Coherent radiative decay of molecular rotations: a comparative study of terahertz-oriented versus optically aligned molecular ensembles

Abstract

The decay of field-free rotational dynamics is experimentally studied in two complementary methods: laser-induced molecular alignment and terahertz-field-induced molecular orientation. Comparison between the decay rates of different molecular species at various gas pressures reveals that oriented molecular ensembles decay faster than aligned ensembles. The discrepancy in decay rates is attributed to the coherent radiation emitted by the transiently oriented ensembles and is absent from aligned molecules. The experimental results reveal the dramatic contribution of coherent radiative emission to the observed decay of rotational dynamics and underline a general phenomenon expected whenever field-free coherent dipole oscillations are induced.

References in corpus (4)

• Laser-induced alignment and orientation of quantum-state-selected large molecules
• Field-free orientation of CO molecules by femtosecond two-color laser fields
• Effects of ultrafast molecular rotation on collisional decoherence
• On the observation of field-free orientation of a symmetric top molecule by terahertz laser pulses at high temperature

Cited by in corpus (4)

• Enantioselective Orientation of Chiral Molecules Induced by Terahertz Pulses with Twisted Polarization
• Giant Polarization Drag in a Gas of Molecular Superrotors
• Shaping of the time-evolution of field-free molecular orientation by THz laser pulses
• Rotational Coherence of Encapsulated Ortho and Para Water in Fullerene-C60