An optical centrifuge made from shaped laser pulses with field intensities more than 1013 W/cm2 is used to excite molecules such as CO2, N2O and CO with large amounts of rotational energy and oriented angular momentum. Polarization-dependent, high-resolution transient IR spectroscopy measures the rotational, translational and vibrational energies of the centrifuged molecules and characterizes the orientational anisotropy, translational energy distributions and relaxation dynamics. For CO, additional strong-field pathways are seen at higher field intensities as evidenced by laser-induced plasma filaments and C2 Swan band emission. Differences are observed based on the elliptical or circular polarization of shaped pulses. Results will be discussed in terms of the rotational trajectories of molecules in angularly accelerating fields.

Molecules in extreme rotational states made with strong optical fields: Transient spectroscopy of high-J molecules made in an optical centrifuge

256th National Meeting (2018)

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