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Samuel Palato

Publications and source records attributed to Samuel Palato.

3 recordsLinked to original sources

Time-resolved SNOM via phase-domain sampling

Time-resolved scanning near-field optical microscopy (tr-SNOM) enables the measurement of the dynamic optical response of functional surfaces beyond the diffraction limit. Experimental challenges are imposed both by the use of a pulsed light source, and by the need for interferometric signal modulation to isolate the near-field contribution. We present a novel experimental approach to retrieve the tr-SNOM signal using a 200 kHz laser system and pseudo-heterodyne modulation. We circumvent the Nyquist limit for spectral demodulation by sampling modulation phases, pump intensity and SNOM signal for every laser shot. A general time-resolved SNOM signal is derived, independent of detection scheme or physical assumptions about the near-field enhancement, and is successfully measured and isolated on WS$_2$ monolayer and multilayer regions. We confirm localization by signal-distance curves, spatial confinement at material boundaries, and by identifying signal contributions at individual modulation harmonics. Disentangling the dynamic contributions enables us to extract the dynamic dielectric function of the sample. Showing the capability of phase-domain sampling paves the way to integration of more diverse and specialized light sources, growing the potential of optical ultrafast near-field measurements.

physics.optics

Real-Time Formation of a Landau Polaron

Polarons are electronic excitations dressed by a self-consistent lattice distortion, yet their formation has not been directly resolved in real time. We develop a microscopic lineshape framework that connects the growth of a collective lattice polarization to the population-time evolution of the anti-diagonal linewidth in coherent multidimensional spectroscopy. Within this formalism, the anti-diagonal linewidth directly tracks the decay of lattice frequency-frequency correlations. Underdamped phonon environments produce oscillatory linewidth modulation, whereas overdamped collective polarization dynamics generate monotonic exponential broadening. Applying this framework to multidimensional measurements on perovskite quantum dots, we show that the observed approximately 150 femtosecond exponential anti-diagonal broadening reflects the decay of a collective polarization order parameter. These results establish anti-diagonal linewidth dynamics as a direct real-time signature of Landau polaron formation.

cond-mat.other

Discontinuous character of the ultrafast exciton Mott transition in monolayer WS$_2$

There are conflicting predictions and reports on the character of the exciton Mott transition (EMT) in monolayer transition metal dichalcogenides. It could be either a discontinuous or a continuous transition from the excitonic to the plasma phase, with important implications for devices such as photoswitches. To resolve the nature of the transition in monolayer WS$_2$, we study its ultrafast optical response upon resonant photoexcitation of the A exciton across a broad range of photoexcitation densities. In agreement with previously reported measurements we observe that the A exciton quenches gradually with increasing excitation density. However, a detailed lineshape analysis unveils an abrupt red shift in the transient peak positions of the A and B exciton resonances above an excitation density threshold. This is attributed to band gap renormalization arising from the formation of free charge carrier plasma, i.e., the EMT. The plasma phase decays with a time constant of 0.65 ps back into the excitonic state. The abrupt appearance of the plasma phase at the threshold density suggests that the EMT is a discontinuous and not a continuous transition. This work demonstrates how transient optical spectroscopy combined with lineshape analysis of two excitonic resonances simultaneously can be used to investigate the EMT in 2D materials.

cond-mat.mtrl-sci