Nonperturbative Treatment Research Articles

Exact-Two-Component Complete Active Space Method with Variational Treatment of Magnetic Field and Spin-Orbit Coupling: Application to X-ray Magnetic Circular Dichroism Spectroscopy.

We introduce an exact-two-component complete active space self-consistent-field (X2C-CASSCF) method formulated under the restricted-magnetic-balance condition. This framework allows for the nonperturbative treatment of static magnetic fields using gauge-including atomic orbitals (GIAOs). The GIAO-X2C-CASSCF methodology effectively captures all microstates within the same 2J + 1-degenerate manifold and their splitting in a static magnetic field, which are not accessible through single-reference-based methods. We also present mathematical recursive expressions for evaluating one-electron relativistic integrals by using GIAOs in the presence of a finite magnetic field. Benchmark studies include oxygen and nitrogen K-edge X-ray magnetic circular dichroism spectroscopy (XMCD) for closed-shell organic compounds, as well as L-edge XMCD spectroscopy for the high-spin open-shell transition metal ion Mn2+ and the tetrahedral Mn(II)O46- complex.

Les Houches lectures on deep learning at large and infinite width*

Abstract These lectures, presented at the 2022 Les Houches Summer School on Statistical Physics and Machine Learning, focus on the infinite-width limit and large-width regime of deep neural networks. Topics covered include the various statistical and dynamical properties of these networks. In particular, the lecturers discuss properties of random deep neural networks, connections between trained deep neural networks, linear models, kernels and Gaussian processes that arise in the infinite-width limit, and perturbative and non-perturbative treatments of large but finite-width networks, at initialization and after training.

Phonon collapse and anharmonic melting of the 3D charge-density wave in kagome metals

The charge-density wave (CDW) mechanism and resulting structure of the AV3Sb5 family of kagome metals has posed a puzzling challenge since their discovery four years ago. In fact, the lack of consensus on the origin and structure of the CDW hinders the understanding of the emerging phenomena. Here, by employing a non-perturbative treatment of anharmonicity from first-principles calculations, we reveal that the charge-density transition in CsV3Sb5 is driven by the large electron-phonon coupling of the material and that the melting of the CDW state is attributed to ionic entropy and lattice anharmonicity. The calculated transition temperature is in very good agreement with experiments, implying that soft mode physics are at the core of the charge-density wave transition. Contrary to the standard assumption associated with a pure kagome lattice, the CDW is essentially three-dimensional as it is triggered by an unstable phonon at the L point. The absence of involvement of phonons at the M point enables us to constrain the resulting symmetries to six possible space groups. The unusually large electron-phonon linewidth of the soft mode explains why inelastic scattering experiments did not observe any softened phonon. We foresee that large anharmonic effects are ubiquitous and could be fundamental to understand the observed phenomena also in other kagome families.

The triton lifetime from nuclear lattice effective field theory

In this work, we present a calculation of the triton β-decay lifetime using Nuclear Lattice Effective Field Theory (NLEFT) at next-to-next-to-next-to-leading order in the chiral expansion. By incorporating a non-perturbative treatment of the higher-order corrections, we achieve consistent predictions for the Fermi and Gamow-Teller matrix elements, which are crucial for determining the triton lifetime. Our results are consistent with earlier theoretical calculations, confirming the robustness of our approach. This study marks a significant advancement in the systematic application of NLEFT to nuclear β-decay processes, paving the way for future high-precision calculations in more complex nuclear systems. Additionally, we discuss potential improvements to our approach, including the explicit inclusion of two-pion exchange mechanisms and the refinement of three-nucleon forces. These developments are essential for extending the applicability of NLEFT to a broader range of nuclear phenomena, including neutrinoless double-β decay.

Gauge-invariant renormalization of four-quark operators

We study the renormalization of four-quark operators in one-loop perturbation theory. We employ a coordinate-space gauge-invariant renormalization scheme (GIRS), which can be advantageous compared to other schemes, especially in nonperturbative lattice investigations. From our perturbative calculations, we extract the conversion factors between GIRS and the modified minimal subtraction scheme (MS¯) at the next-to-leading order. As a by-product, we also obtain the relevant anomalous dimensions in the GIRS scheme. A formidable issue in the study of the four-quark operators is that operators with different Dirac matrices mix among themselves upon renormalization. We focus on both parity-conserving and parity-violating four-quark operators, which change flavor numbers by two units (ΔF=2). The extraction of the conversion factors entails the calculation of two-point Green’s functions involving products of two four-quark operators, as well as three-point Green’s functions with one four-quark and two bilinear operators. The significance of our results lies in their potential to refine our understanding of QCD phenomena, offering insights into the precision of Cabibbo-Kobayashi-Maskawa (CKM) matrix elements and shedding light on the nonperturbative treatment of complex mixing patterns associated with four-quark operators. Published by the American Physical Society 2024

Dynamic and static dipole polarizability of an Aharonov–Bohm ring

The properties of nanoscale rings are sensitive to Aharonov–Bohm fluxes threading the ring. In particular, neighboring angular momentum eigenstates become degenerate in cases of half-integer flux. Such degeneracies have a profound effect on the dipole polarizability leading to a divergent response. We analyze circular finite-width nanorings and derive a simple and compact expression for the polarizability valid for arbitrary ring geometry, frequency and magnetic flux. The dipole response is significantly reduced by finite-width effects, yet divergencies at half-integer flux are predicted irrespective of width. Finally, a non-divergent (but large) response is restored through a non-perturbative treatment of both magnetic and electric fields.

The two upper critical dimensions of the Ising and Potts models

We derive the exact actions of the Q-state Potts model valid on any graph, first for the spin degrees of freedom, and second for the Fortuin-Kasteleyn clusters. In both cases the field is a traceless Q-component scalar field Φα. For the Ising model (Q = 2), the field theory for the spins has upper critical dimension \\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${d}_{{\ ext{c}}}^{{\ ext{spin}}}$$\\end{document} = 4, whereas for the clusters it has \\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${d}_{{\ ext{c}}}^{{\ ext{cluster}}}$$\\end{document} = 6. As a consequence, the probability for three points to be in the same cluster is not given by mean-field theory for d within 4 < d < 6. We estimate the associated universal structure constant as \\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$C=\\sqrt{6-d}+\\mathcal{O}{\\left(6-d\\right)}^{3/2}$$\\end{document}. This shows that some observables in the Ising model have an upper critical dimension of 4, while others have an upper critical dimension of 6. Combining perturbative results from the ϵ = 6 – d expansion with a non-perturbative treatment close to dimension d = 4 allows us to locate the shape of the critical domain of the Potts model in the whole (Q, d) plane.

Nonadiabatic dynamics of molecules interacting with metal surfaces: A quantum-classical approach based on Langevin dynamics and the hierarchical equations of motion.

A novel mixed quantum-classical approach to simulating nonadiabatic dynamics of molecules at metal surfaces is presented. The method combines the numerically exact hierarchical equations of motion approach for the quantum electronic degrees of freedom with Langevin dynamics for the classical degrees of freedom, namely, low-frequency vibrational modes within the molecule. The approach extends previous mixed quantum-classical methods based on Langevin equations to models containing strong electron-electron or quantum electronic-vibrational interactions, while maintaining a nonperturbative and non-Markovian treatment of the molecule-metal coupling. To demonstrate the approach, nonequilibrium transport observables are calculated for a molecular nanojunction containing strong interactions.

Quantum-Acoustical Drude Peak Shift.

Quantum acoustics-a recently developed framework parallel to quantum optics-establishes a nonperturbative and coherent treatment of the electron-phonon interaction in real space. The quantum-acoustical representation reveals a displaced Drude peak hiding in plain sight within the venerable Fröhlich model: the optical conductivity exhibits a finite frequency maximum in the far-infrared range and the dc conductivity is suppressed. Our results elucidate the origin of the high-temperature absorption peaks in strange or bad metals, revealing that dynamical lattice disorder steers the system towards a non-Drude behavior.

Nonperturbative theory for the QED corrections to elastic electron-nucleus scattering

A potential for the vertex and self-energy correction is derived from the first-order Born theory. The inclusion of this potential in the Dirac equation, together with the Uehling potential for vacuum polarization, allows for a nonperturbative treatment of these quantum electrodynamical effects within the phase-shift analysis. Investigating the 12C and 208Pb targets, a considerable deviation of the respective cross section change from the Born results is found for the heavier target. It is shown that at low impact energies the dispersion effects play no role. Estimates for the correction to the beam-normal spin asymmetry and its accuracy at 5 MeV (for 208Pb and 197Au) are also provided.

Non-perturbative many-body treatment of molecular magnets.

Molecular magnets have received significant attention because of their potential applications in quantum information and quantum computing. A delicate balance of electron correlation, spin-orbit coupling (SOC), ligand field splitting, and other effects produces a persistent magnetic moment within each molecular magnet unit. The discovery and design of molecular magnets with improved functionalities would be greatly aided by accurate computations. However, the competition among the different effects poses a challenge for theoretical treatments. Electron correlation plays a central role since d- or f-element ions, which provide the magnetic states in molecular magnets, often require explicit many-body treatments. SOC, which expands the dimensionality of the Hilbert space, can also lead to non-perturbative effects in the presence of strong interaction. Furthermore, molecular magnets are large, with tens of atoms in even the smallest systems. We show how an abinitio treatment of molecular magnets can be achieved with auxiliary-field quantum Monte Carlo, in which electron correlation, SOC, and material specificity are included accurately and on an equal footing. The approach is demonstrated by an application to compute the zero-field splitting of a locally linear Co2+ complex.

Non-perturbative treatment of the solid effect of dynamic nuclear polarization.

In the solid effect of dynamic nuclear polarization (DNP), the concerted flips of the electronic and nuclear spins, which are needed for polarization transfer, are induced by the microwaves. Commonly, the effect of the microwaves is modeled by a rate process whose rate constant is determined perturbatively. According to quantum mechanics, however, the coherent microwave excitation leads to Rabi nutation, which corresponds to a rotation rather than a rate process. Here we reconcile the coherent effect of the microwaves with the description by rate equations by focusing only on the steady state of the spin dynamics. We show that the phenomenological rate constants describing the synchronous excitation of the electronic and nuclear spins can be selected such that the description by rate equations yields the same steady state as the exact quantum-mechanical treatment. The resulting non-perturbative rates differ from the classical, perturbative ones and remain valid also at the high microwave powers used in modern-day DNP. Our treatment of the solid effect highlights the role of the coherences in the mechanistic steps of polarization transfer and reveals the importance of the dispersive (i.e., out-of-phase) component of the EPR line. Interestingly, the multiplicative dependence of the DNP enhancement on the dispersive EPR component was intuited in the very first report of the solid effect in liquids . The time-domain description of the solid effect developed here is extendable to liquids, where the dipolar interaction changes randomly in time due to molecular diffusion.

Charge transfer and ionization cross-sections in collisions of singly charged lithium ions with helium and nitrogen atoms

We present a non-perturbative classical treatment of the charge transfer and ionization processes in collisions between singly charged lithium ions with helium and nitrogen atomic targets. Single capture and single ionization total cross sections are calculated using a three-body classical trajectory Monte Carlo (CTMC) method in which the interaction between the collision partners is described by a Garvey-type model potential. The cross sections are evaluated for collision energies between 20 keV and 100 MeV. In particular, we found excellent agreement between our results and the available experimental data for the case of the single capture of He(1s) by Li+ ions. In addition, our CTMC results are in a reasonable agreement with the experimental results for collision energies higher than 200 keV for single capture of N(2p) atoms by Li+. Furthermore, we present single ionization cross sections for both collision systems.

Time-dependent nuclear-electronic orbital Hartree-Fock theory in a strong uniform magnetic field.

In an ultrastrong magnetic field, with field strength B ≈ B0 = 2.35 × 105 T, molecular structure and dynamics differ strongly from that observed on the Earth. Within the Born-Oppenheimer (BO) approximation, for example, frequent (near) crossings of electronic energy surfaces are induced by the field, suggesting that nonadiabatic phenomena and processes may play a more important role in this mixed-field regime than in the weak-field regime on Earth. To understand the chemistry in the mixed regime, it therefore becomes important to explore non-BO methods. In this work, the nuclear-electronic orbital (NEO) method is employed to study protonic vibrational excitation energies in the presence of a strong magnetic field. The NEO generalized Hartree-Fock theory and time-dependent Hartree-Fock (TDHF) theory are derived and implemented, accounting for all terms that result as a consequence of the nonperturbative treatment of molecular systems in a magnetic field. The NEO results for HCN and FHF- with clamped heavy nuclei are compared against the quadratic eigenvalue problem. Each molecule has three semi-classical modes owing to the hydrogen-two precession modes that are degenerate in the absence of a field and one stretching mode. The NEO-TDHF model is found to perform well; in particular, it automatically captures the screening effects of the electrons on the nuclei, which are quantified through the difference in energy of the precession modes.

Anderson localization at the boundary of a two-dimensional topological superconductor

A one-dimensional boundary of a two-dimensional topological superconductor can host a number of topologically protected chiral modes. Combining two topological superconductors with different topological indices, it is possible to achieve a situation when only a given number of channels ($m$) are topologically protected, while others are not and therefore are subject to Anderson localization in the presence of disorder. We study transport properties of such quasi-one-dimensional quantum wires with broken time-reversal and spin-rotational symmetries (class D) and calculate the average conductance, its variance and the third cumulant, as well as the average shot noise power. The results are obtained for arbitrary wire length, tracing a crossover from the diffusive Drude regime to the regime of strong localization where only $m$ protected channels conduct. Our approach is based on the nonperturbative treatment of the nonlinear supersymmetric sigma model of symmetry class D with two replicas developed in our recent publication [D. S. Antonenko et al., Phys. Rev. B 102, 195152 (2020)]. The presence of topologically protected modes results in the appearance of a topological Wess-Zumino-Witten term in the sigma-model action, which leads to an additional subsidiary series of eigenstates of the transfer-matrix Hamiltonian. The developed formalism can be applied to study the interplay of Anderson localization and topological protection in quantum wires of other symmetry classes.

A DZ white dwarf with a 30 MG magnetic field

ABSTRACTMagnetic white dwarfs with field strengths below 10 MG are easy to recognize since the Zeeman splitting of spectral lines appears proportional to the magnetic field strength. For fields ≳100 MG, however, transition wavelengths become chaotic, requiring quantum-chemical predictions of wavelengths and oscillator strengths with a non-perturbative treatment of the magnetic field. While highly accurate calculations have previously been performed for hydrogen and helium, the variational techniques employed become computationally intractable for systems with more than three to four electrons. Modern computational techniques, such as finite-field coupled-cluster theory, allow the calculation of many-electron systems in arbitrarily strong magnetic fields. Because around 25 per cent of white dwarfs have metal lines in their spectra, and some of those are also magnetic, the possibility arises for some metals to be observed in very strong magnetic fields, resulting in unrecognizable spectra. We have identified SDSS J114333.48+661531.83 as a magnetic DZ white dwarf, with a spectrum exhibiting many unusually shaped lines at unknown wavelengths. Using atomic data calculated from computational finite-field coupled-cluster methods, we have identified some of these lines arising from Na, Mg, and Ca. Surprisingly, we find a relatively low field strength of 30 MG, where the large number of overlapping lines from different elements make the spectrum challenging to interpret at a much lower field strength than for DAs and DBs. Finally, we model the field structure of SDSS J1143+6615 finding the data are consistent with an offset dipole.

Nonperturbative approach to interfacial spin-orbit torques induced by the Rashba effect

Current-induced spin-orbit torque (SOT) in normal metal/ferromagnet (NM/FM) bilayers bears great promise for technological applications, but the microscopic origin of purely interfacial SOTs in ultra-thin systems is not yet fully understood. Here, we show that a linear response theory with a nonperturbative treatment of spin-dependent interactions and impurity scattering potential predicts damping-like SOTs that are strictly absent in perturbative approaches. The technique is applied to a two-dimensional Rashba-coupled ferromagnet (the paradigmatic model of a NM/FM interface), where higher-order scattering processes encoding skew scattering from nonmagnetic impurities allow for current-induced spin polarization with nonzero components along all spatial directions. This is in stark contrast to previous results of perturbative methods (neglecting skew scattering), which predict a coplanar spin-polarization locked perpendicular to the charge current as a result of conventional Rashba-Edelstein effect. Furthermore, the angular dependence of ensuing SOTs and their dependence upon the scattering potential strength is analysed numerically. Simple analytic expressions for the spin-density--charge-current response function, and related SOT efficiencies, are obtained in the weak scattering limit. We find that the extrinsic damping-like torques driven by impurity scattering reaches efficiencies of up to 7% of the field-like (Rashba-Edelstein) torque. Our microscopic theory shows that bulk phenomena, such as the spin Hall effect, are not a necessity in the generation of the damping-like SOTs of the type observed in experiments on ultra-thin systems.

Weak localisation driven by pseudospin-spin entanglement

At low temperatures, quantum corrections, originating from the interference of the many paths an electron may take between two points, tend to dominate the transport properties of two-dimensional conductors. These quantum corrections increase the resistivity in systems such as two-dimensional electron gases (2DEGs) without spin–orbit coupling (SOC), a phenomenon called weak localisation. Including symmetry-breaking SOC leads to a change from weak localisation (WL) to weak anti-localisation (WAL) of the electronic states, i.e. a WL-to-WAL transition. Here, we revisit the Cooperon, the propagator encoding quantum corrections, within the context of ultra-clean graphene-based van der Waals heterostructures with strong symmetry-breaking Bychkov-Rashba SOC to yield two completely counter-intuitive results. Firstly, we find that quantum corrections vary non-monotonically with the SOC strength, a clear indication of non-perturbative physics. Secondly, we observe the exact opposite of that seen in 2DEGs with strong SOC: a WAL-to-WL transition. This dramatic reversal is driven by mode entanglement of the pseudospin and spin degrees of freedom describing graphene’s electronic states. We obtain these results by constructing a non-perturbative treatment of the Cooperon, and observe distinct features in the SOC dependence of the quantum corrections to the electrical conductivity that would otherwise be missed by standard perturbative approaches.

Non-Abelian anyon collider

A collider where particles are injected onto a beam splitter from opposite sides has been used for identifying quantum statistics of identical particles. The collision leads to bunching of the particles for bosons and antibunching for fermions. In recent experiments, a collider was applied to a fractional quantum Hall regime hosting Abelian anyons. The observed negative cross-correlation of electrical currents cannot be understood with fermionic antibunching. Here we predict, based on a conformal field theory and a non-perturbative treatment of non-equilibrium anyon injection, that the collider provides a tool for observation of the braiding statistics of various Abelian and non-Abelian anyons. Its dominant process is not direct collision between injected anyons, contrary to common expectation, but braiding between injected anyons and an anyon excited at the collider. The dependence of the resulting negative cross-correlation on the injection currents distinguishes non-Abelian SU(2)k anyons, Ising anyons, and Abelian Laughlin anyons.

Instability of the ferromagnetic quantum critical point and symmetry of the ferromagnetic ground state in two-dimensional and three-dimensional electron gases with arbitrary spin-orbit splitting

In this work we revisit itinerant ferromagnetism in 2D and 3D electron gases with arbitrary spin-orbit splitting and strong electron-electron interaction. We identify the resonant scattering processes close to the Fermi surface that are responsible for the instability of the ferromagnetic quantum critical point at low temperatures. In contrast to previous theoretical studies, we show that such processes cannot be fully suppressed even in presence of arbitrary spin-orbit splitting. A fully self-consistent non-perturbative treatment of the electron-electron interaction close to the phase transition shows that these resonant processes always destabilize the ferromagnetic quantum critical point and lead to a first-order phase transition. Characteristic signatures of these processes can be measured via the non-analytic dependence of the spin susceptibility on magnetic field both far away or close to the phase transition.