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 (12)

• Laser-induced alignment and orientation of quantum-state-selected large molecules
• Molecular Orientation by Intense Single Cycle THz Pulses
• Manipulation of Molecules with Electromagnetic Fields
• Field-free orientation of CO molecules by femtosecond two-color laser fields
• Oriented rotational wave-packet dynamics studies via high harmonic generation
• Nonlinear two-dimensional terahertz photon echo and rotational spectroscopy in the gas phase
• Effects of ultrafast molecular rotation on collisional decoherence
• Rotational control of asymmetric molecules: dipole- vs. polarizability- driven rotational dynamics
• Field-free molecular orientation by THz laser pulses at high temperature
• Orientation of molecules via laser-induced anti-alignment
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Cited by in corpus (18)

• Quantum control of molecular rotation
• Strong Coupling of Light to Collective Terahertz Vibrations in Organic Materials
• Orienting Asymmetric Molecules by Laser Fields with Skewed Polarization
• Echo Spectroscopy in multi-level quantum-mechanical rotors
• Observing collisions beyond the secular approximation limit
• Long-lasting Molecular Orientation Induced by a Single Terahertz Pulse
• Control of photodissociation with dynamic Stark effect induced by Thz pulses
• Enantioselective Orientation of Chiral Molecules Induced by Terahertz Pulses with Twisted Polarization
• Giant Polarization Drag in a Gas of Molecular Superrotors
• Molecular alignment echoes probe collision-induced rotational-speed changes
• Shaping of the time-evolution of field-free molecular orientation by THz laser pulses
• Three Dimensional Orientation of Complex Molecules Excited by Two-Color Femtosecond Pulses
• Molecular Orientation-Induced Second Harmonic Generation: deciphering different contributions apart
• Intrinsic Calibration of Molecular Alignment Using Rotational Echoes
• Orientation Echoes via Concerted Terahertz and Near-IR excitation
• Optimal Selective Orientation of Chiral Molecules Using Femtosecond Laser Pulses
• Probing rotational decoherence with a trapped-ion planar rotor
• Rotational Coherence of Encapsulated Ortho and Para Water in Fullerene-C60