RESUMEN
Gas-phase fullerenes emit thermal electrons after femtosecond laser excitation in the wavelength range 400-800 nm. We have used angular-resolved photoelectron spectroscopy (PES) to study the influence of the laser's electric field on the dynamics of the thermally emitted electrons. The laser field introduces an asymmetry in the thermal electron distributions with respect to the laser polarization direction, which was confirmed by carrying out experiments at different wavelengths. A simple model could reproduce the trends in measured apparent temperatures in the PES. The asymmetry effect was exploited in a pump-probe experiment to estimate the time scale for thermal electron emission. It was found that, when 400 nm, 120 fs laser pulses of 2 TW cm(-2) intensity are used, thermal electrons are emitted up to ca. 300 fs after the peak of the laser pulse. The pump-probe scheme should be applicable to a wider range of complex molecules and clusters showing thermal electron emission on a femtosecond time scale.
RESUMEN
Angular-resolved photoelectron spectroscopy using wavelength-tuneable femtosecond laser pulses is presented for a series of fullerenes, namely, C70, C82, and Sc3N@C80. The photoelectron kinetic energy distributions for the three molecules show typical thermal electron spectra with a superimposed peak structure that is the result of one-photon ionization of diffuse low-angular momenta states with electron density close to the carbon cage and that are related to so-called super atom molecular orbitals. Photoelectron angular distributions confirm this assignment. The observed structure is less prominent compared to the thermal electron background than what was observed in C60. It can be concluded that hot electron emission is the main ionization channel for the larger and more complex molecules for these excitation conditions.
RESUMEN
Photoelectron angular distributions from both C(60) and C(70) were recorded for low laser intensity femtosecond and picosecond pulses. Rich structure is seen for electron kinetic energies that lie below the photon energy. Strong, broad peaks are observed for photoelectron energies corresponding to single-photon ionization of so-called superatom molecular orbitals (SAMOs). The very simple angular distributions measured for these peaks, the close similarity of the spectra observed from C(60) and C(70), and the comparison with time-dependent density functional theory provide strong support for the SAMO hypothesis.