DOE OSTI · 3003085
Optical interference effect in strong-field electronic coherence spectroscopy
Abstract
Here, we investigate strong-field-induced electronic coherences in argon and molecular nitrogen ions created by high-intensity, few-cycle infrared laser pulses. This is a step toward the long-sought goal of strong-field coherent control in molecular chemistry. We employ high-intensity, few-cycle infrared laser pulses in a pump-probe setup to investigate a recent prediction that electronic coherences in nitrogen molecules change the ion yields versus pump-probe delay. [Yuen et al., Phys. Rev. A 109, L011101 (2024)]. The predicted coherence signals in molecular nitrogen could not be resolved above the optical interference of the pump and probe pulses; a simultaneous measurement clearly resolved the induced cation fine-structure coherence in strong-field-ionized argon. The results of our comparison with simulations suggest that optical interference effects manifest differently in each ionic species and must be carefully accounted for when interpreting experimental data. We find that nonsequential double ionization in the low-intensity region of the focal volume can reduce the visibility of coherence generated by two-pulse sequential ionization, and we quantify the importance of pulse shape and spectral characteristics for isolating the desired coherence signals.
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Weckwerth, Eleanor [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)] (ORCID:0009000910036481), Howard, Andrew J. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)] (ORCID:0000000303033222), Cheng, Chuan [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)] (ORCID:0000000280947047), Gabalski, Ian [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)] (ORCID:0000000267826566), Ghrist, Aaron M. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)] (ORCID:0000000321969278), Mohideen, Salma A. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)], Lin, Chii-Dong [Kansas State Univ., Manhattan, KS (United States)] (ORCID:0000000348478938), Yuen, Chi-Hong [Kansas State Univ., Manhattan, KS (United States); Kennesaw State University, Marietta, GA (United States)] (ORCID:0000000205444976), Bucksbaum, Philip H. [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford Univ., CA (United States)] (ORCID:0000000312585571). 2025-10-14. Optical interference effect in strong-field electronic coherence spectroscopy. https://doi.org/10.1103/rkdq-5skq
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