Title: Dynamics of quantum materials at the nanoscale
Description: Programming the properties of quantum materials on demand is a central goal of condensed matter physics with the potential to usher in a new technological era. Photoexcitation has proven to be an exceptionally capable means of resonant and non-resonant control over matter offering coveted routes to selectively control the electronic, lattice, interband or valley optical and excitonic properties of quantum materials. One major limitation of probing the rich class of phenomena enabled by photoexcitation is the diffraction limit. The properties of quantum materials are often sensitive to the microscopic details of the environment at phase transition boundaries: which naturally leads drastic inhomogeneity at the nanoscale. In other cases, the media may transiently support high-momentum “nano-light” or host topologically protected conductive channels that are localized to one-dimensional physical edges. All of these phenomena demand a probe with the spatial resolution that is commensurate with the emergent behavior.

To address these demands the author contributed to the development of time-resolved scattering near-field optical microscopy (Tr-SNOM). Utilizing the principles developed as part of this thesis amplified laser technology was combined with a commercial near-field optical microscope to produce a state-of-the-art time-resolved nanoscope. The custom apparatus operates with twenty nanometer spatial resolution with unprecedented spectral coverage spanning visible to mid-infrared all with (30-300) femtosecond temporal resolution. The experimental apparatus was, first, applied to investigate the photo-induced insulator-to-metal transition in Vanadium Dioxide. We observe nanoscale inhomogeneity of the transient conductivity. Our data reveals that local nanoscopic variations of the strain exist in our particular VO2 thin film at equilibrium. Regions of compressive strain are, furthermore, found to correlate with regions where a high degree of transient conductivity is attained. Our systematic study of the local fluence dependence and dynamics reveal that the fluence threshold, Fc, for the monoclinic-insulator to rutile-metal transition is inhomogeneous in real-space.

A second growth process is identified, even at excitations fluences well below Fc, which operates on a longer timescale with an inhomogeneous rise time, tau-1. Together Fc and tau-1 govern the inhomogeneous nano-texturing of the transient conductivity. Secondly, we uncover that crystals of van-der Waals (vdW) semiconductors behave as optical waveguides with broadly tunable properties at femto-second time scales. We detect giant optical phase shifts of waveguided photons under strong photo-excitation devoid of any unwanted added losses in the vdW crystal, WSe2. Our results firmly implicate bound excitons in the observed behavior. Our transient spatio-temporal maps reveal two concomitant effects: i) photo-generation of electron-hole plasma that drives the WSe2 crystal towards a Mott transition where excitons dissociate and ii) a coherent interaction between the waveguide material and pump light, known as the optical Stark effect, that alters the phase velocity of guided photons on the femtosecond timescale.