High-density femtosecond transient absorption spectroscopy of semiconductor nanoparticles. A tool to investigate surface quality

At the high laser excitation intensities used in our experiments, more than 50 electron-hole pairs are formed in colloidal semiconductor nanoparticles used in our studies. At this density of charge carriers, new transient absorptions are observed in the femtosecond transient spectra in the 450 to 700 nm region with unresolved fast rise (<100 fs) and two decay components of 660 fs and >150 ps. The absorption at 510 nm could be quenched with the adsorption of electron accepters (e.g., benzoquinone, 1,2-naphthoquinone), whereas the low-energy transient absorption was not affected. For CdS NPs, we found that passivation eliminated most of the transient absorption. The transient absorptions are thus proposed to result from either trap-state absorption, trapped dimers (or complexes) and/or Stark-shifted exciton absorption resulting from surface electric field of the uncompensated trapped electron-hole pairs. All these possibilities require effective surface trapping at these high levels of excitation.