Photoconductivity and Photoemission of Diamond Under Femtosecond Vuv Irradiation

TL;DR

This study investigates diamond's electronic relaxation mechanisms under femtosecond VUV irradiation by combining experimental measurements of photoconductivity and photoemission with ab initio calculations of quasiparticle lifetimes, revealing complex electron dynamics.

Contribution

It provides the first ab initio calculations of quasiparticle lifetimes in diamond and offers new insights into the electron relaxation processes under high-energy femtosecond VUV pulses.

Findings

Photoconductivity saturates and decreases at higher harmonic energies.

Few low energy secondary electrons are observed despite high photon energies.

High energy electrons may excite plasmons, influencing relaxation mechanisms.

Abstract

In order to gain some insight on the electronic relaxation mechanisms occuring in diamond under high intensity laser excitation and/or VUV excitation, we studied experimentally the pulsed conductivity induced by femtosecond VUV pulses, as well as the energy spectra of the photoelectrons released by the same irradiation. The source of irradiation consists in highly coherent VUV pulses obtained through high order harmonic generation of a high intensity femtosecond pulse at a 1.55 eV photon energy (titanium-doped sapphire laser). Harmonics H9 to H17 have been used for photoconductivity (PC) and harmonics H13 to H27 for photoemission experiments (PES). As the photon energy is increased, it is expected that the high energy photoelectrons will generate secondary e-h pairs, thus increasing the excitation density and consequently the PC signal. This is not what we observe : the PC signal first increases for H9 to H13, but then saturates and even decreases. Production of low energy secondary e-h pairs should also be observed in the PES spectrum. In fact we observe very few low energy electrons in the PES spectrum obtained with H13 and H15, despite the sufficient energy of the generated free carriers. At the other end (H21 and above), a very intense low energy secondary electron peak is observed. As a help to interprete such data, we realized the first ab initio calculations of the electronic lifetime of quasiparticles, in the GW approximation in a number of dielectrics including diamond. We find that the results are quite close to a simple "Fermi-liquid" estimation using the electronic density of diamond. We propose that a quite efficient mechanism could be the excitation of plasmons by high energy electrons, followed by the relaxation of plasmons into individual e-h pairs.