Cluster size dependence of high-order harmonic generation

TL;DR

This study examines how the size of noble gas clusters influences high-order harmonic generation, revealing enhanced single-atom responses for small clusters and implications for optimizing harmonic yield.

Contribution

It provides the first detailed analysis of cluster size effects on HHG, considering liquid mass fraction variations and demonstrating enhancement for small clusters (~200 atoms).

Findings

Harmonic emission increases when average cluster size is less than 3000.

Single-atom response is enhanced by about 10 times in very small clusters (~200).

No dependence of cut-off frequency on cluster composition was observed.

Abstract

We investigate high-order harmonic generation (HHG) from noble gas clusters in a supersonic gas jet. To identify the contribution of harmonic generation from clusters versus that from gas monomers, we measure the high-order harmonic output over a broad range of the total atomic number density in the jet (from 3*10^16 cm^{-3} to 3x10^18 cm{-3}) at two different reservoir temperatures (303 K and 363 K). For the firrst time in the evaluation of the harmonic yield in such measurements, the variation of the liquid mass fraction, g, versus pressure and temperature is taken into consideration, which we determine, reliably and consistently, to be below 20% within our range of experimental parameters. By comparing the measured harmonic yield from a thin jet with the calculated corresponding yield from monomers alone, we find an increased emission of the harmonics when the average cluster size is less than 3000. Using g, under the assumption that the emission from monomers and clusters add up coherently, we calculate the ratio of the average single-atom response of an atom within a cluster to that of a monomer and find an enhancement of around 10 for very small average cluster size (~200). We do not find any dependence of the cut-off frequency on the composition of the cluster jet. This implies that HHG in clusters is based on electrons that return to their parent ions and not to neighbouring ions in the cluster. To fully employ the enhanced average single-atom response found for small average cluster sizes (~200), the nozzle producing the cluster jet must provide a large liquid mass fraction at these small cluster sizes for increasing the harmonic yield. Moreover, cluster jets may allow for quasi-phase matching, as the higher mass of clusters allows for a higher density contrast in spatially structuring the nonlinear medium.