mesons. We obtain the kinetic energy μπ2=0.455 GeV2 for the B meson, which is consistent with the experimental result 0.464±0.076 GeV2. For the Bs, D, and Ds mesons, the μπ2 are 0.530, 0.317, and 0.369 GeV2, respectively, and v2=0.0185, 0.0215, 0.121, and 0.140 for B, Bs, D, and Ds, respectively. We obtain some relationships, for example, q0−n(mS)≈q1−n(mS), q0+n(mP)≈q1+′n(mP′)>q1+n(mP)≈q2+n(mP), and qn(mS)<qn(mP) (m=1, 2, 3), etc. Published by the American Physical Society 2024

Phonon-assisted Auger decay of excitons in doped transition metal dichalcogenide monolayers.

The competition between the radiative and nonradiative lifetimes determines the optical quantum yield and plays a crucial role in the potential optoelectronic applications of transition metal dichalcogenides (TMDCs). Here, we show that, in the presence of free carriers, an additional nonradiative decay channel opens for excitons in TMDC monolayers. Although the usual Auger decay channel is suppressed at low doping levels by the simultaneous momentum and energy conservation laws, exciton-phonon coupling relaxes this suppression. By solving a Bethe-Salpeter equation, we calculate the phonon-assisted Auger decay rates in four typical TMDCs as a function of doping, temperature, and dielectric environment. We find that even for a relatively low doping of 1012 cm-2, the nonradiative lifetime ranges from 16 to 165ps in different TMDCs, offering competition to the radiative decay channel.

Stochastic Schrödinger equation for hot-carrier dynamics in plasmonic systems

We present a multiscale method coupling the theory of open quantum systems with real-time ab initio treatment of electronic structure to study hot-carrier dynamics in photoexcited plasmonic systems. We combine the Markovian Stochastic Schrödinger equation with an ab initio GW coupled to the Bethe–Salpeter (BSE) equation description of the electronic degrees of freedom, interacting with a metallic nanoparticle modeled classically according to the polarizable continuum model. We apply this methodology to study the effect of relaxation (T1) and pure dephasing (T2) times on the hot-carrier dynamics in a system composed of a quantum portion described at GW/BSE level, i.e., a CHO fragment adsorbed on a vertex of a rhodium nanocube, and of the rest of the nanocube, treated classically, when irradiated with a 2.7 eV light pulse, inspired by the experimental results on plasmon-driven CO2 photoreduction. A net hole injection from rhodium to CHO is observed, with and without the classical portion of the nanocube. The nanocube effect is to enhance the generated charge population by two orders of magnitude. The nonradiative decay, via a relaxation time T1 based on the energy-gap law, produces a rapid decrease of the charge population. Results with T2 only show that a charge injection retarded with respect to the pulse, which is present in the coherent dynamics, disappears when coherence is erased.

From Many-Body Ab Initio to Effective Excitonic Models: A Versatile Mapping Approach Including Environmental Embedding Effects.

We present an original multistate projective diabatization scheme based on Green's function formalisms that allows the systematic mapping of many-body ab initio calculations onto effective excitonic models. This method inherits the ability of the Bethe-Salpeter equation to describe Frenkel molecular excitons and intermolecular charge-transfer states equally well, as well as the possibility for an effective description of environmental effects in a QM/MM framework. The latter is found to be a crucial element in order to obtain accurate model parameters for condensed phases and to ensure their transferability to excitonic models for extended systems. The method is presented through a series of examples illustrating its quality, robustness, and internal consistency.

Excitonic properties and solar harvesting performance of Cs2ZnY2X2 as quasi-2D mixed-halide perovskites

Due to their low toxicity and high-temperature stability, lead-free quasi-2D metal halide perovskites (MHPs) are promising materials for optoelectronic applications. However, understanding their structural and optoelectronic properties, especially excitonic effects (electron-hole pair, e-h), is challenging due to their quantum well topology. We propose an efficient protocol for band gap correction of Cs2ZnX (X = Cl4, Br2Cl2, and I2Cl2) and Cs2PbI2Cl2 (used as a benchmark) quasi-2D MHPs. This protocol is based on a relativistic quasiparticle approach (DFT-1/2) using density functional theory (DFT). We first examined the hybrid contributions of the halide alloys, leading to excitonic characterization using the Bethe–Salpeter equation within the maximally localized Wannier functions tight-binding method. This method provides a cost-effective approach for describing e-h quasiparticle effects. Additionally, we analyzed the crystal structure, thermodynamic stability, and optoelectronic properties of the newly synthesized Zn-based systems, focusing on their structural stability mechanisms. We found a correlation between the allocation of Cs+ cations in the crystal structure and the formation of two distinct stabilization patterns, influenced by the radii of the metal (Zn or Pb) and halide components. The relativistic correction of the band gap energies yielded results within 10 % of the experimental values. Furthermore, incorporating e-h quasiparticle effects for Cs2PbI2Cl2 resulted in an exciton binding energy of 0.160 eV, in excellent agreement with experimental data. This work represents a significant advance in the optoelectronic characterization of Cs2ZnX systems, previously unexplored for their excitonic properties.

Solving the homogeneous Bethe-Salpeter equation with a quantum annealer

The homogeneous Bethe-Salpeter equation (hBSE), describing a bound system in a genuinely relativistic quantum-field theory framework, was solved for the first time by using a D-Wave quantum annealer. After applying standard techniques of discretization, the hBSE, in ladder approximation, can be formally transformed in a generalized eigenvalue problem (GEVP), with two square matrices: one symmetric and the other nonsymmetric. The latter matrix poses the challenge of obtaining a suitable formal approach for investigating the GEVP by means of a quantum annealer, i.e., to recast it as a quadratic unconstrained binary optimization problem. A broad numerical analysis of the proposed algorithms, applied to matrices of dimension up to 64, was carried out by using both the simulated-annealing package and the D-Wave . The numerical results very nicely compare with those obtained with standard classical algorithms, and also show interesting scalability features. Published by the American Physical Society 2024

Interplay of coulomb and exciton-phonon coupling controls singlet fission dynamics in two pentacene polymorphs.

Pentacene is an important model organic semiconductor in both the singlet exciton fission (SF) and organic electronics communities. We have investigated the effect of changing crystal structure on the SF process, generating multiple triplet excitons from an initial singlet exciton, and subsequent triplet recombination. Unlike for similar organic semiconductors that have strong SF sensitive to polymorphism, we find almost no quantitative difference between the kinetics of triplet pair (TT) formation in the two dominant polymorphs of pentacene. Both pairwise dimer coupling and momentum-space crystal models predict much faster TT formation from the bright singlet excited state of the Bulk vs ThinFilm polymorph, contrasting with the experiment. GW and Bethe-Salpeter equation calculations, including exciton-phonon coupling, reveal that ultrafast phonon-driven transitions in the ThinFilm polymorph compensate the intrinsically slower purely Coulomb-mediated TT formation channel, rationalizing the similarity in observed rates. Taking into account the influence of subtle structural distinctions on both the direct and phonon-mediated SF pathways reveals a predictive capability to these methods, expected to be applicable to a wide variety of molecular crystals.

Strain tunable excitonic optical properties in monolayer Ga2O3

Abstract Two-dimensional (2D) Ga2O3 has been confirmed to be a stable structure with five atomic layer thickness configuration. In this work, we study the quasi-particle electronic band structures and then access the excitonic optical properties through solving the Bethe–Salpeter equation (BSE). The results reveal that the exciton dominates the optical absorption in the visible light region with the binding energy as large as ∼ 1.0 eV, which is highly stable at room temperature. Importantly, both the dominant absorption P1 and P2 peaks are optically bright without dark exciton between them, and thus is favorable for luminescence process. The calculated radiative lifetime of the lowest-energy exciton is 2.0×10−11 s at 0 K. Furthermore, the radiative lifetime under +4% tensile strain is one order of magnitude shorter than that of the strain-free case, while it is less insensitive under the compressive strain. Our findings set the stage for future theoretical and experimental investigation on monolayer Ga2O3.

Discovery of novel silicon allotropes with optimized band gaps to enhance solar cell efficiency through evolutionary algorithms and machine learning

In the pursuit of advancing solar energy technologies, this study presents 20 direct and quasi-direct band gap silicon crystalline semiconductors that satisfy the Shockley-Queisser limit, a benchmark for solar cell efficiency. Employing two evolutionary algorithm-based searches, we optimize structures and calculate fitness function using the DFTB method and Gaussian approximation potential. Following the preselection of structures based on energy considerations, we further optimize them using PBEsol DFT. Subsequently, we screen the structures based on their band gap, employing a DFTB method tailored for band gap calculation of silicon crystals. To ensure accurate band gap determination, we employ HSE and GW methods. To validate the structural stability, we employ phonon analysis via linear regression algorithm applied to PBEsol DFT data. Significantly, the structures unveiled in this study are of great importance due to their proven stability from both mechanical and dynamic perspectives. Furthermore, the ductility and low density of certain structures enhance their potential application. We examine the optical properties by studying the imaginary part of the dielectric function by solving the Bethe–Salpeter Equation on top of GW approximation. By calculating the SLME, we achieve an efficiency of 32.7% for Si22 at a thickness of 500 nm. Moreover, the study harnesses various machine learning algorithms to develop a predictive model for the band gap energy of these silicon structures. Input data for machine learning models are derived from structural MBTR and SOAP descriptors, as well as DFT outputs. Notably, the results reveal that features extracted from DFT outperform the MBTR and SOAP descriptors.