0000000000523737
AUTHOR
Ilya Sh. Averbukh
Orientation and Alignment Echoes
We present one of the simplest classical systems featuring the echo phenomenon---a collection of randomly oriented free rotors with dispersed rotational velocities. Following excitation by a pair of time-delayed impulsive kicks, the mean orientation or alignment of the ensemble exhibits multiple echoes and fractional echoes. We elucidate the mechanism of the echo formation by the kick-induced filamentation of phase space, and provide the first experimental demonstration of classical alignment echoes in a thermal gas of ${\mathrm{CO}}_{2}$ molecules excited by a pair of femtosecond laser pulses.
Visualizing coherent molecular rotation in a gaseous medium
Inducing and controlling the ultrafast molecular rotational dynamics using shaped laser fields is essential in numerous applications. Several approaches exist that allow following the coherent molecular motion in real-time, including Coulomb explosion-based techniques and recovering molecular orientation from the angular distribution of high harmonics. We theoretically consider a non-intrusive optical scheme for visualizing the rotational dynamics in an anisotropic molecular gas. The proposed method allows determining the instantaneous orientation of the principal optical axes of the gas. The method is based on probing the sample using ultra-short circularly polarized laser pulses and recor…
Optical Imaging of Coherent Molecular Rotors
International audience; 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 b…
Rotational echoes as a tool for investigating ultrafast collisional dynamics of molecules
We show that recently discovered rotational echoes of molecules provide an efficient tool for studying collisional molecular dynamics in high-pressure gases. Our study demonstrates that rotational echoes enable the observation of extremely fast collisional dissipation, at timescales of the order of a few picoseconds, and possibly shorter. The decay of the rotational alignment echoes in ${\mathrm{CO}}_{2}$ gas and ${\mathrm{CO}}_{2}\text{\ensuremath{-}}\mathrm{He}$ mixture up to 50 bar was studied experimentally, delivering collision rates that are in good agreement with the theoretical expectations. The suggested measurement protocol may be used in other high-density media, and potentially …
Spatiotemporal rotational dynamics of laser-driven molecules
Molecular alignment and orientation by laser fields has attracted significant attention in recent years, mostly due to new capabilities to manipulate the molecular spatial arrangement. Molecules can now be efficiently prepared for ionization, structural imaging, orbital tomography, and more, enabling, for example, shooting of dynamic molecular movies. Furthermore, molecular alignment and orientation processes give rise to fundamental quantum and classical phenomena like quantum revivals, Anderson localization, and rotational echoes, just to mention a few. We review recent progress on the visualization, coherent control, and applications of the rich dynamics of molecular rotational wave pack…