Observation of Dynamic Stark Resonances in Strong-Field Excitation

TL;DR

This study explores AC Stark-shifted resonances in argon under strong near-infrared fields, revealing how pulse duration and volume effects influence excitation enhancements and state selectivity.

Contribution

It demonstrates the dependence of Stark resonance enhancements on pulse duration, frequency, and intensity, supported by experimental and numerical analysis, highlighting the role of selectivity in strong-field excitation.

Findings

Enhancements occur at 13 and 14 photon absorption regions.

Shorter pulses reduce resonance enhancements due to bandwidth effects.

Volume averaging diminishes state selectivity and enhancement magnitude.

Abstract

We investigate AC Stark-shifted resonances in argon with ultrashort near-infrared pulses. Using 30 fs pulses we observe periodic enhancements of the excitation yield in the intensity regions corresponding to the absorption of 13 and 14 photons. By reducing the pulse duration to 6 fs with only a few optical cycles, we also demonstrate that the enhancements are significantly reduced beyond what is measurable in the experiment. Comparing these to numerical predictions, which are in quantitative agreement with experimental results, we find that even though the quantum-state distribution can be broad, the enhancements are largely due to efficient population of a select few AC Stark-shifted resonant states rather than the closing of an ionization channel. Because these resonances are dependent on the frequency and intensity of the laser field, the broad bandwidth of the 6 fs pulses means that the resonance condition is fulfilled across a large range of intensities. This is further exaggerated by volume-averaging effects, resulting in excitation of the $5g$ state at almost all intensities and reducing the apparent magnitude of the enhancements. For 30 fs pulses, volume averaging also broadens the quantum state distribution but the enhancements are still large enough to survive. In this case, selectivity of excitation to a single state is reduced below 25% of the relative population. However, an analysis of TDSE simulations indicates that excitation of up to 60% into a single state is possible if volume averaging can be eliminated and the intensity can be precisely controlled.