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Physical Review A

Direct observation of two-photon-resonance Autler-Townes splitting of atomic sodium

Wankai Li, Yixuan Wang, Xing Li, Tao Yang, Dongdong Zhang, Dajun Ding

Published Jun 2, 2025• 6 citations
Publisher

Abstract

A two-photon resonance in the sodium atom $3s\text{\ensuremath{-}}4s$ transition is investigated in the strong coupling regime with photoelectron momentum imaging techniques. The kinetic energies of the ionized electron map out the eigenenergies of the dressed states and emerge as the Autler-Townes (AT) splitting, which is proportional to the laser intensity due to the two-photon nature. The partial wave analysis of the angular distribution of the photoelectrons reveals the relative phase shift from dressed states which is related to the attosecond ionization time delays. The phase shift between the two electron wave packets produced from AT splitting are attributed to the combination of the Coulomb phase and the quantum defect phase.

DOI
10.1103/physreva.111.063102

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Abstract Resonance‐enhanced multiphoton ionization (REMPI) in potassium atom is investigated within the strong coupling regime using photoelectron momentum imaging techniques. The kinetic energy distribution of the ionized electrons reveals the eigenenergies of the dressed states, which exhibit Autler–Townes (AT) splitting. This splitting is proportional to the laser field strength. Partial wave analysis of the photoelectrons angular distributions (PAD) uncovers relative phase shifts between the dressed states, shedding light on attosecond ionization time delays. The observed phase shift between the two electron wave packets by the AT splitting arises from the combined effects of the Coulomb phase and the quantum defect phase.
We study the photoelectron spectra of hydrogen and helium ionized by intense ultrafast two-color XUV laser pulses by numerically solving the time-dependent Schrödinger equation.The photon energy of the pump pulse is tuned to the 1s-2p excitation energy, inducing Rabi oscillations between these bound states and forming an Autler-Townes (AT) doublet of dressed states.When ionized by a time-delayed ultrafast XUV pulse with duration shorter than the Rabi oscillation period, we find novel and drastically enhanced AT splittings in the photoionization spectrum.We identify their origin in terms of the temporal interference of two attosecond wave packets whose spectral distribution is controlled by the interplay between Rabi frequency and bandwidth of the probe pulse.These time-dependent features in the spectra can be much larger than the standard AT spacing induced by the pump pulse alone and can be controlled by the time delay and the duration of the probe pulse.
Photoelectron energy spectra resulting from two-photon ionization of calcium atoms by 180 fs pulses have been studied as a function of wavelength (380--405 nm) and intensity ( $9\ensuremath{-}900\phantom{\rule{0ex}{0ex}}\mathrm{GW}/{\mathrm{cm}}^{2}$). When the wavelength is tuned near the $4s\ensuremath{\rightarrow}4p$ or $4s\ensuremath{\rightarrow}5s$ ionic core transition, the photoelectron peaks display a characteristic splitting proportional to the field strength and assignable to a two-electron continuum-continuum Autler-Townes effect. Spectra obtained by an essential-state model involving three coupled continua are compared to the experiment.
We present a bound-continuum ionization model combined with numerical simulations to investigate the asymmetric features of Autler-Townes (AT) splitting in the ionization spectra of hydrogen atoms, induced by a spectrally phase-modulated ultrashort pulse. This model incorporates a resonance-enhanced two-photon ionization process, enabling transitions from the ground electronic state to the continuum state via the first excited electronic state through the absorption of two photons. By comparing our model predictions with exact numerical simulations based on time-dependent electronic wave-packet calculations, we demonstrate that the characteristics of the AT doublets, shaped by the spectral phase, emerge from the competing effects of selective population of dressed states and the transition amplitude to the continuum. In addition, through a perturbative analysis of the photoelectronic spectrum and the application of the Magnus expansion, we reveal a correlation between the number of AT fringes, resonant states, and pulse area, while drawing insights from bound states. This work enhances our understanding of how the spectral phase can be utilized to explore bound-state effects in ultrafast ionization dynamics.
We study the multiphoton ionization of potassium atoms in 800 nm and 400 nm femtosecond laser fields. In the 800 nm laser field, the potassium atom absorbs three photons and emits one electron via one photon resonance with the 4p intermediate state with the help of the ac-Stark shift. The resonance feature is clearly shown as an Autler–Townes (AT) splitting and is mapped out in the electron kinetic energy spectrum. In a 400 nm laser field, although one photon resonance is possible with the 5p state, no splitting is observed. The different transition amplitudes between 4s–4p and 4s–5p explain the observed results. Due to the AT effect, an unexpected peak in the photoelectron energy spectrum that violates the dipole transition rule is observed. A preliminary explanation involving the spin-orbit interaction in the p state is given to account for this component. The observed AT-splitting in the electron kinetic energy distribution can be used as an effective method to calibrate the intensity of a laser field.
The resonant dynamic Stark effect, observed in the Autler-Townes (AT) splitting, plays a central role in ultrafast strong-field physics. Recent experiments have demonstrated the phase control of the AT doublet in atomic resonance-enhanced multiphoton ionization using intense resonant shaped femtosecond laser pulses [Bayer et al., Adv. Chem. Phys. 159, 235 (2016)]. Based on a two-state model, we showed that the underlying control mechanism is the selective population of dressed states (SPODS). In this work, we use a numerical model to calculate the photoelectron momentum distribution (PMD) based on the ab initio solution of the two-dimensional (2D) time-dependent Schr\"odinger equation (TDSE) to obtain a more complete physical picture of the nonperturbative control of the AT doublet. The 2D-TDSE model reproduces the ultrafast switching among the AT components while also revealing deviations from the signatures predicted by the two-state model. These deviations are attributed to the influence of additional intermediate states. To rationalize our observations, we propose a refined five-state model that includes all significantly populated bound states from the full calculation and accurately reproduces the 2D PMD. Based on the validated five-state model, we conduct a dressed-state analysis which provides a clear physical picture of the SPODS mechanism in a multistate system and sheds light on the role of the intermediate states in strong-field control.