title: Axis-dependence of molecular high harmonic emission in three dimensions.
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.
authors: 1] Applied Physics Department, 382 Via Pueblo Mall, Stanford University, Stanford, California 94305, USA [2] Stanford PULSE Institute, 2575 Sand Hill Road, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
authors: Limor S
authors: LS
authors: Spector
authors: Department of Chemistry, 2145 Sheridan Road, Northwestern University, Evanston, Illinois 60208, USA.
authors: Maxim
authors: M
authors: Artamonov
authors: 1] Stanford PULSE Institute, 2575 Sand Hill Road, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA [2] Chemistry Department, 333 Campus Drive, Stanford University, Stanford, California 94305, USA.
authors: Shungo
authors: S
authors: Miyabe
authors: 1] Stanford PULSE Institute, 2575 Sand Hill Road, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA [2] Chemistry Department, 333 Campus Drive, Stanford University, Stanford, California 94305, USA.
authors: Todd
authors: T
authors: Martinez
authors: Department of Chemistry, 2145 Sheridan Road, Northwestern University, Evanston, Illinois 60208, USA.
authors: Tamar
authors: T
authors: Seideman
authors: Stanford PULSE Institute, 2575 Sand Hill Road, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
authors: Markus
authors: M
authors: Guehr
authors: 1] Applied Physics Department, 382 Via Pueblo Mall, Stanford University, Stanford, California 94305, USA [2] Stanford PULSE Institute, 2575 Sand Hill Road, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
authors: Philip H
authors: PH
authors: Bucksbaum