Spatio-temporal ultrafast pulse shaping at the femtosecond–nanometer scale

Abstract

Optical pulse shaping is a fundamental tool for coherent control of the light–matter interaction. While such control enables the measurement of ultrafast temporal dynamics, simultaneous spatiotemporal control is required for studying non-local ultrafast charge dynamics at the nanoscale. However, obtaining accurate spatial control at a sub-wavelength resolution with conventional optical elements poses significant difficulty. Here, we use the spatiotemporal coupling naturally arising in a spatial light modulator based pulse shaping apparatus to achieve accurate control with femto–nano spatiotemporal resolution. We experimentally demonstrate spatial steering at the sub-micron scale of second harmonic generation from nanostructures. In addition, we apply an absolute-value spectral phase to achieve controlled double pulses for nanoscale excitation. We introduce a novel, to the best of our knowledge, scheme for accurate tunable spatiotemporal pump–probe experiments. This method offers rich insight into materials with ultrafast transport phenomena at the femtosecond–nanometer regimes.