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The Journal of Chemical Physics

On the control of the production of hydrogen atom 2s–2p resonance hybrids through the use of competitive one- and two-photon transitions from the ground state

B. N. Jagatap, William J. Meath

Published Jul 22, 2000• 4 citations
Publisher

Abstract

The control of the formation of dipolar hydrogen atom 2s–2p hybrid states, through varying the relative phase δ of two lasers inducing simultaneous one- and two-photon transitions from the ground state, is discussed by using time-dependent perturbation theory. Numerical examples are presented that illustrate how the populations of the hybrid states can be controlled by varying δ. The perturbative calculations are augmented by various exact finite basis set, and full split operator/fast Fourier transform, solutions to the time-dependent wave equation for the problem.

DOI
10.1063/1.481936

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Journal of Physics B Atomic Molecular and Optical Physics•Jun 23, 2008•1 citation
The control of the formation of dipolar hydrogen atom 2s–2p hybrid states, through varying the relative phase δ of two lasers inducing simultaneous one- and two-photon transitions from the ground state, is discussed by using time-dependent perturbation theory. Numerical examples are presented that illustrate how the populations of the hybrid states can be controlled by varying δ. The perturbative calculations are augmented by various exact finite basis set, and full split operator/fast Fourier transform, solutions to the time-dependent wave equation for the problem.
We have solved the time-dependent Schr\"odinger equation to analyze the time evolution of a hydrogen atom, initially in its ground 1s state, interacting with a one- or two-color linearly polarized laser pulse which is tuned close to a two-photon resonance with the 2s metastable state. The two-photon transition therefore does not involve an intermediate resonance state. Using a suitable combination of two laser pulses of different frequencies, population can be transferred from the 1s state to the 2s state via the continuum. In both the single-color and the two-color cases, a maximum amount of 17% of population can be found in the 2s state at the end of the pulse. We compare and interpret our results in terms of the time-independent Floquet eigenvalues. The system can also be modeled by an ``essential states'' two-level atom with decay. Both the Floquet and the time-dependent solutions are compared with the model predictions. The model allows systematic optimization studies for population transfer under a wide range of laser pulse parameters.
We consider the time evolution of the occupation probabilities for the $2s\ensuremath{-}2p$ transition in a hydrogen atom interacting with an external field V(t).V(t).V(t). A two-state model and a dipole approximation are used. In the case of degenerate energy levels an analytical solution of the time-dependent Schr\"odinger equation for the probability amplitudes exists. The form of the solution allows one to choose the ratio of the field amplitude to its frequency that leads to temporal trapping of electrons in specific states. The analytic solution is valid when the separation of the energy levels is small compared to the energy of the interacting radiation.
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.
Within the framework of time-dependent perturbation theory, general expressions are derived for the cross section of multiphoton processes induced by radiation acting on a hydrogen atom. Bound-bound transitions involving emission of a single quantum and bound-free transitions are calculated for a wide range of photon energies. In the case of resonance, the transition probability is also discussed. The procedure used to evaluate the sums over intermediate states is described. The numerical computation allows one to compare the results obtained for various competing processes.
The dynamics and the cross sections associated with the excitation of a ground-state dipolar molecule to an excited state, by the simultaneous absorption of two photons, are discussed using the rotating wave approximation and time-dependent perturbation theory. The excitations of ten- and two-energy level representations of model dipolar molecules are used for illustrative purposes. The temporal development of the final state of the excitation process and the two-photon excitation cross sections are discussed as functions of laser intensity, laser–molecule interaction time and the two types of excitation mechanism (which are available for dipolar molecules, relative to the one mechanism for a non-polar molecule). The results are used to discuss the validity of perturbation theory treatments of the problem and various strategies for the enhancement of the intrinsically weak two-photon excitation process.
Analyses of the resonant multiphoton ionization of atoms require knowledge of ac Stark energy shifts and of multiphoton, bound-to-bound state, transition amplitudes. In this paper, we consider the three-photon photoionization of hydrogen atoms at frequencies that are at and surrounding the two-photon 1s to 2s resonance. AC energy shift sums of both the 1s and 2s states are calculated as a function of the laser frequency along with two-photon 1s ? 2s resonant transition amplitude sums. These quantities are calculated using an extended version of a method, which has often been employed in a variety of ways, of calculating these sums by expressing them in terms of solutions to a variety of differential equations that are derived from the different sums being evaluated. We demonstrate how exact solutions are obtained to these differential equations, which lead to exact evaluations of the corresponding sums. A variety of different cases are analysed, some involving analytic continuation, some involving real number analysis and some involving complex number analysis. A dc Stark sum calculation of the 2s state is carried out to illustrate the case where analytic continuation, pole isolation and pole subtraction are required and where the calculation can be carried out analytically; the 2s state, ac Stark shift sum calculations involve a case where no analytic continuation is required, but where the solution to the differential equation produces complex numbers owing to the finite photoionization lifetime of the 2s state. Results from these calculations are then used to calculate three-photon ionization probabilities of relevance to an analysis of the multiphoton ionization data published by Kyrala and Nichols (1991 Phys. Rev. A 44, R1450).