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Journal of Physics B Atomic Molecular and Optical Physics

Competition of multiphoton ionization pathways in lithium

Balázs István Tóth, Attila Tóth, András Csehi

Published Feb 21, 2024• 10 citations
Publisher

Abstract

Abstract We study the three-photon ionization of atomic lithium by intense, short light pulses, via numerically solving the time-dependent Schrödinger equation. Two-photon Rabi oscillations are induced between the 2s and 4s states, which are damped due to single-photon ionization to the p continuum. Developing a minimal three-level model, we analyze the spectral features of the Autler–Townes (AT) doublet that is formed upon the resonant coupling with the laser pulse. Furthermore, we show that this 2 s →→ 4 s → p c o n t i n u u m pathway is the dominant process, if the duration of the laser pulse exceeds a certain value. For shorter pulses, ionization through the 2p state ( 2 s → 2 p → 4 d → f c o n t i n u u m ) gradually becomes the dominant process, provided that the pulse is strong enough to induce several Rabi floppings. Here, we trace the competition of these ionization pathways by observing the structural changes in the shape of the AT doublet.

DOI
10.1088/1361-6455/ad2b73

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Abstract We study the three-photon ionization of atomic lithium by intense, short light pulses, via numerically solving the time-dependent Schrödinger equation. Two-photon Rabi oscillations are induced between the 2s and 4s states, which are damped due to single-photon ionization to the p continuum. Developing a minimal three-level model, we analyze the spectral features of the Autler–Townes (AT) doublet that is formed upon the resonant coupling with the laser pulse. Furthermore, we show that this 2 s →→ 4 s → p c o n t i n u u m pathway is the dominant process, if the duration of the laser pulse exceeds a certain value. For shorter pulses, ionization through the 2p state ( 2 s → 2 p → 4 d → f c o n t i n u u m ) gradually becomes the dominant process, provided that the pulse is strong enough to induce several Rabi floppings. Here, we trace the competition of these ionization pathways by observing the structural changes in the shape of the AT doublet.
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.
We present numerical simulations of the reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) on lithium by solving the three-dimensional time-dependent Schr\"odinger equation. In our scheme, the infrared (IR) field couples the 2s2s2s and 2p2p2p states of lithium and leads to the Rabi oscillations of populations between these two states. We analyzed the RABBITT phases of the two peaks in the Rabi-oscillation-induced Autler-Townes splittings. Our results show that the relative phase between these two peaks changes with the photoelectron energy and depends on the intensity of the IR field. Moreover, in the angle-resolved RABBITT measurement, the phases of the two peaks depend differently on the emission angle of photoelectrons. These behaviors are traced back to the different initial phases of the electron wave packets emitted from the dressed 2p2p2p states and the competition among different ionization channels.
We theoretically investigate the resonant two-photon ionization of a hydrogen atom in the counter-rotating circularly polarized double-pulse sequences, by solving the time-dependent Schr\"odinger equation. Due to the induced Rabi oscillations between the ground and excited states, the well-known Autler-Townes doublet is observed in the photoelectron spectra. More interestingly, our numerical results reveal an additional peak located between the Autler-Townes doublets, which originates from single-photon ionization from the excited state by the second pulse. By adjusting the laser intensity of the two pulses, the photoelectron yields of the three peaks can be sensitively modulated, under the control of completed Rabi cycles within the first pulse. In addition, our results show a potential of manipulating the photoemission anisotropy by both the laser intensity and the two-pulse time delay, through adjusting the competition of different partial waves generated by the two pulses.
We calculate two-dimensional photoelectron momentum distributions and energy spectra after multiphoton ionization of Li atoms subject to intense laser fields in the one-photon Rabi-flopping regime. The time-dependent Schr\"odinger equation is solved within the single-active-electron approximation using a model potential which reproduces accurately the binding energies and dipole matrix elements of the Li atom. Interaction with the external electromagnetic field is treated within the dipole approximation. We show that the Rabi oscillations of the population between the ground 2s2s2s state and the excited 2p2p2p state in the one-photon resonance regime are reflected in the energy spectra of emitted photoelectrons, which manifest interference structures with minima. Transformations of the interference structures in the photoelectron energy spectra caused by the variation of the laser peak intensity and pulse duration are analyzed.
We study the Rabi flopping of the population between the ground and excited 2p states of the hydrogen atom, induced by intense short laser pulses of different shapes and of carrier frequency ω=0.375 a.u. which resonantly couples the two states, and manifestations of this dynamics in the energy spectra of photoelectrons produced in the subsequent ionization of the atom from the excited state. It is found that, for Gaussian, half-Gaussian and rectangular pulses, characterized by the same pulse area, the final populations take the same values and the spectra consist of similar patterns having the same number of peaks and approximately the same separation between the prominent edge (Autler–Townes) peaks. The additional analysis in terms of dressed states showed that the mechanism of formation of multiple-peak structures during the photoionization process is the same regardless of the pulse shape. These facts disprove the hypothesis proposed in earlier studies with Gaussian pulse, that the multiple-peak pattern appears due to dynamic interference of the photoelectrons emitted with a time delay at the rising and falling sides of the pulse, since the hypothesis is not applicable to either a half-Gaussian pulse that has no rising part or a rectangular pulse whose intensity is constant.
By numerically solving the three-dimensional time-dependent Schr\"odinger equation, two-photon ionization of hydrogen is investigated at the near-resonant frequencies of the $1s\text{\ensuremath{-}}2p$ transition. Due to the Rabi oscillations between the 1s1s1s and 2p2p2p states, the photoelectron energy spectra exhibit the Autler-Townes (AT) doublets and we focus on the energy spacing and the asymmetry of the doublets. Our results show that the laser frequency for the minimum energy spacing of AT doublets locates at the resonant frequency of the ac-stark-shifted states, while the symmetry of the AT doublets is affected both by the ac-stark shift and the nonresonant ionization pathway. Developing the minimal three-state model including all of the nonresonant (nonessential) states, the effects of the ac-stark shift and the nonresonant ionization pathway on the AT doublets due to the nonresonant states are identified. Furthermore, due to the nonresonant ionization pathway, the photoelectron angular distributions are distinctly different for the lower- and higher-energy peaks in the AT doublets and these angular distributions sensitively depend on the laser intensity and pulse duration. These results are well reproduced by our minimal three-state model.