Optical imaging of coherent molecular rotors

Abstract

Short laser pulses are widely used for controlling molecular rotational degrees of freedom and inducing molecular alignment, orientation, unidirectional rotation and other types of coherent rotational motion. To follow the ultra-fast rotational dynamics in real time, several techniques for producing molecular movies have been proposed based on the Coulomb explosion of rotating molecules, or recovering molecular orientation from the angular distribution of high-harmonics. The present work offers and demonstrates a novel non-destructive optical method for direct visualization and recording of movies of coherent rotational dynamics in a molecular gas. The technique is based on imaging the time-dependent polarization dynamics of a probe light propagating through a gas of coherently rotating molecules. The probe pulse continues through a radial polarizer, and is then recorded by a camera. We illustrate the technique by implementing it with two examples of time-resolved rotational dynamics: alignment-antialignment cycles in a molecular gas excited by a single linearly polarized laser pulse, and unidirectional molecular rotation induced by a pulse with twisted polarization. This method may open new avenues in studies on fast chemical transformation phenomena and ultrafast molecular dynamics caused by strong laser fields of various complexities.

References in corpus (10)

• Molecular Orientation by Intense Single Cycle THz Pulses
• Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules
• Observing Molecular Spinning via the Rotational Doppler Effect
• Controlling the sense of molecular rotation
• Control of molecular rotation with a chiral train of ultrashort pulses
• Molecular movie of ultrafast coherent rotational dynamics
• Molecular rotation movie filmed with high-harmonic generation
• Visualizing molecular unidirectional rotation
• Controlling the sense of molecular rotation: classical vs quantum analysis
• Orienting Asymmetric Molecules by Laser Fields with Skewed Polarization

Cited by in corpus (6)

• Bayesian optimization for inverse problems in time-dependent quantum dynamics
• Echoes in Unidirectionally Rotating Molecules
• Rotation of polarization of light propagating through a gas of molecular super-rotors
• Topological charges of periodically kicked molecules
• Orientation Echoes via Concerted Terahertz and Near-IR excitation
• Visualizing coherent molecular rotation in a gaseous medium