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Journal of Optics

Time distribution of stimulated transition probabilities

Pedro Pereyra

Published May 11, 2024• 2 citations
Publisher

Abstract

Abstract In recent years, an increasing number of experimental results have been published for a wide variety of systems in which high-precision, ultra-fast, and ultra-short laser pulses techniques have been used to study time-resolved dynamical processes. In the absence of a theoretical prediction of the time distribution of the transition probabilities, the lifetimes τ are generally extracted by fitting the decay time with an exponential, bi-exponential or three-exponential function. In fitting the data, the short-time behavior is generally neglected. The purpose of this study is to show that an explicit formula for the time distribution of the transition probability can be determined rigorously using time-dependent perturbation theory. A formula that perfectly fits an important subset of the experimental results from t = 0 to t = ∞ . We show that by following a route different from the usual procedure for deriving transition amplitudes and Einstein coefficients in time-dependent perturbation theory, one ends up with a time-dependent factor, that is, a temporal distribution function of the transition probabilities, and for the Einstein coefficients. The time distribution reported here looks in the time domain similar to the Planck distribution in the frequency domain. In fact, the behavior of the time distribution, with a maximum at 2 τ ln ⁡ 2 , and with τ playing the role of temperature, resembles the behavior of the Planck frequency distribution. We present several examples to demonstrate that the theoretical formula allows for easier fitting of the experimental results reported in the literature. We also show that the time distribution explains the difference in resonance heights between the experimental and theoretical blue laser spectra.

DOI
10.1088/2040-8986/ad49b3

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Abstract In recent years, an increasing number of experimental results have been published for a wide variety of systems in which high-precision, ultra-fast, and ultra-short laser pulses techniques have been used to study time-resolved dynamical processes. In the absence of a theoretical prediction of the time distribution of the transition probabilities, the lifetimes τ are generally extracted by fitting the decay time with an exponential, bi-exponential or three-exponential function. In fitting the data, the short-time behavior is generally neglected. The purpose of this study is to show that an explicit formula for the time distribution of the transition probability can be determined rigorously using time-dependent perturbation theory. A formula that perfectly fits an important subset of the experimental results from t = 0 to t = ∞ . We show that by following a route different from the usual procedure for deriving transition amplitudes and Einstein coefficients in time-dependent perturbation theory, one ends up with a time-dependent factor, that is, a temporal distribution function of the transition probabilities, and for the Einstein coefficients. The time distribution reported here looks in the time domain similar to the Planck distribution in the frequency domain. In fact, the behavior of the time distribution, with a maximum at 2 τ ln ⁡ 2 , and with τ playing the role of temperature, resembles the behavior of the Planck frequency distribution. We present several examples to demonstrate that the theoretical formula allows for easier fitting of the experimental results reported in the literature. We also show that the time distribution explains the difference in resonance heights between the experimental and theoretical blue laser spectra.
We investigated theoretically the time dependence of ultra-short laser pulse scattering by an atom at the high-frequency limit for the spectral and total probability of the process using new expression which we derived in this paper. We established that the time dependence of spectral scattering is presented by the curve with the maximum for sufficiently large detuning of scattering frequency from the carrier frequency of the pulse, while the total scattering probability is always the monotonically increasing function of time. We also studied the dependence of scattering probability on pulse duration at the long-time limit. It was shown that, at the long-pulse limit, the scattering probability is a linear function of pulse duration, while in the opposite case, it is a function with maximum. The position of this maximum is determined by the detuning of the scattering frequency from the carrier frequency of the pulse.
An exact single-level resonance formula for the survival probability S ( t ) in the full time interval, that depends only on the resonance energy r and the decay width Γ r and fulfils time-reversal invariance, is used to discuss the non-exponential contributions to decay. At short times the formula behaves as S ( t )≈1- ct 1/2 with c a constant, whereas at long times it behaves as S ( t )≈ dt -3 , d being a constant. With the time expressed in lifetime units, the onset of non-exponential decay is given at short times by τ S ≈4/[π( R 2 + R + 1/4)] and at long times by τ L ≈5.41 ln ( R ) + 12.25, where R = r /Γ r . The predictions of the formula are compared with numerical examples and some experimental results searching for non-exponential contributions to decay.
A detailed analysis of the quantum decay processes shows the survival probability ( t ) can not take that exponential form at any time interval including times smaller than the lifetime τ . We show that for times t ∼ τ and for the times later than τ the form of ( t ) looks as a composition of an oscillating and exponential functions. The amplitude of these oscillations is very small for t ≪ τ and grows with increasing time and depends on the model considered. We also study the survival probability of moving relativistic unstable particles with definite momentum : It turns out that late time deviations of the survival probability of these particles from the exponential-like form of the decay law should occur much earlier than it follows from the classical standard approach resolving itself into replacing time t by t / γ (where γ is the relativistic Lorentz factor) in the formula for the survival probability ( t ).
For a perturbed quantum system initially in the ground state, the coefficient ck(t) of excited state k in the time-dependent wave function separates into adiabatic and nonadiabatic terms. The adiabatic term ak(t) accounts for the adjustment of the original ground state to form the new ground state of the instantaneous Hamiltonian H(t), by incorporating excited states of the unperturbed Hamiltonian H0 without transitions; ak(t) follows the adiabatic theorem of Born and Fock. The nonadiabatic term bk(t) describes excitation into another quantum state k; bk(t) is obtained as an integral containing the time derivative of the perturbation. The true transition probability is given by bk(t)2, as first stated by Landau and Lifshitz. In this work, we contrast bk(t)2 and ck(t)2. The latter is the norm-square of the entire excited-state coefficient which is used for the transition probability within Fermi’s golden rule. Calculations are performed for a perturbing pulse consisting of a cosine or sine wave in a Gaussian envelope. When the transition frequency ωk0 is on resonance with the frequency ω of the cosine wave, bk(t)2 and ck(t)2 rise almost monotonically to the same final value; the two are intertwined, but they are out of phase with each other. Off resonance (when ωk0 ≠ ω), bk(t)2 and ck(t)2 differ significantly during the pulse. They oscillate out of phase and reach different maxima but then fall off to equal final values after the pulse has ended, when ak(t) ≡ 0. If ωk0 < ω, bk(t)2 generally exceeds ck(t)2, while the opposite is true when ωk0 > ω. While the transition probability is rising, the midpoints between successive maxima and minima fit Gaussian functions of the form a exp[−b(t − d)2]. To our knowledge, this is the first analysis of nonadiabatic transition probabilities during a perturbing pulse.
We develop a time-dependent perturbation theory (PT) beyond the dipole approximation to analyze the two-photon ionization dynamics of atoms exposed to short laser pulses with an arbitrary polarization. In a wide range of laser parameters, the good performance of the PT method is validated by comparing the results of a number of physical quantities with those calculated by numerically solving the time-dependent Schr\"odinger equation beyond the dipole approximation. Subsequent applications of the PT method in the nonresonant regime allow us to unveil the important role of the interferences between the dipole and nondipole transition pathways to the photoelectron momentum shift along the laser-propagation direction. In particular, we find that the ratio of the probability of each dipole transition channel to the total ionization probability oscillates with the increase of the photon energy. The interferences among different pathways and the oscillatory behavior of the ratios jointly lead to a series of minima in the linear momentum transfer for the case of the linear polarization.
A critical examination of the theory of resonance radiation has been carried through, employing the mathematical technique of Laplace and Stieltjes transforms. Particular attention has been devoted to the question of the temporal behavior of the excited state. With no restrictions on the interaction between atom and radiation field other than that it be real, and that processes of sufficiently high frequency contribute only negligible effects, one can prove that the probability amplitude of the excited state cannot decay according to the general law ${\ensuremath{\Sigma}}_{\ensuremath{\mu},\ensuremath{\nu}}{C}_{\ensuremath{\mu}\ensuremath{\nu}}{t}^{{\ensuremath{\lambda}}_{\ensuremath{\mu}}}{e}^{\ensuremath{-}{\ensuremath{\beta}}_{\ensuremath{\nu}}t},$ where the ${\ensuremath{\lambda}}_{\ensuremath{\mu}}$ and ${\ensuremath{\beta}}_{\ensuremath{\nu}}$ are complex constants lying in the right half-plane and the ${C}_{\ensuremath{\mu}\ensuremath{\nu}}$ are arbitrary complex coefficients. The deviation from the law just cited can be termed a straggling phenomenon since exact analysis shows that the probability amplitude, for sufficiently long times, is greater than that defined according to the radioactive decay law.Rigorous analysis of the source of this apparently anomalous behavior reveals the following explanation. Although the probability amplitude of the excited state is, strictly speaking, a functional of the interaction between the transition current in the atom and the photon states of the electromagnetic field, the essential features are determined principally by those states lying near the resonance frequency. Three elementary observations are immediately apparent. First, a particularly tractable analytical approximation for the interaction can be made such that the value of the actual interaction is reproduced at the resonance frequency and such that the behavior for high and low frequency photon states is at least qualitatively correct. Exact solutions in closed form can be obtained for this interaction. Second, in terms of the preceding representation it is possible to show that, associated with the transition between two atomic states, one is presented with a concomitant picture of a damped oscillation of charge describable in purely classical terms. Third, this classical motion can be interpreted as forming a source function for a continuous stochastic process in terms of which one finally derives the representation of the probability amplitude of the excited state. The straggling phenomenon previously cited is therefore that associated with all diffusion processes. The consideration of the exact interaction leads to more involved diffusion phenomena but does not in any case permit a radioactive decay law.