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Physical Review A

Population transfer between valence states via autoionizing states using two-color ultrafast π pulses in XUV and the limitations of adiabatic passage

Xuan Li, C. William McCurdy, Daniel J. Haxton

Published Mar 31, 2014• 10 citations
Publisher

Abstract

Population transfer between two valence states of the Li atom with a Raman process via intermediate autoionizing states well above the ionization threshold is investigated using a recently developed implementation of the muticonfiguration time-dependent Hartree Fock method. It is found that a properly chosen sequence of pump and Stokes $\ensuremath{\pi}$ pulses can yield a population transfer efficiency of $53%$ at relatively low intensities, while the extension of the stimulated Raman adiabatic passage (STIRAP) approach to the XUV in this case is far less efficient and loses its characteristic robustness at high intensities. A rule of thumb for when STIRAP is practical is given, suggesting that at still shorter wavelengths STIRAP may be possible.

DOI
10.1103/physreva.89.031404

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Population transfer between two valence states of the Li atom with a Raman process via intermediate autoionizing states well above the ionization threshold is investigated using a recently developed implementation of the muticonfiguration time-dependent Hartree Fock method. It is found that a properly chosen sequence of pump and Stokes \ensuremathπ\ensuremath{\pi}\ensuremathπ pulses can yield a population transfer efficiency of 5353%53 at relatively low intensities, while the extension of the stimulated Raman adiabatic passage (STIRAP) approach to the XUV in this case is far less efficient and loses its characteristic robustness at high intensities. A rule of thumb for when STIRAP is practical is given, suggesting that at still shorter wavelengths STIRAP may be possible.
The population transfer of stimulated Raman adiabatic passage (STIRAP) is investigated using a time-dependent quantum wave packet method. The population is transferred from an initial state to a target state through the interaction of the external laser field with the permanent dipole moment and the transition dipole moment. The laser field is composed of an infrared pulse and a near ultraviolet pulse. The two pulses with small detunings are more efficient to achieve the STIRAP transition. The process of STIRAP is sensitive to the detunings of the two pulses. When the two detunings are the same in a Λ transition or the positive detuning of the pump pulse is equal to the negative detuning of the Stokes pulse in a ladder transition, the final population in the intermediate state can be eliminated and the target population is increased.
Abstract The population transfer of a NaH molecule from the ground state X 1 Σ + to the target state A 1 Σ + via stimulated Raman adiabatic passage (STIRAP) is investigated. The results show that the intensity, delay time and detuning have a significant effect on population transfer. A large population transfer is observed with increased pump and Stokes intensity, especially when the pump and Stokes intensity match. Population transfer also depends on the delay time between the pump laser pulse and the Stokes laser pulse. The detuning of the two pulses influences the population transfer. Efficient population transfer can be realized under the resonant or two-photon resonant condition.
Stimulated Raman scattering involving adiabatic passage (STIRAP) is a proven technique for population transfer in three-level systems with strong oscillator strengths. We show that the STIRAP process should also yield high transfer efficiencies when the densities of states near the intermediate and final levels are high, provided certain criteria for the experimentally controllable parameters are met. We also show that high transfer efficiencies may even be possible when the pump and Stokes lasers can access levels outside of the three-level system. The criteria are derived with an approach that emphasizes the adiabatic nature of the transfer process in an eigenvector of the interaction Hamiltonian that resembles a trapped state. The results are compared to density matrix calculations.
We have considered a coherent population transfer to a higher excited singlet state ( S2 ) of molecules with anomalous fluorescence in molecular assemblies (e.g., a dense medium). A direct excitation to S2 requires light in the UV region. Because of this, the transition is conveniently realized by a two-step (two-photon) process: S0→S1→S2 , where transitions S0→S1 and S1→S2 correspond to the optical region. We have shown that efficient stimulated Raman adiabatic passage (STIRAP) in the ladder configuration can be realized in this case, using suitably chirped pulses, to compensate a change of the two-photon transition frequency in time, induced by the pulses themselves, due to near dipole-dipole interactions. We have provided a reduced state formulation of the optical control process. Chirping the “pump” pulse that excites transition S0→S1 is nonequivalent to chirping the “Stokes” pulse that excites transition S1→S2 , with respect to the population of the intermediate state ( S1 ) in the pulse nonadiabatic regime. We have also shown that with suitably chirped pulses, efficient STIRAP still persists even for a rather large decay of the intermediate state.
We propose a technique which produces nearly complete ionization of the population of a discrete state coupled to a continuum by a two-photon transition via a lossy intermediate state whose lifetime is much shorter than the interaction duration. We show that using counterintuitively ordered pulses, as in stimulated Raman adiabatic passage (STIRAP), wherein the pulse coupling the intermediate state to the continuum precedes and partly overlaps the pulse coupling the initial and intermediate states, greatly increases the ionization signal and strongly reduces the population loss due to spontaneous emission through the lossy state. For strong spontaneous emission from that state, however, the ionization is never complete because the dark state required for STIRAP does not exist. We demonstrate that this drawback can be eliminated almost completely by creating a laser-induced continuum structure (LICS) by embedding a third discrete state into the continuum with a third control laser. This LICS introduces some coherence into the continuum, which enables a STIRAP-like population transfer into the continuum. A highly accurate analytic description is developed and numerical results are presented for Gaussian pulse shapes.
Four-photon stimulated Raman adiabatic passage--like (STIRAP-like) processes in the frame of the D1{D}_{1}D1​ optical transition line of atomic 39K^{39}\mathrm{K}39K are investigated theoretically by means of a rigorous model that takes into account all the atomic states involved in the interaction with the pump and Stokes light fields and is valid for any field intensities. The same sequential up-down-up-down transition involving two pump (up) and two Stokes (down) photons, going from the initial ground state $|F=2,M=+2\ensuremath{\rangle}$ to the final ground state $|F=1,M=0\ensuremath{\rangle}$, which was proven in the past to be very convenient for two-photon amplification and lasing, is considered here. The fact that two atomic states, one with F=1F=1F=1 and another with F=2F=2F=2, participate at each intermediate step of the multiphoton process makes the existence of an ideal unique adiabatic transfer state impossible, and at exact four-photon resonance the population-transfer efficiency to the final atomic state is low (below 60% in general, 80% in the best conditions). Nevertheless, it is shown that by choosing appropriate static detunings for the pump and Stokes fields with respect to the atomic transitions the system follows, sequentially, two adiabatic states, connected by an efficient diabatic passage, so that population-transfer efficiency asymptotically approaching 100% for increasing field amplitudes can be reached. These results are quite robust and suggest the possibility of using STIRAP (or STIRAP-like) pumping to, among other applications, increase the (presently very low) efficiency of two-photon amplification and lasing, a so far unfulfilled goal in quantum and nonlinear optics.