Abstract
High-order harmonic generation in an atomic or molecular gas is a promising source of sub-femtosecond vacuum ultraviolet coherent radiation for transient scattering, absorption, metrology and imaging applications. High harmonic spectra are sensitive to Ångstrom-scale structure and motion of laser-driven molecules, but interference from radiation produced by random molecular orientations obscures this in all but the simplest cases, such as linear molecules. Here we show how to extract full body-frame high harmonic generation information for molecules with more complicated geometries by utilizing the methods of coherent transient rotational spectroscopy. To demonstrate this approach, we obtain the relative strength of harmonic emission along the three principal axes in the asymmetric-top sulphur dioxide. This greatly simplifies the analysis task of high harmonic spectroscopy and extends its usefulness to more complex molecules.
| Original language | English (US) |
|---|---|
| Article number | 3190 |
| Journal | Nature communications |
| Volume | 5 |
| DOIs | |
| State | Published - Feb 7 2014 |
Funding
We would like to acknowledge fruitful discussions with Varun Makhija, Xiaoming Ren, Adi Natan, Brian K. McFarland, Song Wang and Joseph P. Farrell. This research is supported through the Chemical Sciences Division of the SLAC National Accelerator Laboratory by the US Department of Energy, Office of Basic Energy Sciences and by a US Department of Energy award (Grant No. DE-FG02-04ER15612). We acknowledge support from a National Defense Science and Engineering Graduate Fellowship (L.S.S.), a Stanford Diversifying Academia, Recruiting Excellence Graduate Fellowship (L.S.S.) and an Office of Science Early Career Research Program Grant (M.G.).
ASJC Scopus subject areas
- General Chemistry
- General Biochemistry, Genetics and Molecular Biology
- General Physics and Astronomy