Tracing spatial confinement in semiconductor quantum dots by high-order harmonic generation

TL;DR

This study investigates how quantum dot size affects high-order harmonic generation, revealing size-dependent suppression of certain harmonics due to electron scattering and confinement effects, highlighting a new laser-solid interaction regime.

Contribution

It provides the first detailed analysis of HHG suppression mechanisms in semiconductor quantum dots of varying sizes, bridging bulk and molecular responses.

Findings

HHG efficiency decreases with smaller quantum dots.

Suppression of above bandgap harmonics increases with driving wavelength.

Quantum confinement and scattering limit electron acceleration and coherence.

Abstract

We report here on results of experimental-theoretical investigation of high-order harmonic generation (HHG) in layers of CdSe semiconductor quantum dots of different sizes and a reference bulk CdSe thin film. We observe a strong decrease in the efficiency, up to complete suppression of HHG with energies of quanta above the bandgap for the smallest dots, whereas the intensity of below bandgap harmonics remains weakly affected by the dot size. In addition, it is observed that the ratio between suppression of above gap harmonics versus below gap harmonics increases with driving wavelength. We suggest that the reduction in the dot size below the classical electron oscillatory radius and the corresponding off the dots wall scattering limits the maximum acceleration by the laser field. Moreover, this scattering leads to a chaotization of motion, causing dephasing and a loss of coherence, therefore suppressing the efficiency of the emission of highest-order harmonics. Our results demonstrate a new regime of intense laser-nanoscale solid interaction, intermediate between the bulk and single molecule response.