Full Wave Function Research Articles

Exact factorization of the photon-electron-nuclear wavefunction: Formulation and coupled-trajectory dynamics.

We employ the exact-factorization formalism to study the coupled dynamics of photons, electrons, and nuclei at the quantum mechanical level, proposing illustrative examples of model situations of nonadiabatic dynamics and spontaneous emission of electron-nuclear systems in the regime of strong light-matter coupling. We make a particular choice of factorization for such a multi-component system, where the full wavefunction is factored as a conditional electronic amplitude and a marginal photon-nuclear amplitude. Then, we apply the coupled-trajectory mixed quantum-classical (CTMQC) algorithm to perform trajectory-based simulations, by treating photonic and nuclear degrees of freedom on equal footing in terms of classical-like trajectories. The analysis of the time-dependent potentials of the theory along with the assessment of the performance of CTMQC allows us to point out some limitations of the current approximations used in CTMQC. Meanwhile, comparing CTMQC with other trajectory-based algorithms, namely multi-trajectory Ehrenfest and Tully surface hopping, demonstrates the better quality of CTMQC predictions.

Electronic Vector Potential from the Exact Factorization of a Complex Wavefunction.

We generalize the definitions of local scalar potentials named and , which are relevant to properly describe phenomena such as molecular dissociation with density-functional theory, to the case in which the electronic wavefunction corresponds to a complex current-carrying state. In such a case, an extra term in the form of a vector potential appears which cannot be gauged away. Both scalar and vector potentials are introduced via the exact factorization formalism which allows us to express the given Schrödinger equation as two coupled equations, one for the marginal and one for the conditional amplitude. The electronic vector potential is directly related to the paramagnetic current density carried by the total wavefunction and to the diamagnetic current density in the equation for the marginal amplitude. An explicit example of this vector potential in a triplet state of two non-interacting electrons is showcased together with its associated circulation, giving rise to a non-vanishing geometric phase. Some connections with the exact factorization for the full molecular wavefunction beyond the Born-Oppenheimer approximation are also discussed.

Deep learning of many-body observables and quantum information scrambling

Machine learning has shown significant breakthroughs in quantum science, where in particular deep neural networks exhibited remarkable power in modeling quantum many-body systems. Here, we explore how the capacity of data-driven deep neural networks in learning the dynamics of physical observables is correlated with the scrambling of quantum information. We train a neural network to find a mapping from the parameters of a model to the evolution of observables in random quantum circuits for various regimes of quantum scrambling and test its generalization and extrapolation capabilities in applying it to unseen circuits. Our results show that a particular type of recurrent neural network is extremely powerful in generalizing its predictions within the system size and time window that it has been trained on for both, localized and scrambled regimes. These include regimes where classical learning approaches are known to fail in sampling from a representation of the full wave function. Moreover, the considered neural network succeeds in extrapolating its predictions beyond the time window and system size that it has been trained on for models that show localization, but not in scrambled regimes.

Time-Dependent Multireference Coupled-Cluster Method (TDMRCCM) for the Bath-Dynamics in System-Bath Approach to Nonadiabatic Dynamics.

The time-dependent multireference coupled-cluster method (TDMRCCM) fits well in the scheme of the system-bath separation used to study the nonadiabatic dynamics. In TDMRCCM, a projection operator is defined as one that projects the full Hilbert space onto the space spanned by the collection of system degrees of freedom, called the model space. The inverse of this projection operator is a wave operator that acts on the model space and takes its projection back to the full wave function. This wave operator is defined as an exponential of the excitation terms and, hence, can be expanded into a Taylor series, which we have truncated in this work at the second-order of excitations. The attraction of using TDMRCCM for describing the bath dynamics is due to the exponential nature of the ansatz used in the method, which makes it possible for the higher-order excitations to be absorbed by the lower-order terms, even upon truncating the series. This improves the accuracy of the numerical calculations using TDMRCCM as an approximation for the bath-mode dynamics in the system-bath framework for nonadiabatic dynamics. We present the theoretical details of TDMRCCM and the numerical results for implementing this method to study the dynamics in the butatriene cation.

Shell-model study of 58Ni using quantum computing algorithm

This study presents a simulated quantum computing approach for the investigation into the shell-model energy levels of 58Ni through the application of the variational quantum eigensolver (VQE) method in combination with a problem-specific ansatz. The primary objective is to achieve a fully accurate low-lying energy spectrum of 58Ni. The chosen isotope, 58Ni is particularly interesting in nuclear physics through its role in astrophysical reactions while also being a simple but non-trivial nucleus for shell-model study, it being two particles outside a closed shell. Our ansatz, along with the VQE method are shown to be able to reproduce exact energy values for the ground state and first and second excited states. We compare a classical shell model code, the values obtained by diagonalization of the Hamiltonian after qubit mapping, and a noiseless simulated ansatz+VQE simulation. The exact agreement between classical and qubit-mapped diagonalization shows the correctness of our method, and the high accuracy of the simulation means that the ansatz is suitable to allow a full reconstruction of the full nuclear wave function.

Cosmological correlators through the looking glass: reality, parity, and factorisation

We consider the evolution of quantum fields during inflation, and show that the total-energy singularities appearing in the perturbative expansion of the late-time Wavefunction of the Universe are purely real when the external states are massless scalars and massless gravitons. Our proof relies on the tree-level approximation, Bunch-Davies initial conditions, and exact scale invariance (IR-convergence), but without any assumptions on invariance under de Sitter boosts. We consider all n-point functions and allow for the exchange of additional states of any mass and integer spin. Our proof makes use of a decomposition of the inflationary bulk-bulk propagator of massive spinning fields which preserves UV-convergence and ensures that the time-ordered contributions are purely real after we rotate to Euclidean time. We use this reality property to show that the maximally-connected parts of wavefunction coefficients, from which total-energy singularities originate, are purely real. In a theory where all states are in the complementary series, this reality extends to the full wavefunction coefficient. We then use our reality theorem to show that parity-odd correlators (correlators that are mirror asymmetric) are factorised and do not diverge when the total-energy is conserved. We pay special attention to the parity-odd four-point function (trispectrum) of inflationary curvature perturbations and use our reality/factorisation theorems to show that this observable is factorised into a product of cubic diagrams thereby enabling us to derive exact shapes. We present examples of couplings between the inflaton and massive spin-1 and spin-2 fields, with the parity-violation in the trispectrum driven by Chern-Simons corrections to the spinning field two-point function, or from parity-violating cubic interactions which we build within the Effective Field Theory of Inflation. In addition, we present a first-of-its-kind example of a parity-violating trispectrum, generated at tree-level, that arises in a purely scalar theory where the inflaton mixes linearly with an additional massive scalar field.

Calculating Potential Energy Surfaces with Quantum Computers by Measuring Only the Density Along Adiabatic Transitions.

We show that chemically accurate potential energy surfaces (PESs) can be generated from quantum computers by measuring only the density along an adiabatic transition between different molecular geometries. In lieu of using phase estimation, the energy is evaluated by performing line-integration using the inverted real-space time-dependent density functional theory Kohn-Sham (KS) potential obtained from the geometry-varying densities of the full wave function. The accuracy of this method depends on the validity of the adiabatic evolution itself and the potential inversion process (which is theoretically exact but can be numerically unstable), whereas the total evolution time is the defining factor for the precision of phase estimation. We examine the method with a one-dimensional system of two electrons for both the ground and first triplet states in first quantization, as well as the ground state of three- and four-electron systems in second quantization. It is shown that few accurate measurements can be utilized to obtain chemical accuracy across the full potential energy curve, with a shorter propagation time than may be required using phase estimation for a similar accuracy. We also show that an accurate potential energy curve can be calculated by making many imprecise density measurements (using a few shots) along the time evolution and smoothing the resulting density evolution. Finally, it is important to note that the method is able to classically provide a check of its own accuracy by comparing the density resulting from a time-independent KS calculation using the inverted potential with the measured density. This can be used to determine whether longer adiabatic evolution times are required to satisfy the adiabatic theorem.

Disentangling the multiorbital contributions of excitons by photoemission exciton tomography

Excitons are realizations of a correlated many-particle wave function, specifically consisting of electrons and holes in an entangled state. Excitons occur widely in semiconductors and are dominant excitations in semiconducting organic and low-dimensional quantum materials. To efficiently harness the strong optical response and high tuneability of excitons in optoelectronics and in energy-transformation processes, access to the full wavefunction of the entangled state is critical, but has so far not been feasible. Here, we show how time-resolved photoemission momentum microscopy can be used to gain access to the entangled wavefunction and to unravel the exciton’s multiorbital electron and hole contributions. For the prototypical organic semiconductor buckminsterfullerene (C60), we exemplify the capabilities of exciton tomography and achieve unprecedented access to key properties of the entangled exciton state including localization, charge-transfer character, and ultrafast exciton formation and relaxation dynamics.

Transfer learning from Hermitian to non-Hermitian quantum many-body physics

Identifying phase boundaries of interacting systems is one of the key steps to understanding quantum many-body models. The development of various numerical and analytical methods has allowed exploring the phase diagrams of many Hermitian interacting systems. However, numerical challenges and scarcity of analytical solutions hinder obtaining phase boundaries in non-Hermitian many-body models. Recent machine learning methods have emerged as a potential strategy to learn phase boundaries from various observables without having access to the full many-body wavefunction. Here, we show that a machine learning methodology trained solely on Hermitian correlation functions allows identifying phase boundaries of non-Hermitian interacting models. These results demonstrate that Hermitian machine learning algorithms can be redeployed to non-Hermitian models without requiring further training to reveal non-Hermitian phase diagrams. Our findings establish transfer learning as a versatile strategy to leverage Hermitian physics to machine learning non-Hermitian phenomena.

Antisymmetrization of the wave functions consisting of spin-isospin and hyperspherical parts

In order to investigate few-particle hypernuclei within the framework of the Hyperspherical Function Method, it is necessary to obtain full wave functions that are anti-symmetric under particle interchange. These wave functions must include not only hyperspherical, but also spin-isospin parts. According to the Parentage Scheme of Symmetrization, N-particle hyperspherical functions (N=3,4,5,6…) symmetrized with respect to (N-1)-particles, can be obtained from the N-particle hyperspherical functions with arbitrary quantum numbers by the use of the transformation coefficients related with the permutations of the last two particles. This article explains how to obtain fully antisymmetrized wave functions consisting of spin-isospin and hyperspherical parts. It is demonstrated that there are sixteen possible combinations in (3+1) configuration and 12 possible combinations in (2+2) configuration when spin and isospin functions are represented by [4], [31], and [22] representations of the four-particle permutation group S4. A complete set of the fully antisymmetrized four-particle wave functions is obtained. It is demonstrated that proposed mathematical formalism can be easily generalized to obtain fully antisymmetrized wave functions for the systems of five and more particles.

Quantum-mechanical four-body versus semi-classical three-body theories for double charge exchange in collisions of fast alpha particles with helium targets

AbstractWithin the two-channel distorted wave second-order perturbative theoretical formalism, we study capture of both electrons from helium-like targets by heavy nuclei as projectiles at intermediate and high impact energies. The emphasis is on the four-body single-double scattering (SDS-4B) method and the three-body continuum distorted wave impact parameter method (CDW-3B-IPM). The SDS-4B method deals with the full quantum-mechanical correlative dynamics of all the four interactively participating particles (two electrons, two nuclei). The CDW-3B-IPM is a semi-classical three-body independent particle model (one electron, two nuclei), using a combinatorial calculus to describe double capture by a product of two uncorrelated probabilities, integrated over impact parameters. Both theories share a common feature in having altogether two electronic full Coulomb continuum wave functions. One such function is centered on the projectile nucleus in the entrance channel, whereas the other is centered on the target nucleus in the exit channel. These two methods satisfy the correct initial and final Coulomb boundary conditions in the asymptotic region of scattering, at infinitely large inter-particle separations. Yet, it is presently demonstrated that most of the available experimental data on total cross sections for the double capture from helium by alpha particles distinctly favor the SDS-4B method. This is especially true at intermediate energies. Such energies are critically important in versatile applications under the general umbrella of ion transport in matter, including thermonuclear fusion (plasma physics) and ion therapy (medicine).

Effective quantum volume, fidelity and computational cost of noisy quantum processing experiments

Today’s experimental noisy quantum processors can compete with and surpass all known algorithms on state-of-the-art supercomputers for the computational benchmark task of Random Circuit Sampling (Boixo et al., 2018, Arute et al., 2019, Wu et al., 2021, Zhu et al., 2022, Morvan et al., 2023). Additionally, a circuit-based quantum simulation of quantum information scrambling (Mi et al., 2021), which measures a local observable, has already outperformed standard full wave function simulation algorithms, e.g., exact Schrodinger evolution and Matrix Product States (MPS). However, this experiment has not yet surpassed tensor network contraction for computing the value of the observable. Based on those studies, we provide a unified framework that utilizes the underlying effective circuit volume to explain the tradeoff between the experimentally achievable signal-to-noise ratio for a specific observable, and the corresponding computational cost. We apply this framework to recent quantum processor experiments of Random Circuit Sampling (Morvan et al., 2023), quantum information scrambling (Mi et al., 2021), and a Floquet circuit unitary (Kim et al., 2023). This allows us to reproduce the results of Ref. (Kim et al., 2023) in less than one second per data point using one GPU.

Reviving product states in the disordered Heisenberg chain

When a generic quantum system is prepared in a simple initial condition, it typically equilibrates toward a state that can be described by a thermal ensemble. A known exception is localized systems that are non-ergodic and do not thermalize; however, local observables are still believed to become stationary. Here we demonstrate that this general picture is incomplete by constructing product states that feature periodic high-fidelity revivals of the full wavefunction and local observables that oscillate indefinitely. The system neither equilibrates nor thermalizes. This is analogous to the phenomenon of weak ergodicity breaking due to many-body scars and challenges aspects of the current phenomenology of many-body localization, such as the logarithmic growth of the entanglement entropy. To support our claim, we combine analytic arguments with large-scale tensor network numerics for the disordered Heisenberg chain. Our results hold for arbitrarily long times in chains of 160 sites up to machine precision.

Program for quantum wave-packet dynamics with time-dependent potentials (new version announcement)

wavepacket is a program to simulate the dynamics of a wave packet interacting with a time-dependent potential, with the time-dependent Schrödinger equation being solved on a one-, two-, or three-dimensional spatial grid using the split operator method. This new version fixes bugs present in the original program. New version program summaryProgram Title: wavepacketCPC Library link to program files:https://doi.org/10.17632/gnxmkygxrw.1Licensing provisions: GPLv3Programming language: C (iso C99)Journal reference of previous version: Comput. Phys. Commun. 185 (2014) 407–414.Does the new version supersede the previous version?: YesReasons for the new version: Bug fixes.Summary of revisions: This new version fixes bugs in the program wavepacket [1]. In the original version, the function print_wf_bin, used (optionally) to write out the wave function as a binary file, contained a bug that would result in only part of the full wave function being written out when the program was run in parallel.Additionally, negative values of the parameters nt and/or nprint could lead to the program being stuck in an infinite loop. Additional checks have been added to ensure that both these parameters are positive (or zero).Nature of problem: Solves the time-dependent Schrödinger equation for a single particle interacting with a time-dependent potential.Solution method: The wave function is described by its value on a spatial grid and the evolution operator is approximated using the split-operator method [2,3], with the kinetic energy operator calculated using a Fast Fourier Transform.Additional comments including restrictions and unusual features: Simulation can be in one, two, or three dimensions. The fftw [4] implementation of the fast Fourier transform is used, so the corresponding library must be installed. Serial and parallel versions are compiled from the same source files. The parallel version is based on the Message-Passing Interface (mpi) [5].

Majorana’s approach to nonadiabatic transitions validates the adiabatic-impulse approximation

The approach by Ettore Majorana for non-adiabatic transitions between two quasi-crossing levels is revisited and significantly extended. We rederive the transition probability, known as the Landau–Zener–Stückelberg–Majorana formula, and introduce Majorana’s approach to modern readers. This result, typically referred as the Landau–Zener formula, was published by Majorana before Landau, Zener and Stückelberg. Moreover, we go well beyond previous results and we now obtain the full wave function, including its phase, which is important nowadays for quantum control and quantum information. The asymptotic wave function correctly describes the dynamics away from the avoided-level crossing, while it has limited accuracy in that region.

Factorized Electron-Nuclear Dynamics with an Effective Complex Potential.

We present a quantum dynamics approach for molecular systems based on wave function factorization into components describing the light and heavy particles, such as electrons and nuclei. The dynamics of the nuclear subsystem can be viewed as motion of the trajectories defined in the nuclear subspace, evolving according to the average nuclear momentum of the full wave function. The probability density flow between the nuclear and electronic subsystems is facilitated by the imaginary potential, derived to ensure a physically meaningful normalization of the electronic wave function for each configuration of the nuclei, and conservation of the probability density associated with each trajectory in the Lagrangian frame of reference. The imaginary potential, defined in the nuclear subspace, depends on the momentum variance in the nuclear coordinates averaged over the electronic component of the wave function. An effective real potential, driving the dynamics of the nuclear subsystem, is defined to minimize motion of the electronic wave function in the nuclear degrees of freedom. Illustration and the analysis of the formalism are given for a two-dimensional model system of vibrationally nonadiabatic dynamics.

Coherent Plasma in a Lattice

We present a fully second-quantized calculation showing the emergence of spontaneous coherent configurations of the electromagnetic field interacting with charged bosons in a regular lattice. The bosons tend to oscillate at their plasma frequency, and in addition are subjected to electrostatic forces which keep them confined close to the lattice sites while causing a frequency shift in the oscillation. Under certain conditions upon these frequencies, we find that a suitably defined set of coherent states (coherent both in the field and matter degrees of freedom) exhibit a negative energy gap with respect to the perturbative ground state. This is true in the RWA approximation and for position-independent fields to both the first and second order in the interaction Hamiltonian. We compare this result with other recent findings from cavity QED, and note that (1) consideration of full 3D wavefunctions and a careful definition of the coherent states are essential for obtaining the energy gap, and (2) although our calculation is made in reference to bosons, it may apply to protons bound in a crystal matrix as well if their density is very low compared to the density of available states.

Nonequilibrium Hole Dynamics in Antiferromagnets: Damped Strings and Polarons

We develop a nonperturbative theory for hole dynamics in antiferromagnetic spin lattices, as described by the t-J model. This is achieved by generalizing the self-consistent Born approximation to nonequilibrium systems, making it possible to calculate the full time-dependent many-body wave function. Our approach reveals three distinct dynamical regimes, ultimately leading to the formation of magnetic polarons. Following the initial ballistic stage of the hole dynamics, coherent formation of string excitations gives rise to characteristic oscillations in the hole density. Their damping eventually leaves behind magnetic polarons that undergo ballistic motion with a greatly reduced velocity. The developed theory provides a rigorous framework for understanding nonequilibrium physics of defects in quantum magnets and quantitatively explains recent observations from cold-atom quantum simulations in the strong coupling regime.

Reduced-density-matrix-based ab initio cavity quantum electrodynamics

A reduced-density-matrix (RDM)-based approach to {\em ab initio} cavity quantum electrodynamics (QED) is developed. The expectation value of the Pauli-Fierz Hamiltonian is expressed in terms of one- and two-body electronic and photonic RDMs, and the elements of these RDMs are optimized directly in polynomial time by semidefinite programming techniques, without knowledge of the full wave function. QED generalizations of important ensemble $N$-representability conditions are derived and enforced in this procedure. The resulting approach is applied to the description of classic ground-state strong electron correlation problems, augmented by the presence of ultrastrong light-matter coupling. First, we assess cavity-induced changes to the singlet-triplet energy gap of the linear oligoacene series; for a heptacene molecule, this gap can change by as much as 1.9 kcal mol$^{-1}$ (or 15\%) when the molecule is aligned along the cavity mode polarization axis. We also explore the metal-insulator transition in linear hydrogen chains and demonstrate that strong electron-photon interactions increase the insulating character of these systems under all coupling strengths considered.

Visualization of nuclear many-body correlations with the most probable configuration of nucleons

A method to visualize many-body correlations using the information of the full wave function is presented. The set of nucleon coordinates which maximizes the square of the wave function, that is, the most probable spatial configuration of nucleons, is visualized. The method is applied to Hartree-Fock (HF) and HF+BCS wave functions of $p$- and $sd$-shell $N=Z$ even-even nuclei to analyze the many-body correlations in those systems. It is found that there are $\alpha$-cluster-like four-body correlations already at the HF level in some of the nuclei. The effects of pairing on the most probable configuration are also investigated. The method is useful to analyze the nuclear many-body correlations, and it suggests a new viewpoint to microscopic nuclear wave functions.