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Advanced Photonics

Rydberg state excitation in molecules manipulated by bicircular two-color laser pulses

Wenbin Zhang, Yongzhe Ma, Chenxu Lu, Fei Chen, Shengzhe Pan, Peifen Lu, Hongcheng Ni, Jian Wu

Published Jan 10, 2023• 19 citations
Publisher

Abstract

Multiphoton resonant excitation and frustrated tunneling ionization, manifesting the photonic and optical nature of the driving light via direct excitation and electron recapture, respectively, are complementary mechanisms to access Rydberg state excitation (RSE) of atoms and molecules in an intense laser field. However, clear identification and manipulation of their individual contributions in the light-induced RSE process remain experimentally challenging. Here, we bridge this gap by exploring the dissociative and nondissociative RSE of H2 molecules using bicircular two-color laser pulses. Depending on the relative field strength and polarization helicity of the two colors, the RSE probability can be boosted by more than one order of magnitude by exploiting the laser waveform-dependent field effect. The role of the photon effect is readily strengthened with increasing relative strength of the second-harmonic field of the two colors regardless of the polarization helicity. As compared to the nondissociative RSE forming H2 * , the field effect in producing the dissociative RSE channel of ( H + , H * ) is moderately suppressed, which is primarily accessed via a three-step sequential process separated by molecular bond stretching. Our work paves the way toward a comprehensive understanding of the interplay of the underlying field and photon effects in the strong-field RSE process, as well as facilitating the generation of Rydberg states optimized with tailored characteristics.

DOI
10.1117/1.ap.5.1.016002

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Multiphoton resonant excitation and frustrated tunneling ionization, manifesting the photonic and optical nature of the driving light via direct excitation and electron recapture, respectively, are complementary mechanisms to access Rydberg state excitation (RSE) of atoms and molecules in an intense laser field. However, clear identification and manipulation of their individual contributions in the light-induced RSE process remain experimentally challenging. Here, we bridge this gap by exploring the dissociative and nondissociative RSE of H2 molecules using bicircular two-color laser pulses. Depending on the relative field strength and polarization helicity of the two colors, the RSE probability can be boosted by more than one order of magnitude by exploiting the laser waveform-dependent field effect. The role of the photon effect is readily strengthened with increasing relative strength of the second-harmonic field of the two colors regardless of the polarization helicity. As compared to the nondissociative RSE forming H2 * , the field effect in producing the dissociative RSE channel of ( H + , H * ) is moderately suppressed, which is primarily accessed via a three-step sequential process separated by molecular bond stretching. Our work paves the way toward a comprehensive understanding of the interplay of the underlying field and photon effects in the strong-field RSE process, as well as facilitating the generation of Rydberg states optimized with tailored characteristics.
To study the physical mechanism of atomic Rydberg state excitation (RSE) in two-color laser fields, we solve the time-dependent Schrödinger equation (TDSE) to calculate the ionization and excitation of hydrogen atoms. The relationship between the excited state population and the excitation rate of hydrogen atoms and the intensity of the fundamental frequency (FW) field can be observed by adjusting the laser intensity of the second harmonic (SH) field. The results demonstrate that multiphoton resonance absorption aligns with the physical mechanism of atomic resonant state excitation in two-color laser fields.
We study the excitation of the hydrogen atom by bichromatic circularly polarized laser pulses using numerical solutions of the time-dependent Schr\"odinger equation. The results are in agreement with the selection rules for multiphoton processes in such fields, namely, excited states are populated in which orbital angular momentum and magnetic quantum numbers are either both odd or both even, independent of the relative helicity, peak intensity, and pulse duration of the pulses. For co-rotating pulses the results show that excitation predominantly proceeds to states with magnetic quantum number of the same helicity as the laser pulses. Besides pathways via direct photon absorption from the ground state our results indicate that a transfer of population among the Rydberg states occurs via $\mathrm{\ensuremath{\Lambda}}$-type transitions. In the case of counter-rotating pulses the largest excitation probability is found for Rydberg states that differ in magnetic quantum number by $\mathrm{\ensuremath{\Delta}}m=\ifmmode\pm\else\textpm\fi{}3$. This pattern allows us to estimate how many photons from each of the two bichromatic fields have been absorbed. Finally, we confirm that a population in Rydberg states beyond a maximum orbital angular quantum number is unlikely.
Quantum Dynamics of H2+H_2^+H2+​ in Orthogonal Two-Color Fields
We present full-dimensional quantum simulations of H2+H_2^+H2+​ dissociative ionization driven by strong orthogonal laser fields. We consider equal-frequency orthogonal components, which generate elliptical or circular polarization depending on their relative phase and amplitude, as well as orthogonal 800800800- and 400400400-nm two-color fields. These two-dimensional fields strongly modify the fragmentation dynamics. Most notably, we identify a high-energy peak in the proton kinetic-energy-release (KER) spectrum at approximately 4−54-54−5 eV that is absent from the corresponding single-color, linearly polarized calculations. The yield of this peak can be coherently controlled by varying the relative carrier-envelope phase of the perpendicular field component. The perpendicular field also disrupts the clear electron-proton energy-sharing pattern observed in the main 3−3.53-3.53−3.5 eV dissociation channel, indicating more complex multichannel dynamics. Time-dependent state projections and calculations initiated from individual excited states attribute the additional peak to laser-induced vibrational excitation of H2+H_2^+H2+​. Furthermore, the perpendicular field rotates the fragment angular distributions, causing the most probable proton and electron emission directions to deviate substantially from the principal zzz axis. These findings demonstrate that the spatial and temporal geometry of orthogonal laser fields provides an additional degree of freedom for controlling ultrafast electron-nuclear dynamics.
We theoretically investigate strong-field ionization of hydrogen atoms by orthogonally polarized two-color (OTC) laser pulses consisting of a fundamental field that is resonant with the 1s - 2p transition and its second harmonic. Numerical simulations are performed by solving the two-dimensional time-dependent Schrödinger equation and recording the photoelectron momentum distribution. In this strong-field resonant ionization, the atom undergoes many Rabi cycles and the electron can be emitted within a completed Rabi-cycle leading to the splitting of the localized momentum distribution. Here, the splitting is attributed to dynamic Rabi-splitting as a result of the dynamic Stark effect. The employed OTC scheme is shown to be efficient for controlling the dynamic Rabi-splitting through the control of quantum-path interferences involved in one-photon and two-photon absorption processes. The control scheme is accomplished by varying the relative ratio intensity and optical phase between the two pulses, and its footprint is mapped in the momentum distribution. This is shown to lead to an asymmetric distribution and suppression of the ionization process. The obtained results suggest the OTC scheme as a tool for coherent control of dynamic Rabi-oscillations via the controlled quantum-path interferences, thus opening new directions towards designing quantum states via the control OTC scheme.
We experimentally demonstrate one- and two-photon phase sensitive coherent control over the excitation and ionization of Rydberg states of Sr atom in the presence of a static homogeneous electric field. Without the field this excitation scheme can only be employed for the manipulation of angular distributions of photoelectrons and molecular photofragmentation products. Total atomic excitation-ionization yields cannot be modulated because the final states excited by each pathway are orthogonal to each other. When, however, a static electric field is applied, sss, ppp and ddd character is admixed into the final Rydberg state, which has no definite parity anymore. Hence, the excitation of the target Stark state from the ground state is possible with either two (fundamental laser frequency) photons or one (second harmonic frequency) photon and its population and further ionization can be controlled by varying the relative phase between the two radiation fields. The concept is successfully tested below as well as above the classical saddle point and with either mutually crossed or parallel linear laser beam polarizations (while the second harmonic beam polarization vector is always parallel to the static field direction). We examine the behavior of the obtained photoionization signal modulation depth VVV as a function of the static field strength FFF for otherwise identical experimental conditions. The V(F)V(F)V(F) curve exhibits a maximum (typically $\ensuremath{\sim}65%--85%$) at a field strength value that is dictated by the interplay between the employed laser power densities, one- and two-photon transition dipole moments, and relative amounts of field-dependent sss, ppp and ddd character. It is therefore shown that the static field strength may serve as an additional, experimentally adjustable, control parameter in a fashion complementary to both the intensities and relative phase of the two light beams.