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Time-resolved spectroscopy of the dynamic Stark effect

Lookup NU author(s): Dr Gareth Roberts


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This study reports on the ac Stark effect of nitric oxide electron-vibration (vibronic) levels dressed by an intense, bichromatic laser field. The aims of the work are to make quantitative measurements of the magnitude of the ac Stark shift of vibrational levels connected by the A 2Σ+ ← X2Π1/2 transition and to map out the cycle-averaged level separation during the Stark field. In pump-probe experiments at intensities up to 30 TW cm-2, the ac Stark shift of the A2Σ+ vA = 2 ← X2Π1/2 vX = 0 transition is found to be Δε2←0(S)(800nm) = 0.34 ± 0.05Up, where Up is the ponderomotive energy. By varying the time delay between component fields, the time dependence of the population in the A2Σ+ vA = 2 state is mapped out under different intensity conditions. Fluorescence monitoring of the upper level serves to identify the Stark-shifted transition and reveals that real population remains in the upper level after interacting with the short-pulse laser fields. Semiclassical calculations of NO irradiated by a bichromatic field indicate the direction of the A2Σ+ and X 2Π1/2 level shifts and show that the population promoted to and retained in the A2Σ+ state is determined predominantly by intra-Rydberg state interactions rather than by multiphoton loss processes. The calculations also indicate that the magnitude of the ac Stark effect of the A2Σ+ ← X 2Π1/2 transition depends on the spatial orientation of the molecule with respect to the linear polarization sense of the applied laser field.

Publication metadata

Author(s): Schmidt TW, Lopez-Martens RB, Roberts G

Publication type: Article

Publication status: Published

Journal: Journal of Physics B: Atomic, Molecular and Optical Physics

Year: 2004

Volume: 37

Issue: 5

Pages: 1125-1140

ISSN (print): 0953-4075

ISSN (electronic): 1361-6455

Publisher: Institute of Physics Publishing Ltd


DOI: 10.1088/0953-4075/37/5/015


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