Multiple pulse coherent dynamics and wave packet control of the N2 a'' 1 Σ dark state by attosecond four-wave mixing

Faraday Discussions
Erika R WarrickStephen R Leone

Abstract

Nonlinear multidimensional spectroscopy is ubiquitous in the optical and radio frequency regions as a powerful tool to access structure and dynamics. The extension of this technique into the extreme ultraviolet (XUV) region with attosecond pulses holds promise for probing electronic dynamics and correlations with unprecedented time and spatial resolution. In this work, we use noncollinear four-wave mixing of a weak XUV attosecond pulse train (11-17 eV) and few-femtosecond NIR pulses (800 nm) to spectroscopically and dynamically probe the dipole-forbidden double-well potential of the a'' 1∑+g electronic state of nitrogen. The results demonstrate optical coupling of the inner and outer limits of the initial XUV-prepared vibrational wave packet in the valence character b' 1∑+u state to the inner and outer wells, respectively, of the a'' 1∑+g double well state by 800 nm light. Two four-wave mixing schemes with different pulse timing sequences and noncollinear beam geometries are used (one NIR pulse collinear and one NIR pulse noncollinear versus both NIR pulses noncollinear to the XUV beam) to measure the a'' dark state energetic structure and to control the dynamical preparation and motion of a dark state wave packet by selective ...Continue Reading

References

Apr 1, 1991·Physical Review. a·A W Kam, F M Pipkin
Apr 6, 2001·Physical Review Letters·O GolonzkaA Tokmakoff
Oct 12, 2004·The Journal of Chemical Physics·D Cossart, C Cossart-Magos
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May 30, 2009·Science·Katherine W StoneKeith A Nelson
Dec 19, 2012·Annual Review of Physical Chemistry·Shaul MukamelJason D Biggs
Feb 11, 2016·The Journal of Physical Chemistry. a·Erika R WarrickStephen R Leone
Feb 13, 2016·Optics Letters·Thomas DingThomas Pfeifer
Oct 7, 2016·Faraday Discussions·Stephen R Leone, Daniel M Neumark

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Citations

Apr 2, 2019·Philosophical Transactions. Series A, Mathematical, Physical, and Engineering Sciences·Romain GeneauxStephen R Leone
Mar 29, 2019·Nature Communications·Ashley P FidlerStephen R Leone
Feb 16, 2020·Nature Communications·Andreas WituschekFrank Stienkemeier
Jan 18, 2022·Chemical Reviews·Somnath BiswasGregory D Scholes

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Methods Mentioned

BETA
X-ray

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