Molecular Orientation-Induced Second-Harmonic Generation: Deciphering Different Contributions Apart

Amit Beer, Ran Damari, Yun Chen, Sharly Fleischer*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review


We demonstrate and explore an all-optical technique for direct monitoring of the orientation dynamics in gas-phase molecular ensembles. The technique termed "MOISH"utilizes the transiently lifted inversion symmetry of polar gas media and provides a sensitive and spatially localized probing of the second-harmonic generation signal that is directly correlated with the orientation of the gas. Our experimental results reveal selective electronic and nuclear dynamical contributions to the overall nonlinear optical signal and decipher them apart using the "reporter gas"approach. "MOISH"provides new crucial means for implementing advanced coherent rotational control via concerted excitation by both terahertz and optical fields.

Original languageEnglish
Pages (from-to)3732-3738
Number of pages7
JournalJournal of Physical Chemistry A
Issue number23
StatePublished - 16 Jun 2022


FundersFunder number
Wolfson FoundationPR/ec/20419
Israel Science Foundation926/18


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