Describing the nanoscale
charge carrier transport at surfaces and
interfaces is fundamental for designing high-performance optoelectronic
devices. To achieve this, we employ time- and angle-resolved photoelectron
spectroscopy with ultraviolet pump and extreme ultraviolet probe pulses.
The resulting high surface sensitivity reveals an ultrafast carrier
population decay associated with surface-to-bulk transport, which
was tracked with a sub-nanometer spatial resolution normal to the
surface, and on a femtosecond time scale, in the case of the inorganic
CsPbBr3 lead halide perovskite. The decay time exhibits
a pronounced carrier density dependence, which is attributed via modeling
to enhanced diffusive transport and concurrent recombination. The
transport is found to approach an ordinary diffusive regime, limited
by electron–hole scattering, at the highest excitation fluences.
This approach constitutes an important milestone in our capability
to probe hot-carrier transport at solid interfaces with sub-nanometer
resolution in a theoretically and experimentally challenging, yet
technologically relevant, high-carrier-density regime.