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arXiv:1007.0371 · Physical Review A

Multiphoton resonance in a three-level system with nearly degenerate excited states

Michał Berent, R. Parzyński

Published Aug 10, 2010• 6 citations
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Abstract

An analytic study is presented of the efficient multiphoton excitation and strong harmonic generation in three-level systems specified by a pair of nearly degenerate, strongly dipole-coupled excited states. Such systems are physically formed by the three lowest states in, e.g., the hydrogen atom or evenly charged homonuclear diatomic molecular ions under reasonably chosen laser intensities. As a detailed analytic result, we found that the laser pulse of photon energy $2.05\text{eV}$, duration $0.23\text{ps}$, and intensity $5\ifmmode\times\else\texttimes\fi{}{10}^{13}\frac{\mathrm{W}}{{\mathrm{cm}}^{2}}$ is able to produce complete inversion of the initial population in the hydrogen atom through the five-photon excitation. At the same photon energy, the pulse of duration $0.41\text{ps}$ and intensity $3.44\ifmmode\times\else\texttimes\fi{}{10}^{14}\frac{\mathrm{W}}{{\mathrm{cm}}^{2}}$ was found to produce the same effect in the molecular ion but through the nine-photon excitation. We show that the accompanying scattering of light has very rich spectrum differing substantially from that of the two-level system.

DOI
10.1103/physreva.82.023804

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An analytic study is presented of the efficient multiphoton excitation and strong harmonic generation in three-level systems specified by a pair of nearly degenerate, strongly dipole-coupled excited states. Such systems are physically formed by the three lowest states in, e.g., the hydrogen atom or evenly charged homonuclear diatomic molecular ions under reasonably chosen laser intensities. As a detailed analytic result, we found that the laser pulse of photon energy 2.05eV2.05\text{eV}2.05eV, duration 0.23ps0.23\text{ps}0.23ps, and intensity 5\ifmmode×\else\texttimes\fi1013Wcm25\ifmmode\times\else\texttimes\fi{}{10}^{13}\frac{\mathrm{W}}{{\mathrm{cm}}^{2}}5\ifmmode×\else\texttimes\fi1013cm2W​ is able to produce complete inversion of the initial population in the hydrogen atom through the five-photon excitation. At the same photon energy, the pulse of duration 0.41ps0.41\text{ps}0.41ps and intensity 3.44\ifmmode×\else\texttimes\fi1014Wcm23.44\ifmmode\times\else\texttimes\fi{}{10}^{14}\frac{\mathrm{W}}{{\mathrm{cm}}^{2}}3.44\ifmmode×\else\texttimes\fi1014cm2W​ was found to produce the same effect in the molecular ion but through the nine-photon excitation. We show that the accompanying scattering of light has very rich spectrum differing substantially from that of the two-level system.
We consider harmonics generation and wave mixing by two-color multiphoton resonant excitation of three-level atoms and molecules in strong laser fields. The coherent part of the spectra corresponding to multicolor harmonics generation is investigated. The obtained analytical results on the basis of a generalized rotating wave approximation are in a good agreement with numerical calculations. The results applied to the hydrogen atoms and homonuclear diatomic molecular ions show that one can achieve efficient generation of moderately high multicolor harmonics via multiphoton resonant excitation by appropriate laser pulses.
Compared to single-photon rates, multiphoton excitation rates of atoms and molecules are generally quite small, even at high laser intensities, at least in a 2-level system. Small multiphoton coupling strengths, large ac Stark shifts, and ionization all inhibit real population transfer between bound states. However, it has recently been shown that a 3-level system consisting of a ground state and a pair of nearly degenerate strongly coupled upper states greatly enhances the multiphoton coupling with the ground state, while also greatly reducing the ac Stark shift of the ground state. In this paper I will derive an analytic expression for the n-photon Rabi frequency, for this system, in the case of degenerate upper states, as well as an expression for the level shifts induced in the case of nondegenerate upper states. Numerical calculations based on the 3-level system are presented to verify the analytic results and to show that high-order \ensuremath{\pi} pulses can be driven at moderate field strengths. To demonstrate the feasibility of this process in a real physical system, I will present fully correlated 2-electron calculations in a model one-dimensional molecular potential, including ionization that show a 12-photon \ensuremath{\pi} pulse driven with near-infrared photons. In other words, a single excited state 18.6 eV above the ground state can be populated with over 90% efficiency with little ionization while the ground state is almost completely depopulated. Besides the possibility of producing an amplifying medium in the vacuum ultraviolet, this 3-level configuration may open the door to other strong field effects previously restricted to single-photon interactions, such as adiabatic passage and inner-shell ionization.
The coherent scattering spectrum of a three-level atom driven by an intense laser field with multiphoton resonant excitation is considered. The spectrum corresponding to harmonic generation is investigated both analytically and numerically for different initial atomic states. The analytical calculations are based on the generalized rotating wave approximation, which allows one to explain obtained spectra containing in general both even and odd harmonics. The results applied to the hydrogen atom show that one can achieve efficient generation of moderately high harmonics using multiphoton resonant excitation by appropriate laser pulses.
The multiphoton resonant excitation of three-level atoms in a strong laser field is investigated. The creation of various superposition states is shown. For implementation of these effects either the mean dipole moment in the excited states of an atom or, in three-level systems, a transition dipole moment between excited states (with energies close enough to each other) must be nonzero. The time evolution of the system is found using a nonperturbative resonant approach. Our calculations for the hydrogen atom suggest that by the appropriate optical pulses with moderate strong intensities one can achieve various superposition states by multiphoton resonant excitation.
Compared to single-photon rates, multiphoton excitation rates of atoms and molecules are generally quite small, even at high laser intensities, at least in a 2-level system. Small multiphoton coupling strengths, large ac Stark shifts, and ionization all inhibit real population transfer between bound states. However, it has recently been shown that a 3-level system consisting of a ground state and a pair of nearly degenerate strongly coupled upper states greatly enhances the multiphoton coupling with the ground state, while also greatly reducing the ac Stark shift of the ground state. In this paper I will derive an analytic expression for the n-photon Rabi frequency, for this system, in the case of degenerate upper states, as well as an expression for the level shifts induced in the case of nondegenerate upper states. Numerical calculations based on the 3-level system are presented to verify the analytic results and to show that high-order {pi} pulses can be driven at moderate field strengths. To demonstrate the feasibility of this process in a real physical system, I will present fully correlated 2-electron calculations in a model one-dimensional molecular potential, including ionization that show a 12-photon {pi} pulse driven with near-infrared photons. In other words, amore » single excited state 18.6 eV above the ground state can be populated with over 90% efficiency with little ionization while the ground state is almost completely depopulated. Besides the possibility of producing an amplifying medium in the vacuum ultraviolet, this 3-level configuration may open the door to other strong field effects previously restricted to single-photon interactions, such as adiabatic passage and inner-shell ionization.« less
We theoretically study intensity-saturation effects in resonant harmonic generation and multiphoton ionization. A first laser excites a two-photon resonance which is coupled by a second laser to an autoionizing state. Starting from an effective Hamiltonian for the three resonant atomic states, we derive a set of equations for the density matrix of the gaseous medium and the electromagnetic field within a semiclassical framework. We present and discuss analytical and numerical solutions of these equations which show a variety of line profiles depending critically on the intensities of the incident laser pulses.