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Chemical Physics

Raman excitation of rovibrational coherent and incoherent states via adiabatic passage assisted by dynamic Stark effect

Bo Y. Chang, Ignacio R. Solá

Published Jun 21, 2007• 3 citations
Publisher
DOI
10.1016/j.chemphys.2007.05.033

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Preparation of Vibrationally Excited H2_{\mathrm{2}}2​ in a Coherent Superposition of MMM-States Using Stark Induced Adiabatic Raman Passage (SARP)
By using Stark-induced adiabatic Raman passage (SARP) with partially overlapping nanosecond pump (532 nm) and Stokes (683 nm) laser pulses, 73% ± 6% of the initial ground vibrational state population of H(2) (v = 0, J = 0) is transferred to the single vibrationally excited eigenstate (v = 1, J = 0). In contrast to other Stark chirped Raman adiabatic passage techniques, SARP transfers population from the initial ground state to a vibrationally excited target state of the ground electronic surface without using an intermediate vibronic resonance within an upper electronic state. Parallel linearly polarized, co-propagating pump and Stokes laser pulses of respective durations 6 ns and 4.5 ns, are combined with a relative delay of ~4 ns before orthogonally intersecting the molecular beam of H(2). The pump and Stokes laser pulses have fluences of ~10 J/mm(2) and ~1 J/mm(2), respectively. The intense pump pulse generates the necessary sweeping of the Raman resonance frequency by ac (second-order) Stark shifting the rovibrational levels. As the frequency of the v = 0 → v = 1 Raman transition is swept through resonance in the presence of the strong pump and the weaker delayed Stokes pulses, the population of (v = 0, J = 0) is coherently transferred via an adiabatic passage to (v = 1, J = 0). A quantitative measure of the population transferred to the target state is obtained from the depletion of the ground-state population using 2 + 1 resonance enhanced multiphoton ionization (REMPI) in a time-of-flight mass spectrometer. The depletion is measured by comparing the REMPI signal of (v = 0, J = 0) at Raman resonance with that obtained when the Stokes pulse is detuned from the Stark-shifted Raman resonance. No depletion is observed with either the pump or the Stokes pulses alone, confirming that the measured depletion is indeed caused by the SARP-induced population transfer from the ground to the target state and not by the loss of molecules from photoionization or photodissociation. The two-photon resonant UV pulse used for REMPI detection is delayed by 20 ns with respect to the pump pulse to avoid the ac Stark shift originating from the pump and Stokes laser pulses. This experiment demonstrates the feasibility of preparing a large ensemble of isolated molecules in a preselected single quantum state without requiring an intermediate vibronic resonance.
Stark-chirped rapid adiabatic passage [T. Rickes et al., J. Chem. Phys. 113, 534 (2000); A. A. Rangelov et al. Phys. Rev. A 72, 053403 (2005)] has been proposed as a laser scheme that allows the optical excitation of atoms or molecules with high quantum yields. The laser control proceeds via adiabatic passage assisted by dynamic Stark shifts. We propose several extensions of the scheme with alternative sequences, by frequency tuning or by repeating the pulse sequences, in order to achieve fine state selectivity within multilevel structures and adiabatic passage of quantum superposition states. The efficiency and selectivity of the schemes is compared with that achieved by other optical coherent methods.