0000000000627593
AUTHOR
Emilien Prost
Ultrafast optics in coherently spinning molecules
This thesis reports on the study of unidirectional rotation of molecules and focuses on the rotational Doppler effect occuring in the course of third-harmonic generation in coherently spinning molecules.The rotational Doppler effect appears when a circularly polarized wave interacts with an anisotropic rotating object. During the interaction, an exchange of angular momentum and energy between the field and the object occurs, leading to a frequency shift of the wave. In this work, the frequency shift of the third-harmonic generated in unidirectionaly rotating molecules has been observed. An anlytical model developped in the mansucript forsees four kinds of frequency shifts depending on the m…
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…