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The Journal of Chemical Physics

Selective photodissociation in diatomic molecules by dynamical Stark-shift control

Hyeonho Choi, Won‐Joon Son, Seokmin Shin, Bo Y. Chang, Ignacio R. Solá

Published Mar 13, 2008• 17 citations
Publisher

Abstract

Selective population transfer in electronic states of dissociative molecular systems is illustrated by adopting a control scheme based on Stark-chirped rapid adiabatic passage (SCRAP). In contrast to the discrete N-level system, dynamical Stark shift is induced in a more complex manner in the molecular electronic states. Wavepacket dynamics on the light-induced potentials, which are determined by the detuning of the pump pulse, can be controlled by additional Stark pulse in the SCRAP scheme. Complete population transfer can be achieved by either lowering the energy barrier along the adiabatic passage or placing the initial wavepacket on a well-defined dressed state suitable for the control. The determination of the pulse sequence is sufficient for controlling population transfer to the target state.

DOI
10.1063/1.2838911

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The Journal of Chemical Physics•Nov 14, 2002•15 citations
Selective population transfer in electronic states of dissociative molecular systems is illustrated by adopting a control scheme based on Stark-chirped rapid adiabatic passage (SCRAP). In contrast to the discrete N-level system, dynamical Stark shift is induced in a more complex manner in the molecular electronic states. Wavepacket dynamics on the light-induced potentials, which are determined by the detuning of the pump pulse, can be controlled by additional Stark pulse in the SCRAP scheme. Complete population transfer can be achieved by either lowering the energy barrier along the adiabatic passage or placing the initial wavepacket on a well-defined dressed state suitable for the control. The determination of the pulse sequence is sufficient for controlling population transfer to the target state.
We present the experimental demonstration of a novel, efficient, and selective technique to prepare population inversion. The technique is an extension of Stark-chirped rapid adiabatic passage (SCRAP), i.e., SCRAP among three states. In this process a Lambda-type quantum system is driven by two laser pulses, the pump and Stokes pulses, which are appropriately detuned from transition frequencies. A third laser pulse induces a dynamic Stark shift in the upper energy level, and the timing of all three pulses is controlled in order to prepare population inversion between the two lower states in the Lambda-type level scheme. Our data on population transfer in nitric oxide (NO) molecules clearly show that SCRAP among three states provides an advantageous alternative to such techniques as stimulated Raman adiabatic passage.
We show that the technique of Stark-chirped rapid adiabatic passage (SCRAP), hitherto used for complete population transfer between two quantum states, offers a simple and robust method for complete population transfer amongst three states in atoms and molecules. In this case SCRAP uses three laser pulses: a strong far-off-resonant pulse modifies the transition frequencies by inducing dynamic Stark shifts and thereby creating time-dependent level crossings amongst the three diabatic states, while near-resonant and moderately strong pump and Stokes pulses, appropriately offset in time, drive the population between the initial and final states via adiabatic passage. The population transfer efficiency is robust to variations in the intensities of the lasers, as long as these intensities are sufficiently large to enforce adiabatic evolution. With suitable pulse timings the population in the (possibly decaying) intermediate state can be minimized, as with stimulated Raman adiabatic passage (STIRAP). This technique applies to one-photon as well as multiphoton transitions and it is also applicable to media exhibiting inhomogeneous broadening; these features represent clear advantages over STIRAP by overcoming the inevitable dynamical Stark shifts that accompany multiphoton transitions as well as unwanted detunings, e.g., induced by Doppler shifts.
We present extended experimental investigations and numerical studies on coherently driven population inversion in a three-state molecular quantum system by sequential double-Stark-chirped rapid adiabatic passage (SCRAP) (D-SCRAP) and three-state-SCRAP (T-SCRAP). D-SCRAP and T-SCRAP are alternative extensions of SCRAP. In D-SCRAP and T-SCRAP, a $\ensuremath{\Lambda}$-type quantum system is coherently driven by two laser pulses, the pump and Stokes pulses, which are slightly detuned from transition frequencies. A third strong laser pulse induces dynamic Stark shifts of the relevant transitions. If the timing of the three pulses is appropriately chosen, the quantum system is prepared to almost complete population inversion between the two lower states in the $\ensuremath{\Lambda}$-type level scheme. The transfer process is robust with regard to fluctuations of experimental parameters, provided some limitations are met. The paper presents convincing experimental data on D-SCRAP and T-SCRAP, driving efficient and selective population transfer to a highly excited vibrational level in nitrous oxide (NO) molecules. T-SCRAP yields transfer efficiencies of up to 95%. The efficiency of T-SCRAP is almost uneffected by the limited lifetime of the intermediate state in the $\ensuremath{\Lambda}$ system. The paper also presents data on the accurate experimental determination of Rabi frequencies and Stark shifts. This involves measurements of power broadening, Autler-Townes splittings, and Stark-shifted spectral lines in NO molecules. Moreover, we discuss the calibration of absolute transfer efficiences by comparison with stimulated emission pumping. The experimental data are confirmed by extended numerical simulations. The simulations also serve to intensively study the properties and dynamics of D-SCRAP and T-SCRAP.
We demonstrate and analyze a novel scheme for complete transfer of atomic or molecular population between two bound states, by means of Stark-chirped rapid adiabatic passage (SCRAP). In this two-laser technique a delayed-pulse laser-induced Stark shift sweeps the transition frequency between two coupled states twice through resonance with the frequency of the population-transferring coupling laser. The delay of the Stark-shifting pulse with respect to the pulse of the coupling-laser Rabi frequency guarantees adiabatic passage of population at one of the two resonances while the evolution is diabatic at the other. The SCRAP method can give a population-transfer efficiency approaching unity. We discuss the general requirements on the intensity and timing of the pulses that produce the Rabi frequency and, independently, the Stark shift. We particularly stress extension to a double-SCRAP technique, a coherent variant of stimulated emission pumping in the limit of strong saturation. We demonstrate the success of the SCRAP method with experiments in metastable helium, where a two-photon transition provides the Rabi frequency.
The stark-chirped rapid adiabatic passage (SCRAP) is analyzed, which can give a complete transfer of atomic or molecular population between two bound states in the two level states and Λ(-three)-level state, by means of level-crossing technique and dressed states theory. SCRAP uses two laser pulses: a nearly-resonant pump laser pulse drives the population between a ground state and an excited state, and an intense far-off-resonance Stark laser pulse modifies the transition frequency and resonates with the Bohr transition frequency for two level crossings. A population-transfer maximal efficiency approaching unity is provided from the ground state to the excited state, when the delay of the Stark-shifting pulse with respect to the pulse of the coupling-laser frequency is appropriate and guarantees the pump pulse is strong at one of these crossings and is weak at second one.
A new scheme of controlling molecular processes by a sequence of linearly chirped pulses is proposed and is applied to selective excitation of an energy level among closely lying ones and to complete electronic excitation of a diatomic molecule. The basic idea is quite different from the conventional ones utilizing chirped pulses in the sense that the present one does not rely on the idea of adiabatic rapid passage at all, but tries to control basic nonadiabatic transitions explicitly. Control of molecular processes can be achieved by controlling nonadiabatic transitions among Floquet (or dressed) states with use of the interference effects. The scheme can be formulated with use of the analytical theories of nonadiabatic transitions, and the proper control parameters can be estimated theoretically. Numerical demonstrations are provided to confirm the robustness of the method in comparison with the other conventional ones. Namely, the present scheme is shown to be stable against the variation of pulse area, complete and selective in population transfer, and fast to accomplish the transition. It is expected that the method can be applied to general multilevel systems and various types of wave packet dynamics. Its experimental realizability can also be expected, since linear chirping can now be relatively easily realized and manipulated.