Quantum Dynamical Problems Research Articles

Resource Optimization for Quantum Dynamics with Tensor Networks: Quantum and Classical Algorithms.

The exponential scaling of the quantum degrees of freedom with the size of the system is one of the biggest challenges in computational chemistry and particularly in quantum dynamics. We present a tensor network approach for the time-evolution of the nuclear degrees of freedom of multiconfigurational chemical systems at a reduced storage and computational complexity. We also present quantum algorithms for the resultant dynamics. To preserve the compression advantage achieved via tensor network decompositions, we present an adaptive algorithm for the regularization of nonphysical bond dimensions, preventing the potentially exponential growth of these with time. While applicable to any quantum dynamical problem, our method is particularly valuable for dynamical simulations of nuclear chemical systems. Our algorithm is demonstrated using ab initio potentials obtained for a symmetric hydrogen-bonded system, namely, the protonated 2,2'-bipyridine, and compared to exact diagonalization numerical results.

Quantum kernels for classifying dynamical singularities in a multiqubit system

Dynamical quantum phase transition is a critical phenomenon involving out-of-equilibrium states and broken symmetries without classical analogy. However, when finite-sized systems are analyzed, dynamical singularities of the rate function can appear, leading to a challenging physical characterization when parameters are changed. Here, we report a quantum support vector machine algorithm that uses quantum Kernels to classify dynamical singularities of the rate function for a multiqubit system. We illustrate our approach using N long-range interacting qubits subjected to an arbitrary magnetic field, which induces a quench dynamics. Inspired by physical arguments, we introduce two different quantum Kernels, one inspired by the ground state manifold and the other based on a single state tomography. Our accuracy and adaptability results show that this quantum dynamical critical problem can be efficiently solved using physically inspiring quantum Kernels. Moreover, we extend our results for the case of time-dependent fields, quantum master equation, and when we increase the number of qubits.

High accuracy exponential decomposition of bath correlation functions for arbitrary and structured spectral densities: Emerging methodologies and new approaches.

This study investigates the decomposition of bath correlation functions (BCFs) in terms of complex exponential functions, with an eye on the realistic modeling of open quantum systems based on the hierarchical equations of motion. We introduce the theoretical background of various decomposition schemes in both time and frequency domains and assess their efficiency and accuracy by demonstrating the decomposition of various BCFs. We further develop a new procedure for the decomposition of BCFs originating from highly structured spectral densities with a high accuracy and compare it with existing fitting techniques. Advantages and disadvantages of each methodology are discussed in detail with special attention to their application to the corresponding quantum dynamical problem. This work provides fundamental tools for choosing and using a variety of decomposition techniques of BCFs for the study of open quantum systems in structured environments.

Beyond Fermi's golden rule with the statistical Jacobi approximation

Many problems in quantum dynamics can be cast as the decay of a single quantum state into a continuum. The time-dependent overlap with the initial state, called the fidelity, characterizes this decay. We derive an analytic expression for the fidelity after a quench to an ergodic Hamiltonian. The expression is valid for both weak and strong quenches, and timescales before finiteness of the Hilbert space limits the fidelity. It reproduces initial quadratic decay and asymptotic exponential decay with a rate which, for strong quenches, differs from Fermi’s golden rule. The analysis relies on the statistical Jacobi approximation (SJA), which was originally applied in nearly localized systems, and which we here adapt to well-thermalizing systems. Our results demonstrate that the SJA is predictive in disparate regimes of quantum dynamics.

Complex time method for quantum dynamics when an exceptional point is encircled in the parameter space

We revisit the complex time method for the application to quantum dynamics as an exceptional point is encircled in the parameter space of the Hamiltonian. The basic idea of the complex time method is using complex contour integration to perform the first-order adiabatic perturbation integral. In this way, the quantum dynamical problem is transformed to a study of singularities in the complex time plane – transition points – which represent complex degeneracies of the adiabatic Hamiltonian as the time-dependent parameters defining the encircling contour are analytically continued to complex plane. As an underlying illustration of the approach we discuss a switch between Rabi oscillations and rapid adiabatic passage which occurs upon the encircling of an exceptional point in a special time-symmetric case.

A Symplectic Algorithm for Constrained Hamiltonian Systems

In this paper, a symplectic algorithm is utilized to investigate constrained Hamiltonian systems. However, the symplectic method cannot be applied directly to the constrained Hamiltonian equations due to the non-canonicity. We firstly discuss the canonicalization method of the constrained Hamiltonian systems. The symplectic method is used to constrain Hamiltonian systems on the basis of the canonicalization, and then the numerical simulation of the system is carried out. An example is presented to illustrate the application of the results. By using the symplectic method of constrained Hamiltonian systems, one can solve the singular dynamic problems of nonconservative constrained mechanical systems, nonholonomic constrained mechanical systems as well as physical problems in quantum dynamics, and also available in many electromechanical coupled systems.

Quantum channel marginal problem

Given a set of local dynamics, are they compatible with a global dynamics? We systematically formulate these questions as quantum channel marginal problems. These problems are strongly connected to the generalization of the no-signaling conditions to quantized inputs and outputs and can be understood as a general toolkit to study notions of quantum incompatibility. In fact, they include as special cases channel broadcasting, channel extendibility, measurement compatibility, and state marginal problems. After defining the notion of compatibility between global and local dynamics, we provide a solution to the channel marginal problem that takes the form of a semidefinite program. Using this formulation, we construct channel incompatibility witnesses, discuss their operational interpretation in terms of an advantage for a state-discrimination task, prove a gap between classical and quantum dynamical marginal problems and show that the latter is irreducible to state marginal problems.

Manipulating the dynamics of a Fermi resonance with light. A direct optimal control theory approach

Direct optimal control theory for quantum dynamical problems presents itself as an interesting alternative to the traditional indirect optimal control. The method relies on the first discretize and then optimize paradigm, where a discretization of the dynamical equations leads to a nonlinear optimization problem. It has been applied successfully to the control of a bistable system where the wavepacket had been approximated by a parameterized Gaussian, leading to a semiclassical set of equations of motion (A. R. Ramos Ramos, O. K\"uhn, Front. Phys. 9 (2021) 615168). Motivated by these results, in the present paper we extend the application of the method to the case of exact wavepacket propagation using the example of a generic Fermi-resonance model. In particular we address the question how population of the involved overtone state can be avoided such as to reduce the effect of intramolecular vibrational energy redistribution. A methodological advantage is that direct optimal control theory offers flexibility when choosing the running cost, since there is no need to compute functional derivatives and coupling terms as in the case of indirect optimal control. We exploit this fact to include state populations in the running cost, which allows their optimization.

Finite temperature quantum dynamics of complex systems: Integrating thermo‐field theories and tensor‐train methods

AbstractThis review provides the fundamental theoretical tools for the development of a complete wave‐function formalism for the study of time‐evolution of chemico‐physical systems at finite temperature. The methodology is based on the non‐equilibrium thermo‐field dynamics (NE‐TFD) representation of quantum mechanics, which is alternative to the commonly used density matrix representation. TFD concepts are extended and integrated with the tensor‐train (TT) numerical tools leading to a novel and powerful theoretical and computational framework for the study of complex quantum dynamical problems. In addition, NE‐TFD techniques are extended to enable the study of dissipative open systems via a new formulation of the hierarchical equations of motion (HEOM) fully integrated with TT methodologies. We demonstrate that the combination of the TFD machinery with computational advantages of TTs results in a powerful theoretical and computational framework for scrutinizing dynamics of complex multidimensional electron‐vibrational systems. We illustrate the validity and the computational advantages of the developed methodologies by applying them to the study of quantum coherence effects in the energy‐transfer processes in antenna systems, to the analysis of fingerprints of vibrational modes in electron‐transfer and charge‐transfer processes in various model and realistic multidimensional molecular systems, as well as to simulation of other fundamental models of physical chemistry.This article is categorized under: Theoretical and Physical Chemistry > Reaction Dynamics and Kinetics Theoretical and Physical Chemistry > Statistical Mechanics

Quantum dynamics of vibrational energy flow in oscillator chains driven by anharmonic interactions

A new model of vibrational energy transfer in molecular systems taking into account anharmonic (third order) interactions of localized vibrations with a chain of harmonic oscillators is developed. The role of the energy spectrum of the chain and of the magnitude of the non-linear coupling is discussed in detail by an exact numerical solution of the quantum dynamical problem based on the tensor-train (matrix product state) representation of the vibrational wave function. Results show that the type of wave packet motion is determined by the eigen-spectrum of the chain and by its excitation time. It is found that when the excitation of the chain takes place on a much shorter timescale than the energy transfer along the chain the vibrational wave packet moves in a ballistic way independently of the length of the chain. On the other hand when the excitation of the chain takes place on the timescale of the energy transfer along the chain the overall motion becomes superballistic. These findings shed new light on recent observations of ballistic energy transfer along polymethylene chains.

Bayesian optimization for inverse problems in time-dependent quantum dynamics.

We demonstrate an efficient algorithm for inverse problems in time-dependent quantum dynamics based on feedback loops between Hamiltonian parameters and the solutions of the Schrödinger equation. Our approach formulates the inverse problem as a target vector estimation problem and uses Bayesian surrogate models of the Schrödinger equation solutions to direct the optimization of feedback loops. For the surrogate models, we use Gaussian processes with vector outputs and composite kernels built by an iterative algorithm with the Bayesian information criterion (BIC) as a kernel selection metric. The outputs of the Gaussian processes are designed to model an observable simultaneously at different time instances. We show that the use of Gaussian processes with vector outputs and the BIC-directed kernel construction reduces the number of iterations in the feedback loops by, at least, a factor of 3. We also demonstrate an application of Bayesian optimization for inverse problems with noisy data. To demonstrate the algorithm, we consider the orientation and alignment of polyatomic molecules SO2 and propylene oxide (PPO) induced by strong laser pulses. We use simulated time evolutions of the orientation or alignment signals to determine the relevant components of the molecular polarizability tensors. We show that, for the five independent components of the polarizability tensor of PPO, this can be achieved with as few as 30 quantum dynamics calculations.

Dzyaloshinskii-Moriya and dipole-dipole interactions affect coupling-based Landau-Majorana-Stückelberg-Zener transitions

It has been theoretically demonstrated that two spins (qubits or qutrits), coupled by exchange interaction only, undergo a coupling-based joint Landau-Majorana-St\"uckelberg-Zener (LMSZ) transition when a linear ramp acts upon one of the two spins. Such a transition, under appropriate conditions on the parameters, drives the two-spin system toward a maximally entangled state. In this paper, effects on the quantum dynamics of the two qudits, stemming from the Dzyaloshinskii-Moriya (DM) and dipole-dipole (d-d) interactions, are investigated qualitatively and quantitatively. The enriched Hamiltonian model of the two spins, shares with the previous microscopic one the same C2-symmetry which once more brings about an exact treatment of the new quantum dynamical problem. This paper transparently reveals that the DM and d-d interactions generate independent, enhancing or hindering, modifications in the dynamical behaviour predicted for the two spins coupled exclusively by the exchange interaction. It is worthy noticing that, on the basis of the theory here developed, the measurement of the time evolution of the magnetization in a controlled LMSZ scenario, can furnish information on the relative weights of the three kinds of couplings describing the spin system. This possibility is very important since it allows in principle to legitimate the choice of the microscopic model to be adopted in a given physical scenario.

Experimental extraction of the quantum effective action for a non-equilibrium many-body system

Far-from-equilibrium situations are ubiquitous in nature. They are responsible for a wealth of phenomena, which are not simple extensions of near-equilibrium properties, ranging from fluid flows turning turbulent to the highly organized forms of life. On the fundamental level, quantum fluctuations or entanglement lead to novel forms of complex dynamical behaviour in many-body systems for which a description as emergent phenomena can be found within the framework of quantum field theory. A central quantity in these efforts, containing all information about the measurable physical properties, is the quantum effective action. Though the problem of non-equilibrium quantum dynamics can be exactly formulated in terms of the quantum effective action, the solution is in general beyond capabilities of classical computers. In this work, we present a strategy to determine the non-equilibrium quantum effective action using analog quantum simulators, and demonstrate our method experimentally with a quasi one-dimensional spinor Bose gas out of equilibrium. Building on spatially resolved snapshots of the spin degree of freedom, we infer the quantum effective action up to fourth order in an expansion in one-particle irreducible correlation functions at equal times. We uncover a strong suppression of the irreducible four-vertex emerging at low momenta, which solves the problem of dynamics in the highly occupied regime far from equilibrium where perturbative descriptions fail. Similar behaviour in this non-pertubative regime has been proposed in the context of early-universe cosmology. Our work constitutes a new realm of large-scale analog quantum computing, where the high level of control of synthetic quantum systems provides the means for the solution of long-standing theoretical problems in high-energy and condensed matter physics with an experimental approach.

2D nondirect product discrete variable representation for Schrödinger equation with nonseparable angular variables

We develop a nondirect product discrete variable representation (npDVR) for treating quantum dynamical problems which involve nonseparable angular variables. The npDVR basis is constructed on spherical functions orthogonalized on the grids of the Lebedev or Popov 2D quadratures for the unit sphere instead of the direct product of 1D quadrature rules. We compare our computational scheme with the old one that used the product of 1D Gaussian quadratures in terms of their convergence and efficiency by calculating, as an example, the spectrum of a hydrogen atom in the magnetic and electric fields arbitrarily oriented to one another. The use of the npDVR based on the Lebedev or Popov 2D quadratures substantially accelerates the convergence of the computational scheme. Moreover, we get the fastest convergence with the npDVR based on the Popov quadratures, which has the largest efficiency coefficient.

Harnessing deep neural networks to solve inverse problems in quantum dynamics: machine-learned predictions of time-dependent optimal control fields.

Inverse problems continue to garner immense interest in the physical sciences, particularly in the context of controlling desired phenomena in non-equilibrium systems. In this work, we utilize a series of deep neural networks for predicting time-dependent optimal control fields, E(t), that enable desired electronic transitions in reduced-dimensional quantum dynamical systems. To solve this inverse problem, we investigated two independent machine learning approaches: (1) a feedforward neural network for predicting the frequency and amplitude content of the power spectrum in the frequency domain (i.e., the Fourier transform of E(t)), and (2) a cross-correlation neural network approach for directly predicting E(t) in the time domain. Both of these machine learning methods give complementary approaches for probing the underlying quantum dynamics and also exhibit impressive performance in accurately predicting both the frequency and strength of the optimal control field. We provide detailed architectures and hyperparameters for these deep neural networks as well as performance metrics for each of our machine-learned models. From these results, we show that machine learning, particularly deep neural networks, can be employed as cost-effective statistical approaches for designing electromagnetic fields to enable desired transitions in these quantum dynamical systems.

Open quantum dynamics of a three-dimensional rotor calculated using a rotationally invariant system-bath Hamiltonian: Linear and two-dimensional rotational spectra.

We consider a rotationally invariant system-bath (RISB) model in three-dimensional space that is described by a linear rigid rotor independently coupled to three harmonic-oscillator baths through functions of the rotor's Euler angles. While this model has been developed to study the dielectric relaxation of a dipolar molecule in solvation as a problem of classical Debye relaxation, here we investigate it as a problem of open quantum dynamics. Specifically, the treatment presented here is carried out as an extension of a previous work [Y. Iwamoto and Y. Tanimura, J. Chem. Phys 149, 084110 (2018)], in which we studied a two-dimensional (2D) RISB model, to a three-dimensional (3D) RISB model. As in the 2D case, due to a difference in the energy discretization of the total Hamiltonian, the dynamics described by the 3D RISB model differ significantly from those described by the rotational Caldeira-Leggett model. To illustrate the characteristic features of the quantum 3D rotor system described by angular momentum and magnetic quantum numbers, we derive a quantum master equation (QME) and hierarchical equations of motion for the 3D RISB model in the high-temperature case. Using the QME, we compute linear and 2D rotational spectra defined by the linear and nonlinear response functions of the rotor dipole, respectively. The quantum transitions between the angular momentum states and magnetic states arising from polarized Stark fields as well as the system-bath interactions can be clearly observed in 2D rotational spectroscopy.

Density matrix dynamics in twin-formulation: An efficient methodology based on tensor-train representation of reduced equations of motion

The twin-formulation of quantum statistical mechanics is employed to describe a new methodology for the solution of the equations of motion of the reduced density matrix in their hierarchical formulation. It is shown that the introduction of tilde operators and of their algebra in the dual space greatly simplifies the application of numerical techniques for the propagation of the density matrix. The application of tensor-train representation of a vector to solve complex quantum dynamical problems within the framework of the twin-formulation is discussed. Next, applications of the hierarchical equations of motion to a dissipative polaron model are presented showing the validity and accuracy of the new approach.

Features of localized plasmons formation in four-particle spaser systems

The article is focused on the management problem of quantum dynamics of localized plasmons in model of a four-particle spaser which consists of metal nanoparticles and semiconductor quantum dots. The conditions for observation stable stationary regime of plasmon formation in the presented model have been determined by the use of mean field approximation.

PsiQuaSP\u2013A library for efficient computation of symmetric open quantum systems

In a recent publication we showed that permutation symmetry reduces the numerical complexity of Lindblad quantum master equations for identical multi-level systems from exponential to polynomial scaling. This is important for open system dynamics including realistic system bath interactions and dephasing in, for instance, the Dicke model, multi-Λ system setups etc. Here we present an object-oriented C++ library that allows to setup and solve arbitrary quantum optical Lindblad master equations, especially those that are permutationally symmetric in the multi-level systems. PsiQuaSP (Permutation symmetry for identical Quantum Systems Package) uses the PETSc package for sparse linear algebra methods and differential equations as basis. The aim of PsiQuaSP is to provide flexible, storage efficient and scalable code while being as user friendly as possible. It is easily applied to many quantum optical or quantum information systems with more than one multi-level system. We first review the basics of the permutation symmetry for multi-level systems in quantum master equations. The application of PsiQuaSP to quantum dynamical problems is illustrated with several typical, simple examples of open quantum optical systems.

An example of interplay between Physics and Mathematics: Exact resolution of a new class of Riccati Equations

A novel recipe for exactly solving in finite terms a class of special differential Riccati equations is reported. Our procedure is entirely based on a successful resolution strategy quite recently applied to quantum dynamical time-dependent SU(2) problems. The general integral of exemplary differential Riccati equations, not previously considered in the specialized literature, is explicitly determined to illustrate both mathematical usefulness and easiness of applicability of our proposed treatment. The possibility of exploiting the general integral of a given differential Riccati equation to solve an SU(2) quantum dynamical problem, is succinctly pointed out.