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The Journal of Chemical Physics

Compacting the density matrix in quantum dynamics: Singular value decomposition of the surprisal and the dominant constraints for anharmonic systems

Ksenia Komarova, F. Remacle, Raphael David Levine

Published Nov 9, 2021• 8 citations
Publisher

Abstract

We introduce a practical method for compacting the time evolution of the quantum state of a closed physical system. The density matrix is specified as a function of a few time-independent observables where their coefficients are time-dependent. The key mathematical step is the vectorization of the surprisal, the logarithm of the density matrix, at each time point of interest. The time span used depends on the required spectral resolution. The entire course of the system evolution is represented as a matrix where each column is the vectorized surprisal at the given time point. Using singular value decomposition, SVD, of this matrix we generate realistic approximations for the time-independent observables and their respective time dependent coefficients. This allows a simplification of the algebraic procedure for determining the dominant constraints (the time-independent observables) in the sense of the maximal entropy approach. A nonstationary coherent initial state of a Morse oscillator is used to introduce the approach. We derive analytical exact expression for the surprisal as a function of time and this offers a benchmark for comparison with the accurate but approximate SVD results. We discuss two examples of a Morse potential of different anharmonicities, the H2 and I2 molecules. We further demonstrate the approach for a two coupled electronic states problem, the well studied non radiative decay of pyrazine from its bright state. Five constraints are found to be enough to capture the ultrafast electronic population exchange and to recover the dynamics of the wave packet in both electronic states.

DOI
10.1063/5.0072351

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We introduce a practical method for compacting the time evolution of the quantum state of a closed physical system. The density matrix is specified as a function of a few time-independent observables where their coefficients are time-dependent. The key mathematical step is the vectorization of the surprisal, the logarithm of the density matrix, at each time point of interest. The time span used depends on the required spectral resolution. The entire course of the system evolution is represented as a matrix where each column is the vectorized surprisal at the given time point. Using singular value decomposition, SVD, of this matrix we generate realistic approximations for the time-independent observables and their respective time dependent coefficients. This allows a simplification of the algebraic procedure for determining the dominant constraints (the time-independent observables) in the sense of the maximal entropy approach. A nonstationary coherent initial state of a Morse oscillator is used to introduce the approach. We derive analytical exact expression for the surprisal as a function of time and this offers a benchmark for comparison with the accurate but approximate SVD results. We discuss two examples of a Morse potential of different anharmonicities, the H2 and I2 molecules. We further demonstrate the approach for a two coupled electronic states problem, the well studied non radiative decay of pyrazine from its bright state. Five constraints are found to be enough to capture the ultrafast electronic population exchange and to recover the dynamics of the wave packet in both electronic states.
A lossless, exact compaction of the time-evolved state of the quantum dynamical system of a perturbed anharmonic molecule is demonstrated using dynamical symmetries. The density matrix of the anharmonic molecule is a linear combination of these symmetries, and it remains so as a time-dependent perturbation is applied. Accurate, unitary-but-approximate, and thereby irreversible compaction is further shown using fewer symmetries, and the fidelity of this lossy compaction is quantified. Perturbations are typically linear in the operators of a Lie algebra. For a Hamiltonian that is also linear, one knows well how to reversibly compact the state of a dynamical system. However, anharmonic vibrations have a finite number of unequally spaced energy levels, and a good description of their spectra typically requires an algebraic-type Hamiltonian that is bilinear in the operators of a Lie algebra. For a bilinear Hamiltonian we show how a matrix-based approach allows us to compact both the populations and the coherences, either exactly reversibly or inexactly irreversibly, with fewer symmetries. A forced Morse oscillator is used as an explicit analytical and numerical example covering the entire range of dynamics from the sudden to the adiabatic limits.
High Resolution Image Download MS PowerPoint Slide A practical approach is put forward for a compact representation of the time evolving density matrix of the forced Morse oscillator. This approach uses the factorized product form of the unitary time evolution operator, à la Wei-Norman. This product form casts the time evolution operator in the basis of operators that form a closed Lie algebra. The further requirement that the Hamiltonian of the system be closed within this Lie algebra is satisfied by restricting the dynamics to its sudden limit. One is thereby able to propagate in time both pure and mixed quantum states. As an example, for a thermal initial state, the time-evolved density matrix of maximum entropy is derived, and it is compacted to be described by only three explicit constraints: one time-dependent constraint, which is a dynamical symmetry, and two constants of the motion, with corresponding time-independent coefficients. This representation is a significant reduction from O ( j 2 ) constraints down to just three, where j is the number of bound states of the Morse oscillator.
When the amount of entanglement in a quantum system is limited, the relevant dynamics of the system is restricted to a very small part of the state space. When restricted to this subspace the description of the system becomes efficient in the system size. A class of algorithms, exemplified by the time-evolving block-decimation (TEBD) algorithm, make use of this observation by selecting the relevant subspace through a decimation technique relying on the singular value decomposition (SVD). In these algorithms, the complexity of each time-evolution step is dominated by the SVD. Here we show that, by applying a randomized version of the SVD routine (RRSVD), the power law governing the computational complexity of TEBD is lowered by one degree, resulting in a considerable speed-up. We exemplify the potential gains in efficiency at the hand of some real world examples to which TEBD can be successfully applied and demonstrate that for those systems RRSVD delivers results as accurate as state-of-the-art deterministic SVD routines.
An attosecond optical pulse can entangle coherently related states of different characters, such as electronic and vibrational, in a molecular system. Using a quantum information theoretic approach, we explicitly define and discuss the surprisal of such a system in the maximal entropy formalism and identify the constraints and their conjugate Lagrange multipliers. Surprisal analysis shows how these constraints become fewer and simpler in the sudden approximation of the dynamics, a limit often valid for an ultrafast excitation. The optically accessible lower electronic states of N2 are used as a numerical example to show the compaction of the dynamics from On2 down to On constraints, where n is the number of vibronic states. The von Neumann entropy is used to confirm the fidelity of the compaction.
Several techniques to solve a hierarchical set of equations of motion for propagating a reduced density matrix coupled to a thermal bath have been developed in recent years. This is either done using the path integral technique as in the original proposal by Tanimura and Kubo [J. Phys. Soc. Jpn. 58, 101 (1998)] or by the use of stochastic fields as done by Yan et al. [Chem. Phys. Lett. 395, 216 (2004)]. Based on the latter ansatz a compact derivation of the hierarchy using a decomposition of the spectral density function is given in the present contribution. The method is applied to calculate the time evolution of the reduced density matrix describing the motion in a harmonic, an anharmonic, and two coupled oscillators where each system is coupled to a thermal bath. Calculations to several orders in the system-bath coupling with two different truncations of the hierarchy are performed. The respective density matrices are used to calculate the time evolution of various system properties and the results are compared and discussed with a special focus on the convergence with respect to the truncation scheme applied.
We present a method to exponentiate nonsparse indefinite low-rank matrices on a quantum computer. Given access to the elements of the matrix, our method allows one to determine the singular values and their associated singular vectors in time exponentially faster in the dimension of the matrix than known classical algorithms. The method extends to non-Hermitian and nonsquare matrices via matrix embedding. Moreover, our method preserves the phase relations between the singular spaces allowing for efficient algorithms that require operating on the entire singular-value decomposition of a matrix. As an example of such an algorithm, we discuss the Procrustes problem of finding a closest isometry to a given matrix.