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arXiv:1010.1228 · Physical Review A

Stimulated Raman adiabatic passage into continuum

Andon A. Rangelov, Nikolay V. Vitanov, E. Arimondo

Published Oct 12, 2007• 13 citations
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Abstract

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.

DOI
10.1103/physreva.76.043414

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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.
We present a fully quantum-mechanical theory of the mutual light-matter effects when two laser pulses interact with three discrete states coupled to a (quasi)continuum. Our formulation uses a single set of equations to describe the time dependence of the discrete and continuum populations, as well as pulse propagation in electromagnetically induced transparency (EIT) and stimulated Raman adiabatic passage (STIRAP) situations, for both weak and strong laser pulses. The theory gives a mechanistic picture of the ``slowing down of light'' and the state of spontaneously emitted photons during this process. Surprising features regarding the time dependence of material and radiative transients as well as limitations on quantum light storage and retrieval are unraveled.
This work explores the effect of spontaneous emission on the population transfer efficiency in stimulated Raman adiabatic passage (STIRAP). The approach uses adiabatic elimination of weakly coupled density matrix elements in the Liouville equation, from which a very accurate analytic approximation is derived. The loss of population transfer efficiency is found to decrease exponentially with the factor ${\ensuremath{\Omega}}_{0}^{2}∕\ensuremath{\Gamma}$, where $\ensuremath{\Gamma}$ is the spontaneous emission rate and ${\ensuremath{\Omega}}_{0}$ is the peak Rabi frequency. The transfer efficiency increases with the pulse delay and reaches a steady value. For large pulse delay and large spontaneous emission rate STIRAP degenerates into optical pumping.
We propose a pulse-shaping method for improving population transfer in multistate stimulated Raman adiabatic passage (STIRAP) with nearest-neighbour couplings only. The method extends the quasiparallel-eigenenergy approach, previously used for two- and three-state systems, to multistate chains without introducing additional shortcut fields. The pump and Stokes fields are shaped so that the eigenenergies closest to the dark state remain nearly parallel to it during the central part of the interaction, where nonadiabatic transitions are most likely to occur. We derive analytic prescriptions for the required pulse shapes and apply them to five-, seven-, and nine-state chains formed by magnetic sublevels of degenerate manifolds with angular momenta Jg→Je=JgJ_g\rightarrow J_e=J_gJg​→Je​=Jg​ and Jg→Je=Jg−1J_g\rightarrow J_e=J_g-1Jg​→Je​=Jg​−1 driven by a pair of right- and left-circularly polarized pulses. Numerical simulations show that the optimized pulses can reduce the population transfer error by several orders of magnitude compared to standard Gaussian pulses. The same shapes also improve robustness against variations of the peak Rabi frequency, the single-photon detuning, and the multiphoton detuning. The comparison between the two angular-momentum families shows that the Jg→JgJ_g\rightarrow J_gJg​→Jg​ chains are generally more favourable, because their Clebsch-Gordan coefficients keep the relevant bright-state gap larger in the region where the dark state changes most rapidly. Finally, simulations with spontaneous emission show that the optimized resonant pulses remain advantageous in the lossy regime as well.
This paper discusses a generalization of stimulated Raman adiabatic passage (STIRAP) in which the single intermediate state is replaced by N intermediate states. Each of these states is connected to the initial state ${\ensuremath{\psi}}_{i}$ with a coupling proportional to the pump pulse and to the final state ${\ensuremath{\psi}}_{f}$ with a coupling proportional to the Stokes pulse, thus forming a parallel multi-\ensuremath{\Lambda} system. It is shown that the dark (trapped) state exists only when the ratio between each pump coupling and the respective Stokes coupling is the same for all intermediate states. We derive the conditions for existence of a more general adiabatic-transfer state that includes transient contributions from the intermediate states but still transfers the population from state ${\ensuremath{\psi}}_{i}$ to state ${\ensuremath{\psi}}_{f}$ in the adiabatic limit. We present various numerical examples for success and failure of multi-\ensuremath{\Lambda} STIRAP, which illustrate the analytic predictions. Our results suggest that in the general case of arbitrary couplings, it is most appropriate to tune the pump and Stokes lasers either just below or just above all intermediate states.
STIRAP (stimulated Raman adiabatic passage) has proven to be an efficient and robust technique for transferring population in a three-level system without populating the intermediate state. Here we show that the counterintuitive pulse sequence in STIRAP, in which the Stokes pulse precedes the pump, emerges automatically from a variant of optimal control theory we have previously called ``local'' optimization. Since local optimization is a well-defined, automated computational procedure, this opens the door to automated computation of generalized STIRAP schemes in arbitrarily complicated NNN-level coupling situations. If the coupling is sequential, a simple qualitative extension of STIRAP emerges: the Stokes pulse precedes the pump as in the three-level system. But, in addition, spanning both the Stokes and pump pulses are pulses corresponding to the transitions between the $N\ensuremath{-}2$ intermediate states with intensities about an order of magnitude greater than those of the Stokes and pump pulses. This scheme is amazingly robust, leading to almost 100% population transfer with significantly less population transfer to the $N\ensuremath{-}2$ intermediate states than in previously proposed extensions of STIRAP.
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.