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ACS Photonics

Zeptosecond Control of Fano Line Shapes in Laser-Dressed Atoms Excited by Time-Delayed Attosecond Pulse Pairs

Yong Fu, Bincheng Wang, Xiangyu Tang, Jiahao You, Feier Xu, C. D. Lin, Cheng Jin

Published Apr 20, 2026• 1 citation
Publisher

Abstract

The attosecond pump-femtosecond probe technique is widely used in electron dynamics research, with temporal resolution reaching tens of attoseconds. Here, we propose a scheme for controlling the Fano line shapes of helium doubly excited states by replacing the pump source with a pair of time-delayed attosecond pulses. We show that the interference induced by this delay provides an additional, highly effective means of controlling electron dynamics, enabling temporal resolution on the zeptosecond scale. We demonstrate that the corresponding line shapes in transient absorption spectra can shift dramatically within a time-delay variation of just a few hundred zeptoseconds. This extreme spectral modulation occurs under two key conditions: (i) when the time delay aligns with the spectral minimum of the coherently combined attosecond pulses in the frequency domain, and (ii) when the delay between the infrared probe pulse and the first attosecond pulse is held constant. This approach opens a new pathway to zeptosecond-scale control in quantum systems and demonstrates the powerful synergy between phase manipulation in both light and electron waves for achieving ultrafast spectral transformations.

DOI
10.1021/acsphotonics.6c00251

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Communications in Theoretical Physics•Oct 19, 2022•2 citations
The attosecond pump-femtosecond probe technique is widely used in electron dynamics research, with temporal resolution reaching tens of attoseconds. Here, we propose a scheme for controlling the Fano line shapes of helium doubly excited states by replacing the pump source with a pair of time-delayed attosecond pulses. We show that the interference induced by this delay provides an additional, highly effective means of controlling electron dynamics, enabling temporal resolution on the zeptosecond scale. We demonstrate that the corresponding line shapes in transient absorption spectra can shift dramatically within a time-delay variation of just a few hundred zeptoseconds. This extreme spectral modulation occurs under two key conditions: (i) when the time delay aligns with the spectral minimum of the coherently combined attosecond pulses in the frequency domain, and (ii) when the delay between the infrared probe pulse and the first attosecond pulse is held constant. This approach opens a new pathway to zeptosecond-scale control in quantum systems and demonstrates the powerful synergy between phase manipulation in both light and electron waves for achieving ultrafast spectral transformations.
In the present paper, we investigate the time-resolved transient absorption spectroscopy of doubly excited states of helium atoms by solving the time-dependent two-electron Schr\"odinger equation numerically based on a one-dimensional model. The helium atoms are subjected to an extreme ultraviolet (XUV) attosecond pulse and a time-delayed infrared (IR) few-cycle laser pulse. A superposition of doubly excited states populated by the XUV pulse is identified, which interferes with the direct ionization pathway leading to Fano resonance profiles in the photoabsorption spectrum. In the presence of an IR laser, however, the Fano line profiles are strongly modified: A shifting, splitting, and broadening of the original absorption lines is observed when the XUV attosecond pulse and infrared few-cycle laser pulse overlap in time, which is in good agreement with recent experimental results. At certain time delays, we observe symmetric Lorentz, inverted Fano profiles, and even negative absorption cross sections indicating that the XUV light can be amplified during the interaction with atoms. We further prove that the above pictures are general for different doubly excited states by suitably varying the frequency of the IR field to coherently couple the corresponding states.
Metastable states are important actors in the ionisation of atoms and molecules. Sub-femtosecond extreme ultraviolet pulses can coherently populate several transiently bound states at once, thus starting the attosecond clocks which are required to monitor and control ultrafast electronic evolution above the ionisation threshold. Here we illustrate, from a theoretical point of view, the effects coherent superpositions of 1 P o doubly excited states in the helium atom have on channel-resolved photoelectron spectra as well as on the transient absorption spectrum of the atom in the extreme ultraviolet region, when they are created by a single-attosecond pulse in the presence of a strong few-cycle near-infrared/visible pulse which acts as a probe. Interference fringes varying rapidly with the pump-probe time delay are visible in both photoelectron and transient absorption spectra. From such fringes, the wave packet itself can conceivably be reconstructed. Conversely, all observables are modulated by the characteristic beating periods of the wave packet, so that control of partial ionisation yields, branching ratios, and light absorption or amplification can be achieved.
Within this work, electron dynamics in atoms are experimentally and numerically investigated on their natural attosecond time scales. To access these dynamics, ultrashort and moderately-intense few-cycle laser pulses are superposed with attosecond pulsed radiation in the extreme-ultraviolet spectral region. Both these sources are combined in a new experimental vacuum setup which was designed and built up from scratch, also in order to generate the attosecond pulses. Novel experimental schemes are developed which involve the temporal and spectral interferometric utilization of both ultrashort light sources and include the multidimensional spectroscopy employing different dynamical parameters. These are the intensity and the carrier-envelope phase of the laser pulses, as well as their temporal delay with respect to the attosecond pulses. Scientifically, the observation and control of the quantum-motion of bound electrons, as well as the laser-driven quasi-classical motion of free electrons was a key goal of this work. In particular, a bound two-electron wave packet in helium on attosecond time scales was experimentally observed for the first time. This was realized by combining unprecedented high temporal and spectral resolution. In addition, a new coupling mechanism of several doubly-excited states to an effective single-electron continuum is identified and analyzed. Both these two-electron states as well as single-electron states are interferometrically investigated with access to the phase of their quantum-mechanical wave function. This allows the observation and control of the quantum dynamics of two correlated electrons in atoms on the attosecond time scale which was demonstrated within the scope of this work.
Line shapes observed in attosecond transient absorption spectra (ATAS) encode information on the phase of the optical dipole response. Understanding and controlling the phase evolution of interference fringes is among the fundamental goals of exploring coherent interaction. Here, we simulate the attosecond transient absorption in the near-infrared (NIR) dressing field by considering a three-level model in the adiabatic approximation. We find that the absorption line shape can be changed from Lorentzian to Fano to inverted Lorentzian and back again at two-photon dressed energy levels “ω ± 2ωι”, and line shapes evolve in half-cycle periodicity (T/2). Moreover, the direction of phase evolution of “ω ± 2ωι” is opposite, while the phases of “ω ± 2ωι” are roughly the same at certain delays with an interval of approximately a quarter-cycle periodicity (T/4). These results demonstrate that absorbance of two-photon dressed energy levels “ω ± 2ωι” can qualitatively map the AC Stark shift. These observations provide new insights into the control of spectral line shapes and open the way for the modulation of quantum optical interference in the laser-driven atom.
An optical coherent control scheme has been proposed and theoretically investigated where an extreme ultraviolet single attosecond pulse (SAP) propagates through dense helium gas dressed by a time-delayed femtosecond laser pulse. The laser pulse couples the 2s2p( 1 P) and 2s 2 ( 1 S) autoionizing states when the SAP excites the 2s2p state. After going through the gas, the spectral and temporal profiles of the SAP are strongly distorted. A narrowed but enhanced spike in the spectrum shows up for specific intensities and time delays of the laser, which exemplifies the control of a broadband photon wave packet by an ultrashort dressing field for the first time. We analyse the photon and electron dynamics and determine the dressing condition that maximizes this enhancement. The result demonstrates new possibilities of attosecond optical control.
Abstract Attosecond transient absorption (ATA) has been developed as an all-optical technique for probing electron dynamics in matter. Here we present a scheme that can modify the laser-induced state and the corresponding ATA spectrum via excitation by a pair of XUV attosecond pulses and by a time-delayed mid-infrared (MIR) laser probe. Different from the scheme of the electronic excitation by a single XUV attosecond pulse, the application of a pair of XUV pulses provides extra degrees of freedom, such as the time delay and the intensity ratio between two XUV pulses, which make it possible to adjust the pump process, resulting in the modification of the ATA spectrum. We show that by varying the time delay between the two XUV pulses, the population of the dark state and the ATA spectrum of the laser-induced state have periodic modulations. We also demonstrate that the peak of the ATA spectrum of the laser-induced state appears at a fixed time delay between the XUV pair and the MIR laser when the intensity ratio is large, and it changes with the time delay when the intensity ratio is small, which can be related to either one of two peaks in the population of the dark state.