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arXiv:1810.05860 · New Journal of Physics

Ultrafast dynamic evolution of multilevel systems in medium-strength laser fields

Zhenhao Wang, Guoqiang Shi, Yu He, Quanjun Wang, J. J. Ding, Shaohua Sun, Zuoye Liu, Bitao Hu

Published Mar 28, 2019• 6 citations
arXivHTMLPDF

Abstract

Abstract The ultrafast dynamic evolution of an atomic system under medium-strength laser fields is studied by performing transient absorption measurement. An analytical model developed from perturbation theory with a modified transition dipole moment is presented to explain the spectral features of the multilevel system. By fitting the measured absorption spectra to the model, the system’s dynamic evolution is quantified by different amplitude and phase modulation factors in the pump-probe and probe-pump scenarios. This study provides a way to understand laser-matter interaction in the transition area between the strong-field and weak-field regimes.

DOI
10.1088/1367-2630/ab145a

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•Jan 1, 2018•0 citations
Abstract The ultrafast dynamic evolution of an atomic system under medium-strength laser fields is studied by performing transient absorption measurement. An analytical model developed from perturbation theory with a modified transition dipole moment is presented to explain the spectral features of the multilevel system. By fitting the measured absorption spectra to the model, the system’s dynamic evolution is quantified by different amplitude and phase modulation factors in the pump-probe and probe-pump scenarios. This study provides a way to understand laser-matter interaction in the transition area between the strong-field and weak-field regimes.
The evolution of a V-type three-level system is studied, whose two resonances are coherently excited and coupled by two ultrashort laser pump and probe pulses, separated by a varying time delay. We relate the quantum dynamics of the excited multilevel system to the absorption spectrum of the transmitted probe pulse. In particular, by analyzing the quantum evolution of the system, we interpret how atomic phases are differently encoded in the time-delay-dependent spectral absorption profiles when the pump pulse either precedes or follows the probe pulse. This scheme is experimentally applied to atomic Rb, whose fine-structure-split 5s (2)S{1/2}→5p(2)P{1/2} and 5s(2)S_{1/2}→5p(2)P{3/2} transitions are driven by the combined action of a pump pulse of variable intensity and a delayed probe pulse. The provided understanding of the relationship between quantum phases and absorption spectra represents an important step towards full time-dependent phase reconstruction (quantum holography) of bound-state wave packets in strong-field light-matter interactions with atoms, molecules, and solids.
Abstract The quantum dynamics of a system of Rb atoms, modeled by a V -type three-level system interacting with intense probe and pump pulses, are studied. The time-delay-dependent transient-absorption spectrum of an intense probe pulse is thus predicted, simulating pump-probe experiments in which this is preceded or followed by a strong pump pulse. Numerical results are interpreted in terms of an analytical model based on interaction operators , which quantify the transformation undergone by the system under the action of an intense pulse. The oscillating features of the resulting transient-absorption spectra, due to the coupling of several excited states, are thus interpreted in terms of the atomic population and phase changes imposed by the pump and probe pulses. Strong-field-induced phases and their influence on the resulting transient-absorption spectra are thereby investigated for different values of pump and probe intensities and frequencies, focusing on the atomic properties which are encoded in the absorption line shapes for positive and negative time delays.
The quantum dynamics of a system of Rb atoms, modeled by a V-type three-level system interacting with intense probe and pump pulses, are studied. The time-delay-dependent transient-absorption spectrum of an intense probe pulse is thus predicted, when this is preceded or followed by a strong pump pulse. Numerical results are interpreted in terms of an analytical model, which allows us to quantify the oscillating features of the resulting transient-absorption spectra in terms of the atomic populations and phases generated by the intense pulses. Strong-field-induced phases and their influence on the resulting transient-absorption spectra are thereby investigated for different values of pump and probe intensities and frequencies, focusing on the atomic properties which are encoded in the absorption line shapes for positive and negative time delays.
The coherent excitation and manipulation of a two-level system with ultrashort intense extreme-ultraviolet laser fields is investigated theoretically, based on numerically solving the time-dependent Schr\"odinger equation. We are particularly interested in the dynamical phase excursion of the energy states over the course of the interaction and the resulting spectral modifications. Fitting the absorption line shapes with the Fano profile quantifies the asymmetry parameter and the corresponding dipole phase offset, capturing the phase difference of the state coefficients after the interaction. Nonperturbative analytical calculations using rectangular driving pulses are employed, yielding physical insights into the dependence of the dipole phase shift on the external field. The validity of the formulas is validated by comparing their predictions with numerical results, which proves to be robust against the variation of laser parameters. The present investigation of strong-field dressing effects complements recent attosecond transient absorption studies assuming weak excitation, and marks a ubiquitous phenomenon that should be generally considered for the interaction of matter with intense laser fields.
Attention is focused on the dynamic evolution of the emission spectrum following abrupt excitation of a near-resonant two-level absorber by a strong laser field. The multiphoton character of the absorption-emission process is evident in the AC Stark splitting of the spectrum, which begins approximately half an atomic lifetime after excitation, if the laser field is strong enough. Analytic expressions for the spectra are given of arbitrary laser field strength, atomic lifetime, laser-atom detuning, and the bandwidth of the spectrometer used to analyse the spectrum. Selected graphs are included to illustrate various time-dependent features of the spectrum. The influence on the transient spectrum of three different states of atomic excitation prior to laser irradiation and the effect on the spectrum of irradiation by a phase-noisy laser are also considered. Comparison of the transient spectra from atoms initially prepared in ' pi /2' and '3 pi /2' states show clearly that phase relationships between the irradiating field and the emitting dipole are important even in fluorescence.
The goal of this work is to study and understand dynamics of atomic systems interacting with strong fields. To this end, a method referred to as strong-field spectroscopy is used, which measures the absorption spectrum of atoms interacting with such fields. In the scope of this work, a technique which allows the simultaneous measurement of absorption spectra of attosecond pulses and their reference signal is developed, which significantly increases the sensitivity to absorption changes. Additionally, a reconstruction method is introduced which retrieves the time-dependent evolution of the dipole response of an atomic system directly from a single absorption spectrum. Strong-field spectroscopy combines these techniques to examine the nonlinear strong-field dynamics in atomic and molecular systems and is applied to study the strongly correlated doubly excited states in helium. Furthermore, a measurement approach is introduced which uses the interaction with a high-intensity laser pulse to impose a time gate on the evolution of the coherent response of a system, which has previously been excited by an ultrashort laser pulse. With this approach the buildup of resonance phenomena in a wide range of physical systems can be studied. As a first application, the time-dependent buildup of a Fano resonance as well as the buildup of a whole Rydberg series are investigated.