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Journal of Applied Science and Engineering

Theoretical Treatments of Quantum Beats

Michitoshi Hayashi, Ruey‐Feng Chang, Kuo Kan Liang, Chih‐Yung Chang, Y. J. Shiu, Jun Chang, Fang‐Chi Hsu, A. M. Mebel', S. H. Lin

Published Sep 1, 2000• 0 citations
Publisher

Abstract

Basic theoretical treatments of quantum beats are presented using the effective Hamiltonian method and the density matrix method. To describe the states involved in quantum beats, the molecular-eigen state basis set and the zeroth order basis set are introduced. Based on these basis sets for the two-state model, the condition under which molecular coherence can be created is discussed.

DOI
10.6180/jase.2000.3.3.04

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Basic theoretical treatments of quantum beats are presented using the effective Hamiltonian method and the density matrix method. To describe the states involved in quantum beats, the molecular-eigen state basis set and the zeroth order basis set are introduced. Based on these basis sets for the two-state model, the condition under which molecular coherence can be created is discussed.
Detecting quantum coherence Observing quantum coherence is a tricky business. Even before we fire up the femtosecond laser systems and start our search, we need to ask ourselves some basic questions: What is coherence? How does coherence manifest in measurements? What methods can we use to detect and measure coherence? Only then, can we begin to interpret data to search for coherence and to try to make sense of the observed signals. In this section, I will discuss detecting quantum coherence both in theory and in practice. The goal of this section is to present a unified view of experimental approaches in broad strokes and to provide useful references to guide further exploration. What is ‘quantum coherence’? Firstly, the precise meaning of ‘quantum coherence’ must be pinned down. I define quantum coherences to be off-diagonal elements of the density matrix representing the ensemble. (I am explicitly setting aside questions of ‘quantum’ versus ‘classical’ coherences; let us simply assume that the system in question is best described quantum mechanically and presume that the coherences in such a system are also quantum in nature. The simple fact is that we don't yet have the tools to answer this debate definitively.) This definition, however, is still insufficient. The density matrix and the magnitudes of its off-diagonal elements in particular depend on the basis set used to write down the matrix. For the purposes of this chapter, I will consider the density matrix only in the Hamiltonian eigenbasis.
It is shown that the standard reduction procedure (i.e., the calculation of the density matrix of the observable subsystem from the density matrix of a closed quantum system) bringing about decoherence corresponds to the limiting approximation, where the unobservable subsystem is assumed to be in the stationary state with minimum information (infinite temperature). An approximate set of interrelation (correlation) equations for the density matrices of the subsystems is derived. It is shown that the correlation of atom and field can be manifested as the inversion beats of a two-level atom in the known experimental scheme of resonator QED. Experimental observation of such beats would indicate that the observable subsystem (atom) generally conserves information about quantum coherence of the unobservable subsystem (field).
Quantum beats are analyzed by means of a boson-type second-quantization method which exhibits the collective behavior of nnn-level systems and displays both quantum mechanical and classical (or semiclassical) results. Theoretical criteria for predicting the existence of beats are found which differ from those in the recent literature and indicate a reevaluation of suggested experiments.
An expression for the probability of time-resolved three-photon ionization via coherently excited resonant states of a molecular system is derived in the perturbative density matrix formalism with the aid of the Liouville space Feynman diagram. It is shown how the time evolution of the molecular coherence in the first resonant state can be detected as a function of the delay time between the pumping and probing lasers through the probing two-photon ionization process. The three-photon ionization process consists of the simultaneous and sequential processes which are classified by the Liouville space Feynman diagrams. The possibility of appearance of quantum beats in the pump–probe three-photon ionization is discussed by performing model calculations of the probability of ionization. The role of the direct and redistributed processes is discussed. The redistributed process is induced by intramolecular processes in the resonant state. The theoretical treatment is applied to the (1+2) three-photon ionization of pyrazine observed by Knee et al. It is demonstrated that the fast decay component (110 ps) of the pyrazine spectra originates from the intramolecular dephasing of the vibronic coherence created by the pumping pulse laser, and this component appears only when the redistributed process (the ionization process through triplet levels) is absent.
The coherence of an individual quantum state can be meaningfully discussed only when referring to a preferred basis. This arbitrariness can, however, be lifted when considering sets of quantum states. Here we introduce the concept of set coherence for characterizing the coherence of a set of quantum systems in a basis-independent way. We construct measures for quantifying set coherence of sets of quantum states as well as quantum measurements. These measures feature an operational meaning in terms of discrimination games and capture precisely the advantage offered by a given set over incoherent ones. Along the way, we also connect the notion of set coherence to various resource-theoretic approaches recently developed for quantum systems.