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Physical Review A

Entanglement in shape phase transitions of coupled molecular benders

Manuel Calixto, Francisco Pérez-Bernal

Published Mar 24, 2014• 14 citations
Publisher

Abstract

We study the entanglement properties of the shape phase transitions between different geometric limits of two coupled equivalent molecular benders modeled with the two-dimensional limit of the vibron model. This system has four possible geometric configurations: linear, cis-bent, trans-bent, and nonplanar. We show how the entanglement, accessed through the calculation of the linear entropy, between benders and between rotational and vibrational degrees of freedom changes sensitively in the critical regions of this two-fluid bosonic model. The numeric calculation is complemented with a variational approach to the ground-state wave function in terms of symmetry-adapted coherent states.

DOI
10.1103/physreva.89.032126

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We study the entanglement properties of the shape phase transitions between different geometric limits of two coupled equivalent molecular benders modeled with the two-dimensional limit of the vibron model. This system has four possible geometric configurations: linear, cis-bent, trans-bent, and nonplanar. We show how the entanglement, accessed through the calculation of the linear entropy, between benders and between rotational and vibrational degrees of freedom changes sensitively in the critical regions of this two-fluid bosonic model. The numeric calculation is complemented with a variational approach to the ground-state wave function in terms of symmetry-adapted coherent states.
We propose coherent (‘Schrödinger cat-like’) states adapted to the parity symmetry providing a remarkable variational description of the ground and first excited states of vibron models for finite ( N )-size molecules. Vibron models undergo a quantum shape phase transition (from linear to bent) at a critical value ξ c of a control parameter. These trial cat states reveal a sudden increase in vibration–rotation entanglement linear ( L ) and von Neumann ( S ) entropies from zero to (to be compared with L ( N ) max (ξ) = 1 − 1/( N + 1)) and , respectively, above the critical point, ξ > ξ c , in agreement with exact numerical calculations. We also compute inverse participation ratios, for which these cat states capture a sudden delocalization of the ground-state wave packet across the critical point. Analytic expressions for entanglement entropies and inverse participation ratios of variational states, as functions of N and ξ, are given in terms of hypergeometric functions.
We investigate the entanglement between electronic and vibrational degrees of freedom produced by a vibronic coupling in a molecular system described in the Born-Oppenheimer approximation. Entanglement in a pure state of the Hilbert space H=Hel⨂Hvib\mathcal{H}={\mathcal{H}}_{\mathrm{el}}⨂{\mathcal{H}}_{\mathrm{vib}}H=Hel​⨂Hvib​ is quantified using the von Neumann entropy of the reduced density matrix and the reduced linear entropy. Expressions for these entanglement measures are derived for the $2\ifmmode\times\else\texttimes\fi{}{N}_{v}$ and $3\ifmmode\times\else\texttimes\fi{}{N}_{v}$ cases of the bipartite entanglement, where 2 and 3 are the dimensions of the electronic Hilbert space H\mathcal{H}Hel{}_{\mathrm{el}}el​, and Nv{N}_{v}Nv​ is the dimension of H\mathcal{H}Hvib{}_{\mathrm{vib}}vib​. We study the entanglement dynamics for two electronic states coupled by a laser pulse (a $2\ifmmode\times\else\texttimes\fi{}{N}_{v}$ case), taking as an example a coupling between the ${a}^{3}{{\ensuremath{\Sigma}}_{u}}^{+}(6s,6s)$ and 1g(6s,6p3/2){1}_{g}(6s,6{p}_{3/2})1g​(6s,6p3/2​) states of the Cs2{}_{2}2​ molecule. The reduced linear entropy expression obtained for the $3\ifmmode\times\else\texttimes\fi{}{N}_{v}$ case is used to follow the entanglement evolution in a scheme proposed for the control of the vibronic dynamics in a Cs2{}_{2}2​ cold molecule, implying the ${a}^{3}{{\ensuremath{\Sigma}}_{u}}^{+}(6s,6s)$, ${0}_{g}{}^{\ensuremath{-}}(6s,6{p}_{3/2})$, and ${0}_{g}{}^{\ensuremath{-}}(6s,5d)$ electronic states, which are coupled by a nonadiabatic radial coupling and a sequence of chirped laser pulses.
We characterize both entanglement and quantum coherence in a molecular system by connecting the linear entropy of electronic-nuclear entanglement with Wigner-Yanase skew information measuring vibronic coherence and local quantum uncertainty on electronic energy. Linear entropy of entanglement and quantifiers of quantum coherence are derived for a molecular system described in a bipartite Hilbert space H=Hel⨂Hvib\mathcal{H}={\mathcal{H}}_{el}⨂{\mathcal{H}}_{vib}H=Hel​⨂Hvib​ of finite dimension ${N}_{el}\ifmmode\times\else\texttimes\fi{}{N}_{v}$, and relations between them are established. For the specific case of the electronic-vibrational entanglement, we find the linear entropy of entanglement as having a more complex informational content than the von Neumann entropy. By keeping the information carried by the vibronic coherences in a molecule, linear entropy seizes vibrational motion in the electronic potentials as entanglement dynamics. We analyze entanglement oscillations in an isolated molecule, and show examples for the control of entanglement dynamics in a molecule through the creation of coherent vibrational wave packets in several electronic potentials by using chirped laser pulses.
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.
The Husimi distribution is proposed for a phase-space analysis of quantum phase transitions in the two-dimensional U(3) vibron model for NNN-size molecules. We show that the inverse participation ratio and Wehrl's entropy of the Husimi distribution give sharp signatures of the quantum (shape) phase transition from linear to bent. Numerical results are complemented with a variational approach using parity-symmetry-adapted U(3) coherent states, which reach the minimum Wehrl entropy N(3+2N)(N+1)(N+2)\frac{N(3+2N)}{(N+1)(N+2)}(N+1)(N+2)N(3+2N)​, in the rigidly linear phase, according to a generalized Wehrl-Lieb conjecture. We also propose a characterization of the vibron-model quantum phase transition by means of the zeros of the Husimi distribution.
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.