SearcharxivSearch

arXiv · 1710.04474

Signatures of electronic structure in bi-circular high-harmonic spectroscopy

Abstract

High-harmonic spectroscopy driven by circularly-polarized laser pulses and their counter-rotating second harmonic is a new branch of attosecond science which currently lacks quantitative interpretations. We extend this technique to the mid-infrared regime and record detailed high-harmonic spectra of several rare-gas atoms. These results are compared with the solution of the Schrodinger equation in three dimensions and calculations based on the strong-field approximation that incorporate accurate scattering-wave recombination matrix elements. A quantum-orbit analysis of these results provides a transparent interpretation of the measured intensity ratios of symmetry-allowed neighboring harmonics in terms of (i) a set of propensity rules related to the angular momentum of the atomic orbitals, (ii) atom-specific matrix elements related to their electronic structure and (iii) the interference of the emissions associated with electrons in orbitals co- or counter-rotating with the laser fields. These results provide the foundation for a quantitative understanding of bi-circular high-harmonic spectroscopy.

Explore related subjects

Keep this discovery

Explore connections, maps & timelines

BibTeXRIS

Denitsa Baykusheva, Simon Brennecke, Manfred Lein, Hans Jakob Wörner. 2017-10-12. Signatures of electronic structure in bi-circular high-harmonic spectroscopy. https://doi.org/10.1103/physrevlett.119.203201

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related papers

Delay-engineered dynamical phases in a programmable non-Markovian spin oscillator

Non-Markovian dynamics offer a new route towards engineering non-equilibrium matter, where memory and feedback act as programmable resources for controlling order in time. Here we report the realization of a non-Markovian spin oscillator in a hot vapour $^{129}$Xe-Cs co-magnetometer with programmable feedback delay and gain. By tuning these parameters, we observe a hierarchy of dynamical phases, including time-crystalline response, nonlinear bifurcations, and frequency-comb formation. The measured spectra and phase boundaries are captured by linear stability analysis of delayed Bloch equations, revealing these phenomena as different manifestations of the same memory-induced instability structure. These results establish time-delayed feedback as a powerful strategy for controlling non-equilibrium phases, enabling quantum sensing, frequency referencing, and synchronization within a single spin-based platform.

physics.atom-ph

Non-stick vacuum wall collisions with a laser-coolable molecule

Molecular species that are suitable for direct laser cooling are typically considered lost or destroyed if they collide with an ambient temperature vacuum wall. Here, we study surface collisions with aluminum monofluoride (AlF), a laser-coolable molecule that survives this process with unusually high probability. We detect the outgoing AlF molecules from a single wall collision via Doppler-sensitive laser-induced fluorescence spectroscopy, using incoming supersonic (pulsed) and thermochemical (continuous) molecular beams. The angular, velocity and rovibrational level distributions of the outgoing molecules show near-complete thermalisation to the wall in a single collision event. We determine an upper limit to the surface residence time of about 5$~\mu$s, and by monitoring the decay in density of pulses of molecules loaded into a small storage volume, we deduce the surface sticking probability for different materials. For a siloxane-coated metallic surface, the sticking probability of AlF is about 0.015, allowing us to accumulate molecules from the thermochemical source into an ambient temperature storage vessel at densities near $10^{8}~$cm$^{-3}$. This provides a route to compact, portable traps for neutral molecules.

physics.atom-ph

Kinetic modeling of molecular beam formation in a cryogenic buffer-gas cell

Cryogenic buffer-gas cells are widely used to produce cold molecular beams, but the microscopic dynamics governing beam formation remain challenging to model. Here we present fully kinetic simulations of a cryogenic buffer-gas cell using the Direct Simulation Monte Carlo method implemented in the PICLas framework, treating the buffer gas and ablated molecules within a single unified model. We capture characteristic features of cryogenic buffer-gas sources, including plume cooling, directed transport toward the aperture, and the formation of a slow molecular beam, while also resolving energy transfer from the hot ablation plume to the helium buffer gas that is inaccessible to existing approaches relying on the background-gas approximation. Our results demonstrate that fully kinetic simulations can provide detailed insights into buffer-gas cell dynamics and open a route toward a systematic optimization of such sources.

physics.atom-ph