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Physical Review A

Observation of short-lived laser-dressed quantum states in the frequency plane

M. Žitnik, A. Mihelič, K. Bučar, Mateja Hrast, Žiga Barba, Špela Krušič, Primož Rebernik Ribič, Jurij Urbančič, B. Ressel, Matija Stupar, Luca Poletto, Marcello Coreno, David Gauthier, Giovanni De Ninno

Published May 28, 2019• 3 citations
Publisher

Abstract

We present a method for measuring a complete frequency map of laser-dressed states with femtosecond lifetimes. It is based on collecting decay products as a function of the frequency of the excitation pulse and its delay with respect to the linearly chirped laser pulse, centered at the resonant transition frequency. The method has been tested on the case of laser-coupled $2s2p\phantom{\rule{4pt}{0ex}}^{1}P^{o}$ and $2{p}^{2}\phantom{\rule{4pt}{0ex}}^{1}S^{e}$ autoionizing resonances in He and is applicable to other quantum systems with short-lived states. When the laser coupling effects are known, the excitation pulse properties can be extracted from the map.

DOI
10.1103/physreva.99.053423

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We present a method for measuring a complete frequency map of laser-dressed states with femtosecond lifetimes. It is based on collecting decay products as a function of the frequency of the excitation pulse and its delay with respect to the linearly chirped laser pulse, centered at the resonant transition frequency. The method has been tested on the case of laser-coupled 2s2p1Po2s2p\phantom{\rule{4pt}{0ex}}^{1}P^{o}2s2p1Po and 2p21Se2{p}^{2}\phantom{\rule{4pt}{0ex}}^{1}S^{e}2p21Se autoionizing resonances in He and is applicable to other quantum systems with short-lived states. When the laser coupling effects are known, the excitation pulse properties can be extracted from the map.
Extreme ultraviolet (EUV) transient absorption spectrum of helium dressed by a moderately intense infrared laser pulse is investigated. Strategies for correct retrieval of the time-dependent quasi-energies of helium with excitation energies covering both singly and doubly excited states are proposed. For long-lived singly excited states, the profound hyperbolic structures due to long lasting dipole can be diminished by convoluting the transient absorption spectrogram with a spectral window, allowing the time-dependent quasi-energies close to 1s2p resonance to be correctly mapped out. For short-lived doubly excited states near 2s2p resonance, the radiation dipole decays rapidly due to autoionization and the transient absorption spectrogram already recovers the main structure of quasi-energies without the convolution operation. The quantum simulation indicates that the convolution operation controls the effective decay speed of the dipole moment, which effectively builds up an instant probe that is essential for mapping time dependent quasi-energies of laser dressed systems.
Within this work, electron dynamics inside argon atoms are observed by probing the autoionizing states of argon atoms, so-called window resonances, with both attosecond XUV and timed-delayed few-cycle femtosecond NIR laser pulses, using attosecond transient absorption spectroscopy. The window resonances in the energy region of 25 - 29.3 eV are first excited with the XUV pulse and then dressed by the NIR laser, where the natural decay process of the states is greatly affected by the strong-field of the NIR pulse. Preliminary results of the measurement are presented in this work, with a hypothetical description of some of the effects that are present. A comparison has been made with the experimental results from a paper publishing measurements of autoionizing states with attosecond transient absorption spectroscopy for the first time, where the same resonances were probed. The comparison is only partly possible due to different experimental parameters and conditions, where more pronounced and new effects have been observed in the here performed measurement.
We study theoretically the photoabsorption spectra of an attosecond extreme ultraviolet (XUV) pulse by a laser-dressed atomic system. A weak XUV excites an autoionizing state which is strongly coupled to another autoionizing state by a laser. The theory was applied to explain two recent experiments [Loh, Greene, and Leone, Chem. Phys. 350, 7 (2008); Wang, Chini, Chen, Zhang, Cheng, He, Cheng, Wu, Thumm, and Chang, Phys. Rev. Lett. 105, 143002 (2010)] where the absorption spectra of the XUV lights were measured against the time delay between the laser and the XUV. In another example, we study an attosecond pulse exciting the 2s2p(1P)2s2p{(}^{1}\phantom{\rule{-0.16em}{0ex}}P)2s2p(1P) resonance of helium which is resonantly coupled to the 2s2(1S)2{s}^{2}{(}^{1}\phantom{\rule{-0.16em}{0ex}}S)2s2(1S) resonance by a moderately intense 540-nm laser. The relation between the photoabsorption spectra and the photoelectron spectra and the modification of the transmitted lights in such an experiment are analyzed. The role of Rabi flopping between the two autoionizing states within their lifetimes is investigated with respect to the laser intensity and detuning.
We report a measurement of the 5P3/2 excited-state lifetime using two-pulse photon echoes in Rb vapor. The measurement is precise to ∼1% and agrees with the best measurement of atomic lifetime in Rb. The results suggest that a measurement precise to ∼0.25% is possible through additional data acquisition and study of systematic effects. The experiment relies on short optical pulses generated from a cw laser using acousto-optic modulators. The excitation pulses are on resonance with the F=3-->F′=4 transition in Rb85 or the F=2-->F′=3 transition in Rb87. The resulting photon echo signal is detected using a heterodyne detection technique. The excited-state lifetime is determined by measuring the exponential decay of the echo intensity as a function of the time between the excitation pulses. We also present a study of the echo intensity as a function of excitation pulse area and compare the results to simulations based on optical Bloch equations. The simulations include the effects of spontaneous emission as well as spatial and temporal variations of the intensities of excitation pulses.
The AC Stark shift of electronic levels is ubiquitous in the interaction of intense light fields with atoms and molecules. As the light intensity changes on the rising and falling edges of a femtosecond laser pulse, it shifts the Rydberg states in and out of multiphoton resonances with the ground state. The two resonant pathways for transient excitation arising at the leading and the trailing edges of the pulse generate Young's type interference, generally referred to as the St\"uckelberg oscillations. Here we report the observation of the St\"uckelberg oscillations in the intensity of the coherent free-induction decay following resonant multiphoton excitation. Moreover, combining the experimental results with accurate numerical simulations and a simple model, we use the St\"uckelberg oscillations to recover the population dynamics of strongly driven Rydberg states inside the laser pulse by all-optical measurements after the end of the pulse. We demonstrate the potential of this spectroscopy to characterize lifetimes of Rydberg states dressed by laser fields with strengths far exceeding the Coulomb field between the Rydberg electron and the core.