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arXiv:1703.04005 · The Journal of Physical Chemistry Letters

Quantum Nonadiabatic Cloning of Entangled Coherent States

Artur F. Izmaylov, Loïc Joubert-Doriol

Published Apr 5, 2017• 10 citations
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Abstract

We propose a systematic approach to the basis set extension for nonadiabatic dynamics of entangled combination of nuclear coherent states (CSs) evolving according to the time-dependent variational principle (TDVP). The TDVP provides a rigorous framework for fully quantum nonadiabatic dynamics of closed systems; however, the quality of results strongly depends on available basis functions. Starting with a single nuclear CS replicated vertically on all electronic states, our approach clones this function when replicas of the CS on different electronic states experience increasingly different forces. Created clones move away from each other (decohere), extending the basis set. To determine a moment for cloning, we introduce generalized forces based on derivatives that maximally contribute to a variation of the total quantum action and thus account for entanglement of all basis functions.

DOI
10.1021/acs.jpclett.7b00596

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We propose a systematic approach to the basis set extension for nonadiabatic dynamics of entangled combination of nuclear coherent states (CSs) evolving according to the time-dependent variational principle (TDVP). The TDVP provides a rigorous framework for fully quantum nonadiabatic dynamics of closed systems; however, the quality of results strongly depends on available basis functions. Starting with a single nuclear CS replicated vertically on all electronic states, our approach clones this function when replicas of the CS on different electronic states experience increasingly different forces. Created clones move away from each other (decohere), extending the basis set. To determine a moment for cloning, we introduce generalized forces based on derivatives that maximally contribute to a variation of the total quantum action and thus account for entanglement of all basis functions.
Coupled quantum electron-nuclear dynamics is often associated with the Born-Huang expansion of the molecular wave function and the appearance of nonadiabatic effects as a perturbation. On the other hand, native multicomponent representations of electrons and nuclei also exist, which do not rely on any a priori approximation. However, their implementation is hampered by prohibitive scaling. Consequently, quantum computers offer a unique opportunity for extending their use to larger systems. Here, we propose a quantum algorithm for simulating the time-evolution of molecular systems and apply it to proton transfer dynamics in malonaldehyde, described as a rigid scaffold. The proposed quantum algorithm can be easily generalized to include the explicit dynamics of the classically described molecular scaffold. We show how entanglement between electronic and nuclear degrees of freedom can persist over long times if electrons do not follow the nuclear displacement adiabatically. The proposed quantum algorithm may become a valid candidate for the study of such phenomena when sufficiently powerful quantum computers become available.
We present a novel quantum-classical approach to nonadiabatic dynamics, deduced from the coupled electronic and nuclear equations in the framework of the exact factorization of the electron-nuclear wave function. The method is based on the quasiclassical interpretation of the nuclear wave function, whose phase is related to the classical momentum and whose density is represented in terms of classical trajectories. In this approximation, electronic decoherence is naturally induced as an effect of the coupling to the nuclei and correctly reproduces the expected quantum behavior. Moreover, the splitting of the nuclear wave packet is captured as a consequence of the correct approximation of the time-dependent potential of the theory. This new approach offers a clear improvement over Ehrenfest-like dynamics. The theoretical derivation presented in this Letter is supported by numerical results that are compared to quantum mechanical calculations.
In this work, we extensively study the problem of broadcasting of entanglement. In the first part of the work, we reconceptualize the idea of state dependent quantum cloning machine, and in that process we introduce different types of state dependent cloners like static and dynamic state dependent cloners. We derive the conditions under which we can make these cloners independent of the input state. In the broadcasting part, as our resource initial state, we start with general two qubit state and consider specific examples like, non maximally entangled state (NME), Werner like state (WS), and Bell diagonal state (BDS). We apply both state dependent/ state independent cloners, both locally and non-locally, in each of these cases. Incidentally, we find several instances where state dependent cloners outperform state independent cloners in broadcasting. This work gives us a holistic view on the broadcasting of entanglement in various two qubit states, when we have an almost exhaustive sets of cloning machines in our arsenal
In this paper, we present a variational treatment of the linear dependence for a non-orthogonal time-dependent basis set in solving the Schrödinger equation. The method is based on (i) the definition of a linearly independent working space and (ii) a variational construction of the propagator over finite time steps. The second point allows the method to properly account for changes in the dimensionality of the working space along the time evolution. In particular, the time evolution is represented by a semi-unitary transformation. Tests are carried out on a quartic double-well potential with Gaussian basis functions whose centers evolve according to classical equations of motion. We show that the resulting dynamics converges to the exact one and is unitary by construction.
The time-dependent variational principle of the Schr\"odinger equation is applied to a formally exact solution of the Schr\"odinger equation whose variational elements are operators which define a collective subspace of the many-body system under study. This generalizes the procedure employed to derive time-dependent Hartree-Fock theory. Four distinct formally exact time-independent variational principles, including several familiar forms, are derived. Application to a class of exactly soluble models, studied in the vibrational regime, illustrates the different modes of implementation of two of the principles. The general theory of large amplitude collective motion is derived. It is shown that the principles can be applied equally well, using either boson or fermion pair degrees of freedom. Some aspects of the relation to the semiclassical limit are discussed.[NUCLEAR STRUCTURE Time-dependent variational principle for collective motion. Invariance principle of Schr\"odinger equation. Generalized coherent state trial function. Exact time-independent variational principles. Variational principle for intrinsic state. Cranking variational principle. Large amplitude collective motion. Semiclassical limit.]
Methods of quantum nuclear wave-function dynamics have become very efficient in simulating large isolated systems using the time-dependent variational principle (TDVP). However, a straightforward extension of the TDVP to the density matrix framework gives rise to methods that do not conserve the energy in the isolated system limit and the total system population for open systems where only energy exchange with environment is allowed. These problems arise when the system density is in a mixed state and is simulated using an incomplete basis. Thus, the basis set incompleteness, which is inevitable in practical calculations, creates artificial channels for energy and population dissipation. To overcome this unphysical behavior, we have introduced a constrained Lagrangian formulation of TDVP applied to a non-stochastic open system Schrödinger equation [L. Joubert-Doriol, I. G. Ryabinkin, and A. F. Izmaylov, J. Chem. Phys. 141, 234112 (2014)]. While our formulation can be applied to any variational ansatz for the system density matrix, derivation of working equations and numerical assessment is done within the variational multiconfiguration Gaussian approach for a two-dimensional linear vibronic coupling model system interacting with a harmonic bath.