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Optics Letters

First passage time of laser-driven tunneling

Aleksei M. Zheltikov

Published Aug 2, 2023• 2 citations
Publisher

Abstract

The notion of the first passage time is shown to offer a meaningful extension to quantum tunneling, providing a closed-integral-form analytical unification of the tunneling rate and the tunneling passage time. We demonstrate that, in suitable potential settings, the quantum first passage time, found as a solution to the Fokker-Planck and backward Kolmogorov's equations for the quantum probability density, recovers the hallmark results for the Kramers escape rate, the lifetime of tunneling quasi-stationary wave packets, leads to a classical, distance-over-speed passage time for a free-particle wave function, and offers useful insights into Keldysh's intimation on the electron barrier-traversal time in field-induced ionization.

DOI
10.1364/ol.497818

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The notion of the first passage time is shown to offer a meaningful extension to quantum tunneling, providing a closed-integral-form analytical unification of the tunneling rate and the tunneling passage time. We demonstrate that, in suitable potential settings, the quantum first passage time, found as a solution to the Fokker-Planck and backward Kolmogorov's equations for the quantum probability density, recovers the hallmark results for the Kramers escape rate, the lifetime of tunneling quasi-stationary wave packets, leads to a classical, distance-over-speed passage time for a free-particle wave function, and offers useful insights into Keldysh's intimation on the electron barrier-traversal time in field-induced ionization.
Rapidly progressing laser technologies provide powerful tools to study potential barrier-passage dynamics in physical, chemical, and biological systems with unprecedented temporal and spatial resolution and a remarkable chemical and structural specificity. The available theories of barrier passage, however, operate with equations, potentials, and parameters that are best suited for a specific area of research and a specific class of systems and processes. Making connections among these theories is often anything but easy. Here, we address this problem by presenting a unified framework for the description of a vast variety of classical and quantum barrier-passage phenomena, revealing an innate connection between various types of barrier-passage dynamics and providing closed-form equations showing how the signature exponentials in classical and quantum barrier-passage rates relate to and translate into each other. In this framework, the Arrhenius-law kinetics, the emergence of the Gibbs distribution, Hund's molecular wave-packet well-to-well oscillatory dynamics, Keldysh photoionization, and Kramers' escape over a potential barrier are all understood as manifestations of a potential-driven Markovian dynamics whereby a system evolves from a state of local stability. Key to the irreducibility of quantum tunneling to thermally activated barrier passage is the difference in the ways the diffusion-driving potentials emerge in these two tunneling settings, giving rise to stationary states with a distinctly different structure.
Motivated by recent time-domain experiments on ultrafast atom ionization, we analyze the transients and time scales that characterize, aside from the relatively long lifetime, the decay of a localized state by tunneling. While the tunneling starts immediately, some time is required for the outgoing flux to develop. This short-term behavior depends strongly on the initial state. For the initial state, tightly localized so that the initial transients are dominated by over-the-barrier motion, the time scale for flux propagation through the barrier is close to the B\"uttiker-Landauer traversal time. Then a quasistationary, slow-decay process follows, which sets ideal conditions for observing diffraction in time at longer times and distances. To define operationally a tunneling time at the barrier edge, we extrapolate backward the propagation of the wave packet that escaped from the potential. This extrapolated time is considerably longer than the time scale of the flux and density buildup at the barrier edge.
The time a quantum particle spends traversing a classically forbidden region has resisted un-ambiguous definition since the earliest analyses of wave-packet tunneling, and the proliferation ofmutually incompatible “clocks”—the Wigner phase time, the Büttiker–Landauer traversal time, theLarmor time, and the path-integral complex time among them—has kept the question open fordecades. The controversy has been sharpened, not settled, by the advent of attosecond angular-streaking metrology, in which competing analyses of tunnel ionization continue to disagree over theexistence of a finite delay. Here we show that these rival definitions are not alternative answersto a single question but distinct cumulants of one traversal-time quasi-distribution, generated bythe exact rectangular-barrier transmission amplitude when the latter is promoted to a cumulantgenerating functional through a barrier-height counting field. The first cumulant unifies the Wignerphase time and the Larmor/Büttiker–Landauer time as the real and imaginary parts of a singlecomplex traversal time, recovering the celebrated Hartman saturation as the width-independentvalue ℏ/V0 of its real part. The second cumulant—which, to our knowledge, has not previouslybeen enlisted as a tunneling-time observable—yields a traversal-time variance that entirely evadesthe Hartman saturation and instead grows linearly with the barrier width d. The standard devia-tion of the tunneling time therefore scales as στ ∝ √d: rather than becoming superluminally sharpfor thick barriers, the tunneling time grows progressively more uncertain, in direct opposition tothe naive superluminal reading of the Hartman effect. This parameter-free scaling, independentof the O(1) coefficient that fixes its magnitude, constitutes a falsifiable prediction: attosecond an-gular streaking, which resolves the full arrival-time distribution of tunneled electrons rather thanmerely its centroid, should register a temporal spread broadening as √d even where the mean delaysaturates. We thereby recast a nearly century-old semantic dispute as a concrete experimentalquestion.
The wave-packet simulation (WPS) method for calculating the time a tunneling particle spends inside a one-dimensional potential barrier is reexamined using the Feynman path-integral technique. Following earlier work by Sokolovski and Baskin [Phys. Rev. A 36, 4604 (1987)], the tunneling (or traversal) time tpackT{\mathit{t}}_{\mathrm{pack}}^{\mathit{T}}tpackT​ is defined as a matrix element of a classical nonlocal functional between two states that represent the initial and transmitted wave packets. These states do not lie on the same orbit in Hilbert space; as a result, tpackT{\mathit{t}}_{\mathrm{pack}}^{\mathit{T}}tpackT​ is complex-valued. It is shown that RetpackT{\mathit{t}}_{\mathrm{pack}}^{\mathit{T}}tpackT​ reduces to the standard WPS result, tphaseT{\mathit{t}}_{\mathrm{phase}}^{\mathit{T}}tphaseT​, for conditions similar to those employed in the conventional WPS analysis. Similarly, ImtpackT{\mathit{t}}_{\mathrm{pack}}^{\mathit{T}}tpackT​ is shown to contain information about the energy dependence of the transmission probability. Under semiclassical conditions, ImtpackT{\mathit{t}}_{\mathrm{pack}}^{\mathit{T}}tpackT​ reduces to the well-known Wentzel-Kramers-Brillouin expression for the tunneling time. It is shown there are different definitions for the traversal time of a classical moving object, whose size is comparable to the width of the region of interest. In the quantum case, these different definitions correspond to different ways of analyzing the WPS experiment. The path-integral approach demonstrates that the tunneling-time problem is one of understanding the physical significance of complex-valued off-orbit matrix elements of an operator or functional. The physical content of complex-valued tunneling times is discussed. It is emphasized that the use of complex tunneling times includes real-time approaches as a special case. Nevertheless, there is a limitation in the description of tunneling experiments using tunneling times, whether real or complex. The path-integral approach does not supply a universal traversal time, analogous to a classical time, that can be used in quantum situations. It is demonstrated that the often expressed hope of finding a well-defined and universal real tunneling time is erroneous.
The precise definition and physical interpretation of a tunneling time is a fundamental problem in quantum mechanics. The lack of a well-defined time operator in quantum theory precludes the calculation of time in terms of an expectation value. Consequently, model calculations and simulation studies have been proposed and used to determine the time for a particle to traverse a quantum-mechanical barrier. The results offer both qualitatively and quantitatively, disparate predictions. One of the more commonly used approaches is the phase method, which we have applied to several one-dimensional model potentials to show that the tunneling time is characterized by the ratio of the typical decay length in the barrier to the incident velocity, τ∼(1/κ)/v0. We also show that the phase and the spin precession methods are equivalent when the magnetic field is applied throughout the space containing the particle wave function and the tunneling barrier. In principle, the spin precession method can be regarded as an operational definition of the tunneling time. It also has been shown that a tunneling time can be defined operationally for a time-dependent barrier, for which the model calculations predict a tunneling time given by the mean barrier width divided by the magnitude of the imaginary velocity of the particle in the barrier, τ∼d/‖v‖. This pseudokinematic result has been inferred by magnetic field dependent tunneling through heterostructures and computer simulation of wave packet tunneling through one-dimensional square barriers. Other tunneling time theories predict one or the other of the above mentioned characteristic times; several theories predict both. We interpret these different results for τ to mean that a tunneling time is not uniquely defined as a function of particle energy and the barrier shape unless the process in which the tunneling is involved is also specified. That is, the tunneling time is a meaningful and unique concept only for particular tunneling processes or definite operational procedures.