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arXiv:1504.00261 · Physical Review Letters

Phase Reconstruction of Strong-Field Excited Systems by Transient-Absorption Spectroscopy

Zuoye Liu, Stefano M. Cavaletto, Christian Ott, Kristina Meyer, Yonghao Mi, Z. Harman, Christoph H. Keitel, Thomas Pfeifer

Published Jul 13, 2015• 28 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevlett.115.033003

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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 transient-absorption spectrum of a VVV-type three-level system is investigated, when this is periodically excited by a train of equally spaced, $\ensuremath{\delta}$-like pump pulses as, e.g., from an optical-frequency-comb laser. We show that, even though the probe pulse is not assumed to be much shorter than the pump pulses, light-induced states appear in the absorption spectrum. The frequency- and time-delay-dependent features of the absorption spectra are investigated as a function of several laser control parameters, such as the number of pump pulses used, their pulse area, and the pulse-to-pulse phase shift. We show that the frequencies of the light-induced states and the time-delay-dependent features of the spectra contain information on the action of the intense pulses exciting the system, which can thus complement the information on light-imposed amplitude and phase changes encoded in the absorption line shapes.
Strong-field quantum-state control is investigated, taking advantage of the full---amplitude and phase---characterization of the interaction between matter and intense ultrashort pulses via transient-absorption spectroscopy. As an example, we apply the method to a nondegenerate VVV-type three-level system modeling atomic Rb, and use a sequence of intense delayed pulses, whose parameters are tailored to steer the system into a desired quantum state. We show how to experimentally enable this optimization by retrieving all quantum features of the light-matter interaction from observable spectra. This provides a full characterization of the action of strong fields on the atomic system, including the dependence upon possibly unknown pulse properties and atomic structures. Precision and robustness of the scheme are tested, in the presence of surrounding atomic levels influencing the system's dynamics.
The reconstruction of the full temporal dipole response of a strongly driven time-dependent system from a single absorption spectrum is demonstrated, only requiring that a sufficiently short pulse is employed to initialize the coherent excitation of the system. We apply this finding to the time-domain observation of Rabi cycling between doubly excited atomic states in the few-femtosecond regime. This allows us to pinpoint the breakdown of few-level quantum dynamics at the critical laser intensity near 2 TW/cm^{2} in doubly excited helium. The present approach unlocks single-shot real-time-resolved signal reconstruction across timescales down to attoseconds for nonequilibrium states of matter. In contrast to conventional pump-probe schemes, there is no need for scanning time delays in order to access real-time information. The potential future applications of this technique range from testing fundamental quantum dynamics in strong fields to measuring and controlling ultrafast chemical and biological reaction processes when applied to traditional transient-absorption spectroscopy.
Abstract Despite the wide employment of transient absorption spectroscopy in capturing fast-evolving dynamics, the experiments lack further exploration of macroscopic effects beyond the single-atom response. Here, the absorbance of Rb atoms excited and coupled by two near-infrared pulses with a variable interpulse delay is studied both experimentally and theoretically, from the limit of a dilute-gas medium into high-density cases. Our results reveal that with increasing atomic density, the absorption lines are broadened with substructures emerging therein. However, the spectral evolutions are rather distinctive for positive and negative time delays, pointing toward different mechanisms behind them. As a distinguishing characteristic of the V -type levels, delay-dependent oscillations are entwined and complicate the resulting profiles considerably. The obtained intensity- and density-controlled line shapes are well reproduced based on the density matrix theory with the inclusion of pulse propagation. We believe these observations will not only play a crucial role in studying strong-field dynamics in dense systems, but could also serve as key ingredients for optical pulse shaping.