The semiclassical Herman–Kluk initial value approximation of the quantum-mechanical propagator, which is heavily used in dynamical studies of atomic and molecular systems, takes into account nonlinearity of the underlying classical dynamics by using multiple classical initial value solutions. In applications to the propagation of Gaussian wavepackets non-Gaussian distortions in the course of time and therefore a realistic description of the quantum dynamics are possible. This is in contrast to the single-trajectory approximations investigated in a recent paper by Baranger et al , one of which was erroneously termed Herman–Kluk approximation.
The semiclassical Herman–Kluk initial value approximation of the quantum-mechanical propagator, which is heavily used in dynamical studies of atomic and molecular systems, takes into account nonlinearity of the underlying classical dynamics by using multiple classical initial value solutions. In applications to the propagation of Gaussian wavepackets non-Gaussian distortions in the course of time and therefore a realistic description of the quantum dynamics are possible. This is in contrast to the single-trajectory approximations investigated in a recent paper by Baranger et al , one of which was erroneously termed Herman–Kluk approximation.
The Herman–Kluk (HK) formula was shown in (Baranger et al J. Phys. A: Math. Gen. 34 7227 ) not to be a correct semiclassical limit of an exact quantum mechanical formula. Two previous attempts to derive it using semiclassical arguments contain serious errors. These statements are left totally untouched by Herman and Grossmann's comment. They argue that the formula which we found to be at fault is not the one that should be called the HK formula. However, the formula we criticized is definitely one of the steps, in fact the main step, in these two published derivations of the HK formula. Very recently, a new derivation was published by Miller. It is interesting, but it is not semiclassical.
We formulate various semiclassical propagators for the Wigner phase space representation from a unified point of view. As is shown in several studies, the Moyal equation, which is an equation of motion for the Wigner distribution function, can be regarded as the Schrödinger equation of an extended Hamiltonian system where its "position" and "momentum" correspond to the middle point of two points of the original phase space and the difference between them, respectively. Then we show that various phase-space semiclassical propagators can be formulated just by applying existing semiclassical propagators to the extended system. As a result, a phase space version of the Van Vleck propagator, the initial-value Van Vleck propagator, the Herman-Kluk propagator, and the thawed Gaussian approximation are obtained. In addition, we numerically compare the initial-value phase-space Van Vleck propagator, the phase-space Herman-Kluk propagator, and the classical mechanical propagation as approximation methods for the time propagation of the Wigner distribution function in terms of both accuracy and convergence speed. As a result, we find that the convergence speed of the Van Vleck propagator is far slower than others as is the case of the Hilbert space, and the Herman-Kluk propagator keeps its accuracy for a long period compared with the classical mechanical propagation while the convergence speed of the latter is faster than the former.
In two recent papers (Baranger et al 2001 J. Phys. A: Math. Gen. 34 7227; 2002 J. Phys. A: Math. Gen. 35 9493) co-authored by us, we mentioned the work of Dr Kenneth G Kay (Kay 1994 J. Chem. Phys. 100(6) 4377; 100 4432) in an unfavourable light. In this comment we correct this impression, as it was based on a misunderstanding of his work. The point at issue has been the derivation of the Herman–Kluk formula (Herman and Kluk 1984 Chem. Phys. 91 27). We find Kay's derivation to be the most solid at the moment.
We present a time-dependent semiclassical method based on quantum trajectories. Quantum-mechanical effects are described via the quantum potential computed from the wave function density approximated as a linear combination of Gaussian fitting functions. The number of the fitting functions determines the accuracy of the approximate quantum potential (AQP). One Gaussian fit reproduces time-evolution of a Gaussian wave packet in a parabolic potential. The limit of the large number of fitting Gaussians and trajectories gives the full quantum-mechanical result. The method is systematically improvable from classical to fully quantum. The fitting procedure is implemented as a gradient minimization. We also compare AQP method to the widely used semiclassical propagator of Herman and Kluk by computing energy-resolved transmission probabilities for the Eckart barrier from the wave packet time-correlation functions. We find the results obtained with the Herman–Kluk propagator to be essentially equivalent to those of AQP method with a one-Gaussian density fit for several barrier widths.
We present a complete derivation of the semiclassical limit of the coherent-state propagator in one dimension, starting from path integrals in phase space. We show that the arbitrariness in the path integral representation, which follows from the overcompleteness of the coherent states, results in many different semiclassical limits. We explicitly derive two possible semiclassical formulae for the propagator, we suggest a third one, and we discuss their relationships. We also derive an initial-value representation for the semiclassical propagator, based on an initial Gaussian wavepacket. It turns out to be related to, but different from, Heller's thawed Gaussian approximation. It is very different from the Herman-Kluk formula, which is not a correct semiclassical limit. We point out errors in two derivations of the latter. Finally we show how the semiclassical coherent-state propagators lead to WKB-type quantization rules and to approximations for the Husimi distributions of stationary states.
Abstract Recent experimental progress in monitoring the dynamics of ultracold gases in optical lattices necessitates a quantitative theoretical description for a significant number of bosons. In the present paper, we investigate if time-dependent semiclassical initial value methodology, with propagators expressed as integrals over phase space and using classical trajectories, is suitable to describe interacting bosons, concentrating on a single mode. Despite the nonlinear contribution from the self-interaction, the corresponding classical dynamics allows for a largely analytical treatment of the semiclassical propagator. We find that application of the Herman–Kluk (HK) propagator conserves unitarity in the semiclassical limit, but a decay of the norm is seen for low particle numbers n . The frozen Gaussian approximation (FGA) (HK with unit prefactor) is explicitly shown to violate unitarity in the present system for non-vanishing interaction strength, even in the semiclassical limit. Furthermore, we show by evaluating the phase space integral in steepest descent approximation, that the HK propagator reproduces the exact spectrum correctly in the semiclassical limit ( ). An error is, however, incurred in next-to-next-to-leading order (small parameter ), as seen upon numerical evaluation of the integral and confirmed analytically by considering finite n corrections to the steepest descent calculations. The FGA, in contrast, is only accurate to lowest order, and an erroneous next-to-leading order term in the energy spectrum was found analytically. Finally, as an example application, we study the dynamics of wave packets by computing the time evolution of the Wigner function. While the often-used truncated Wigner approximation cannot capture any interferences present in the exact quantum mechanical solution (known analytically), we find that the HK approach, despite also using classical information only, reproduces the salient features of the exact solution correctly.