We present an experimental technique using orbital angular momentum (OAM) in a fundamental laser field to drive High Harmonic Generation (HHG). The mixing of beams with different OAM allows to generate two laser foci tightly spaced to study the phase and amplitude of HHG produced in diatomic nitrogen. Nitrogen is used as a well studied system to show the quality of OAM based HHG interferometry.
Optical vortices are currently one of the most intensively studied topics in optics. These light beams, which carry orbital angular momentum (OAM), have been successfully utilized in the visible and infrared in a wide variety of applications. Moving to shorter wavelengths may open up completely new research directions in the areas of optical physics and material characterization. Here, we report on the generation of extreme-ultraviolet optical vortices with femtosecond duration carrying a controllable amount of OAM. From a basic physics viewpoint, our results help to resolve key questions such as the conservation of angular momentum in highly-nonlinear light-matter interactions, and the disentanglement and independent control of the intrinsic and extrinsic components of the photons angular momentum at short-wavelengths. The methods developed here will allow testing some of the recently proposed concepts such as OAM-induced dichroism, magnetic switching in organic molecules, and violation of dipolar selection rules in atoms.
We study theoretically and experimentally the electronic relaxation of NO2 molecules excited by absorption of one ~400 nm pump photon. Semi-classical simulations based on trajectory surface hopping calculations are performed. They predict fast oscillations of the electronic character around the intersection of the ground and first excited diabatic states. An experiment based on high-order harmonic transient grating spectroscopy reveals dynamics occuring on the same timescale. A systematic study of the detected transient is conducted to investigate the possible influence of the pump intensity, pump wavelength, and rotational temperature of the molecules. The quantitative agreement between measured and predicted dynamics shows that, in NO2, high harmonic transient grating spectroscopy encodes vibrational dynamics underlying the electronic relaxation.
The interplay between spin and orbital angular momentum in the up-conversion process allows us to control the macroscopic wave front of high harmonics by manipulating the microscopic polarizations of the driving field. We demonstrate control of orbital angular momentum in high harmonic generation from both solid and gas phase targets using the selection rules of spin angular momentum. The gas phase harmonics extend the control of angular momentum to extreme-ultraviolet wavelength. We also propose a bi-color scheme to produce spectrally separated extreme-ultraviolet radiation carrying orbital angular momentum.
We study the manipulation of slow light with an orbital angular momentum propagating in a cloud of cold atoms. Atoms are affected by four copropagating control laser beams in a double tripod configuration of the atomic energy levels involved, allowing to minimize the losses at the vortex core of the control beams. In such a situation the atomic medium is transparent for a pair of copropagating probe fields, leading to the creation of two-component (spinor) slow light. We study the interaction between the probe fields when two control beams carry optical vortices of opposite helicity. As a result, a transfer of the optical vortex takes place from the control to the probe fields without switching off and on the control beams. This feature is missing in a single tripod scheme where the optical vortex can be transferred from the control to the probe field only during either the storage or retrieval of light.
High-order harmonic generation in polyatomic molecules generally involves multiple channels, each associated with a different orbital. Their unambiguous assignment remains a major challenge for high-harmonic spectroscopy. Here we present a multi-modal approach, using unaligned SF$_6$ molecules as an example, where we combine methods from extreme-ultraviolet spectroscopy, above-threshold ionization and attosecond metrology. Channel-resolved above-threshold ionization measurements reveal that strong-field ionization opens four channels. Two of them, identified by monitoring the ellipticity dependence of the high-harmonic emission, are found to dominate the harmonic signal. A switch from the HOMO-3 to the HOMO-1 channel at 26 eV is confirmed by a phase jump in the harmonic emission, and by the differing dynamical responses to molecular vibrations. This study demonstrates a modus operandi for extending high-harmonic spectroscopy to polyatomic molecules, where complex attosecond dynamics are expected.