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Semiclassical propagators for quantum coherent states and applications of extra quantum phase to large-spin tunneling of magnetic molecules

Kee-Su Park

Published Jan 1, 2001• 0 citations

Abstract

A continuous path integral is used to obtain the semiclassical expressions of quantum propagators by means of coherent states in the holomorphic representation together with the appropriate boundary conditions. It allows us to express the total actions including boundary terms, classical trajectories, and extra phases in the stationary phase approximation. In particular, in the semiclassical expression for the quantum spin propagator, we pay attention to the extra quantum phase discovered by Solari and Kochetov. It is shown that this extra phase is related to an anomaly in the fluctuation determinant. It is verified that once this extra phase is included, the semiclassical propagator leads to the correct short time behaviour to O(T²), and shows its consistency under dissection of the path. In the application to the instanton methods, the extra quantum phase yields the correct formula for the tunnel splitting including both the exponential factor and the prefactor. The quantum phase leads to the correct spectrum with a shift of the spin quantum number by 1/2. We apply the semiclassical propagators and the tunnel splitting to a few models in magnetic molecular systems. It is shown that the formula gives the correct exponential factor and prefactors for quantum tunneling of a large spin if the extra quantum phase is taken into account.

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A continuous path integral is used to obtain the semiclassical expressions of quantum propagators by means of coherent states in the holomorphic representation together with the appropriate boundary conditions. It allows us to express the total actions including boundary terms, classical trajectories, and extra phases in the stationary phase approximation. In particular, in the semiclassical expression for the quantum spin propagator, we pay attention to the extra quantum phase discovered by Solari and Kochetov. It is shown that this extra phase is related to an anomaly in the fluctuation determinant. It is verified that once this extra phase is included, the semiclassical propagator leads to the correct short time behaviour to O(T²), and shows its consistency under dissection of the path. In the application to the instanton methods, the extra quantum phase yields the correct formula for the tunnel splitting including both the exponential factor and the prefactor. The quantum phase leads to the correct spectrum with a shift of the spin quantum number by 1/2. We apply the semiclassical propagators and the tunnel splitting to a few models in magnetic molecular systems. It is shown that the formula gives the correct exponential factor and prefactors for quantum tunneling of a large spin if the extra quantum phase is taken into account.

The problem of an origin of the Solary-Kochetov extra-phase contribution to the naive semiclassical form of a generalized phase-space propagator is addressed with the special reference to the su(2) spin case which is the most important in applications. While the extra-phase correction to a flat phase-space propagator can straightforwardly be shown to appear as a difference between the principal and the Weyl symbols of a Hamiltonian in the next-to-leading order expansion in the semiclassical parameter, the same statement for the semiclassical spin coherent-state propagator holds provided the Holstein-Primakoff representation of the su(2) algebra generators is employed.

A central challenge to the semiclassical description of quantum mechanics is the quantum phenomenon of "deep" tunneling. Here we show that real time classical trajectories suffice to account correctly even for deep quantum tunneling, using a recently formulated semiclassical initial value representation series of the quantum propagator and a prefactor free semiclassical propagator. Deep quantum tunneling is effected through what we term as coherent classical paths which are composed of one or more classical trajectories that lead from reactant to product but are discontinuous along the way. The end and initial phase space points of consecutive classical trajectories contributing to the coherent path are close to each other in the sense that the distance between them is weighted by a coherent state overlap matrix element. Results are presented for thermal and energy dependent tunneling through a symmetric Eckart barrier.

The spin coherent state path integral describing the dynamics of a spin-½ system in a magnetic field of arbitrary time dependence is considered. Defining the path integral as the limit of a Wiener regularized expression, the semiclassical approximation leads to a continuous minimal action path with jumps at the endpoints. The resulting semiclassical propagator is shown to coincide with the exact quantum mechanical propagator. A nonlinear transformation of the angle variables allows for a determination of the semiclassical path and the jumps without solving a boundary-value problem. The semiclassical spin dynamics is thus readily amenable to numerical methods.