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Physical Review A

Pathways to excitation of atoms with bicircular laser pulses

Joel Venzke, Yonas Gebre, Andreas Becker, Agnieszka Jaroń-Becker

Published May 14, 2020• 7 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.101.053425

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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 \ensuremathΛ\mathrm{\ensuremath{\Lambda}}\ensuremathΛ-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 \ensuremathΔm=\ifmmode±\else\textpm\fi3\mathrm{\ensuremath{\Delta}}m=\ifmmode\pm\else\textpm\fi{}3\ensuremathΔm=\ifmmode±\else\textpm\fi3. 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.
We present a study of higher-order Raman ($\mathrm{\ensuremath{\Lambda}}, V$, and SSS) transitions between Rydberg states involving the absorption and emission of at least three photons in the interaction of two-color corotating circularly polarized laser pulses with the hydrogen atom. Our analysis is based on results of numerical solutions of the corresponding time-dependent Schr\"odinger equation. The results for the interaction with ($\ensuremath{\omega},2\ensuremath{\omega}$) fields show that the simultaneous interaction with both fields results in an excited state distribution over a broad range of magnetic quantum numbers. Indications of the impact of the $\mathrm{\ensuremath{\Lambda}}, V$, and SSS transitions are found via the analysis of final distributions resulting from the preparation of the atom in specific Rydberg states. Furthermore, we show that similar mechanisms for the redistribution of population between Rydberg states are present in two-color fields with larger differences in the central frequencies, i.e., ($\ensuremath{\omega},3\ensuremath{\omega}$) and ($\ensuremath{\omega},4\ensuremath{\omega}$) fields.
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.
Abstract We consider the excitation of Rydberg states through photons carrying an intrinsic orbital angular momentum degree of freedom. Laguerre–Gauss modes, with a helical wave-front structure, correspond to such a set of laser beams, which carry units of orbital angular momentum in their propagation direction, with ℓ 0 the winding number. We demonstrate that, in a proper geometry setting, this orbital angular momentum can be transferred to the internal degrees of freedom of the atoms, thus violating the standard dipole selection rules. Higher orbital angular momentum states become accessible through a single photon excitation process. We investigate how the spacial structure of the Laguerre–Gauss beam affects the radial coupling strength, assuming the simplest case of hydrogen-like wavefunctions. Finally we discuss a generalization of the angular momentum coupling, in order to include the effects of the fine and hyperfine splitting, in the context of the Wigner–Eckart theorem.
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.
Numerical integration of the Schr\"odinger equation for the resonant single-photon excitation from the 1s1s1s to 10p10p10p state in atomic hydrogen has been used to produce solutions converged to a precision of a few parts per million. At all intensities investigated (in the range 10−−100TW/cm2),10--100{\mathrm{T}\mathrm{W}/\mathrm{c}\mathrm{m}}^{2}),10−−100TW/cm2), the population in the states having angular momentum higher than l=1\mathcal{l}=1l=1 after a narrowband (500 fs) laser pulse are found to be neglible. This shows that off-resonant states can effectively suppress Raman-like transitions to degenerate states of higher angular momentum. Instead of such mixing, strong Rabi-like oscillations between 1s1s1s and the np\mathrm{np}np Rydberg series are observed.
We present a comprehensive and ab initio nonperturbative investigation of the coherent population transfer among the 3D high-lying Rydberg hydrogen and alkali atomic states via linearly polarized chirped microwave pulses. The time-dependent Schrödinger equation for the dynamical evolution of Rydberg atoms is accurately and efficiently solved by means of the time-dependent generalized pseudospectral method. For atomic H, the population transfer from n = 35 to 30 with nearly 100% efficiency is achieved by means of the sequential two-photon Deltan = -1 transitions. The calculation fully utilizes all of the available orbital angular momentum l states for a given n, and the interference pattern and population evolution dynamics of individual l states are analyzed in detail. It is shown that the coherent control of the population transfer from the high n to the low n states can be accomplished by the optimization of the chirping parameters and microwave field strength. Similar analysis is performed for the Na atom, where the alkali atomic structure is described by an accurate model potential. We found that while the global population transfer pattern is qualitatively similar, there are significant differences in the dynamical response of atomic H and Na to the chirped microwave fields. Due to the degeneracy of the l states (for a given n) in unperturbed atomic H, the population transfer involves significant coupling and interference among a number of low-lying l states. For the case of Na atoms, however, the population transfer from the n to (n - 1) state is dominated by a single channel, namely, from the |n,l = 0> to the |n - 1,l = 0> state.