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arXiv:2405.02031 · The Journal of Physical Chemistry Letters

Vibrational Entanglement through the Lens of Quantum Information Measures

Nina Glaser, Alberto Baiardi, Annina Z. Lieberherr, Markus Reiher

Published Jun 28, 2024• 6 citations
arXivHTMLPDF

Abstract

High Resolution Image Download MS PowerPoint Slide We introduce a quantum information analysis of vibrational wave functions to understand complex vibrational spectra of molecules with strong anharmonic couplings and vibrational resonances. For this purpose, we define one- and two-modal entropies to guide the identification of strongly coupled vibrational modes and to characterize correlations within modal basis sets. We evaluate these descriptors for multiconfigurational vibrational wave functions which we calculate with the n -mode vibrational density matrix renormalization group algorithm. Based on the quantum information measures, we present a vibrational entanglement analysis of the vibrational ground and excited states of CO 2, which display strong anharmonic effects due to the symmetry-induced and accidental (near-) degeneracies. We investigate the entanglement signature of the Fermi resonance and discuss the maximally entangled state arising from the two degenerate bending modes.

DOI
10.1021/acs.jpclett.4c01298

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High Resolution Image Download MS PowerPoint Slide We introduce a quantum information analysis of vibrational wave functions to understand complex vibrational spectra of molecules with strong anharmonic couplings and vibrational resonances. For this purpose, we define one- and two-modal entropies to guide the identification of strongly coupled vibrational modes and to characterize correlations within modal basis sets. We evaluate these descriptors for multiconfigurational vibrational wave functions which we calculate with the n -mode vibrational density matrix renormalization group algorithm. Based on the quantum information measures, we present a vibrational entanglement analysis of the vibrational ground and excited states of CO 2, which display strong anharmonic effects due to the symmetry-induced and accidental (near-) degeneracies. We investigate the entanglement signature of the Fermi resonance and discuss the maximally entangled state arising from the two degenerate bending modes.
The dynamics of quantum entanglement described by the von Neumann entropy is studied for the localized states of Fermi-resonance coupling vibrations in molecule CS2, where the interacting energy between the stretching and the bending modes is considered to establish a connection between entanglement and energy. It is shown that entanglement reveals dominant anti-correlation with the interacting energy for the stretch-localized state, while that exhibits dominantly positive correlation for the bend-localized state. The entanglement and the energy for the dislocalized states are discussed as well. Those are useful for molecular quantum computing and quantum information in high dimensional states.
The dynamics of quantum entropy, energy, and entanglement is studied for various initial states in an important spectroscopic Hamiltonian of bent triatomic molecules H2O, D2O, and H2S. The total quantum correlation is quantified in terms of the mutual information and the entanglement by the concurrence borrowed from the theory of quantum information. The Pauli entropy and the intramolecular energy usually used in the theory of molecules are calculated to establish a possible relationship between both theories. Sections of two quantities among these four quantities are introduced to visualize such relationship. Analytic and numerical simulations demonstrate that if an initial state is taken to be the stretch- or the bend-vibrationally localized state, the mutual information, the Pauli entropy, and the concurrence are dominant-positively correlated while they are dominantly anti-correlated with the interacting energy among three anharmonic vibrational modes. In particular, such correlation is more distinct for the localized state with high excitations in the bending mode. The nice quasi-periodicity of those quantities in D2O molecule reveals that this molecule prepared in the localized state in the stretching or the bending mode can be more appreciated for molecular quantum computation. However, the dynamical correlations of those quantities behave irregularly for the dislocalized states. Moreover, the hierarchy of the mutual information and the Pauli entropy is explicitly proved. Quantum entropy and energy in every vibrational mode are investigated. Thereby, the relation between bipartite and tripartite entanglements is discussed as well. Those are useful for the understanding of quantum correlations in high-dimensional states in polyatomic molecules from quantum information and intramolecular dynamics.
The dynamics of tripartite entanglement and intramolecular energy for one harmonic- and two anharmonic-vibrational modes in a symmetric trimer molecule is studied for various initial states, where the entanglement is quantified in terms of concurrence and the interacting energy among three modes is calculated to establish a link between entanglement and energy. It is shown that the concurrence and the interacting energy behave dominantly positive correlation for the localized state in the anharmonic-vibrational mode, while they are dominantly anti-correlated for the localized state in the harmonic-vibrational mode. The relation between bipartite entanglement and the energy in a subsystem is discussed as well. Those are useful for quantum computing and quantum information in high dimensional states prepared in polyatomic molecules.
Harmonic chains are used as a model in quantum information theory for ion traps and simple solid state systems. Entanglement is a quantum effect in which observations made on one object instantaneously affect measurement outcomes on the other. This study investigates interparticle entanglement in finite chains of coupled harmonic oscillators as a function of the vibrational modes, mode excitations, and bipartition of oscillators. The methods used and results extend previous work for the Gaussian ground state to excited states. Entanglement is analyzed by calculating the purity of the reduced density matrix of the combined wavefunctions of the oscillators in the chain, tracing over subensembles. Analytic and numerical results for a varying effective spring constants between the particles and number of particles in the chain are presented. Interesting correlations between the symmetries of the vibrational modes and their excitations, and the symmetries of the partitions were discovered. Results show that higher excitation numbers result in higher entanglement. Adding energy to the modes will never decrease entanglement, however, the relationship between energy and entanglement is not simple. Different combinations of mode energy excitations will produce the same entanglement, even if the total energy of the system differs. Patterns indicate that the combination of symmetry in mode shapes and partition determines excitation number purity equivalence classes.
The entanglement dynamics of Fermi resonance coupling vibrations in a spectroscopic Hamiltonian for molecules CHD3\mathrm{C}\mathrm{H}{\mathrm{D}}_{3}CHD3​, CHCl3\mathrm{C}\mathrm{H}{\mathrm{Cl}}_{3}CHCl3​, and CHF3\mathrm{C}\mathrm{H}{\mathrm{F}}_{3}CHF3​ is studied in terms of the von Neumann entropy and negativity with three kinds of initial states that are direct products of coherent states, thermal states, and squeezed states of each mode. It is demonstrated that the increasing rate of entanglement in the early-time evolution is the largest for the squeezed states, while that is the smallest for the coherent states. For small parameters in the coherent and thermal states, entanglement displays a quasiperiodicity with the quasiperiod in CHF3\mathrm{C}\mathrm{H}{\mathrm{F}}_{3}CHF3​ being the longest. Furthermore, the dynamical correlation between the von Neumann entropy and negativity shows that positively correlated or anticorrelated behaviors of both measures strongly depend on initial states and molecules. For those states with small parameters, both measures exhibit dominantly positive correlation. These are useful for molecular quantum computing and information processing.
We consider the quantum entanglement of the electronic and vibrational degrees of freedom in molecules with tendencies towards double welled potentials. In these bipartite systems, the von Neumann entropy of the reduced density matrix is used to quantify the electron-vibration entanglement for the lowest two vibronic wavefunctions obtained from a model Hamiltonian based on coupled harmonic diabatic potential-energy surfaces. Significant entanglement is found only in the region in which the ground vibronic state contains a density profile that is bimodal (i.e., contains two separate local maxima). However, in this region two distinct types of density and entanglement profiles are found: one type arises purely from the degeneracy of energy levels in the two potential wells and is destroyed by slight asymmetry, while the other arises through strong interactions between the diabatic levels of each well and is relatively insensitive to asymmetry. These two distinct types are termed fragile degeneracy-induced entanglement and persistent entanglement, respectively. Six classic molecular systems describable by two diabatic states are considered: ammonia, benzene, BNB, pyridine excited triplet states, the Creutz-Taube ion, and the radical cation of the "special pair" of chlorophylls involved in photosynthesis. These chemically diverse systems are all treated using the same general formalism and the nature of the entanglement that they embody is elucidated.