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The evolution of charge carriers in photoexcited room temperature ZnOnanoparticles in solution is investigated using ultrafast ultravioletphotoluminescence spectroscopy, ultrafast Zn K-edge absorption spectroscopy andab-initio molecular dynamics (MD) simulations. The photoluminescence is excitedat 4.66 eV, well above the band edge, and shows that electron cooling in theconduction band and exciton formation occur in <500 fs, in excellent agreementwith theoretical predictions. The X-ray absorption measurements, obtained uponexcitation close to the band edge at 3.49 eV, are sensitive to the migrationand trapping of holes. They reveal that the 2 ps transient largely reproducesthe previously reported transient obtained at 100 ps time delay in synchrotronstudies. In addition, the X-ray absorption signal is found to rise in ~1.4 ps,which we attribute to the diffusion of holes through the lattice prior to theirtrapping at singly-charged oxygen vacancies. Indeed, the MD simulations showthat impulsive trapping of holes induces an ultrafast expansion of the cage ofZn atoms in <200 fs, followed by an oscillatory response at a frequency of ~100cm-1, which corresponds to a phonon mode of the system involving the Znsub-lattice.

Disentangling the Evolution of Electrons and Holes in photoexcited ZnO nanoparticles