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Physical Review A

Stimulated Raman adiabatic passage through permanent dipole moment transitions

Ying‐Yu Niu, Rong Wang, Ming‐Hui Qiu

Published Apr 12, 2010• 7 citations
Publisher

Abstract

The rovibrational dynamics of stimulated Raman adiabatic passage (STIRAP) through permanent dipole moment transitions are investigated theoretically using a time-dependent quantum wave packet method for the ground electronic state of an HF molecule. The two basic STIRAP processes, $\ensuremath{\Lambda}$ and ladder systems, are simulated. The calculated results show that nearly $100%$ of the population can be transferred to the target state. Besides the interested transitions, the pulses can induce other transitions which affect the dynamics of STIRAP. The final populations of the initial and target states depend on delay time.

DOI
10.1103/physreva.81.043406

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Advances in Physical Chemistry•Dec 22, 2010•6 citations
The rovibrational dynamics of stimulated Raman adiabatic passage (STIRAP) through permanent dipole moment transitions are investigated theoretically using a time-dependent quantum wave packet method for the ground electronic state of an HF molecule. The two basic STIRAP processes, \ensuremathΛ\ensuremath{\Lambda}\ensuremathΛ and ladder systems, are simulated. The calculated results show that nearly 100100%100 of the population can be transferred to the target state. Besides the interested transitions, the pulses can induce other transitions which affect the dynamics of STIRAP. The final populations of the initial and target states depend on delay time.
The rovibrational dynamics of an extended ladder stimulated Raman adiabatic passage (STIRAP) system through permanent dipole moment transitions is investigated theoretically using the time-dependent quantum-wave-packet method for the ground electronic state of the HF molecule. The calculated results show that nearly 100% of the population can be transferred to the target state through (1+2), (1+3), and (2+2) STIRAP schemes. By choosing a suitable excitation pathway, the effects of the background states on the final population of the target state can be removed. For the multiphoton STIRAP process, the one-photon overtone pump scheme is more efficient than the two-photon pump scheme in controlling the population transfer to the target state.
We explore theoretically the rovibrational dynamics of stimulated Raman adiabatic passage (STIRAP) in molecular electronic states including both the rotational and the vibrational degrees of freedom, with the LiH molecule as an example. By using a pure rovibrational state as initial state, we find that, under the condition of two-photon resonance, an efficient rovibrational population transfer can be achieved via STIRAP in molecular electronic states and the desired target state can be selected by adjusting laser-pulse parameters. Besides the interested rovibrational states, however, some unwanted rovibrational states may affect population transfer process, especially while the two-photon detuning is taken into account. By inspecting the evolution process of wave packet, we can easily search these unwanted rovibrational states and study their influences. Moreover, the effect of rotational temperature on the population transfer process is discussed using thermal mixed state as initial state.
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.
This work explores the effect of phase relaxation on the population transfer efficiency in stimulated Raman adiabatic passage (STIRAP). The study is based on the Liouville equation, which is solved analytically in the adiabatic limit. The transfer efficiency of STIRAP is found to decrease exponentially with the dephasing rate; this effect is stronger for shorter pulse delays and weaker for larger delays, since the transition time is found to be inversely proportional to the pulse delay. Moreover, it is found that the transfer efficiency of STIRAP in the presence of dephasing does not depend on the peak Rabi frequencies at all, as long as they are sufficiently large to enforce adiabatic evolution; hence increasing the field intensity cannot reduce the dephasing losses. It is shown also that for any dephasing rate, the final populations of the initial state and the intermediate state are equal. For strong dephasing all three populations tend to 13\frac{1}{3}31​.
The technique of stimulated Raman adiabatic passage (STIRAP) is an efficient and robust technique for population transfer in three-state chain-wise connected quantum systems, 1-2-3. Here we analyze the transition time in STIRAP, that is the time it takes for the population to be transferred from state 1 to state 3. We derive a very simple formula for this transition time, which shows that it is inversely proportional to the nonadiabatic coupling $\mathrm{\ensuremath{\vartheta}\ifmmode \dot{}\else \.{}\fi{}}({t}_{c})$, estimated at the time tc{t}_{c}tc​ when the pump and Stokes couplings have the same value. Explicit formulas for several pulse shapes of the pump and Stokes fields are derived. Contrary to the naive expectation that the transition time might be proportional to the delay between the pump and Stokes pulses, or to the width of their overlap region, we find that the transition time is inversely proportional to the delay, i.e., larger delays produce faster transitions. We also calculate the transition time in two important variations of the STIRAP technique---bright-STIRAP and STIRAP in multistate systems---where similar features are found.
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.