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Raphael Schwenzer

Publications and source records attributed to Raphael Schwenzer.

2 recordsLinked to original sources

Localized Photon Absorption in a Single-Crystalline Material

The absorption of light is one of the most fundamental processes in condensed-matter physics and optics. Here we investigate under which conditions laser light is absorbed by a crystalline material as an electromagnetic wave with delocalized properties or rather as photons that cause discrete, localized, nanometer-sized consequences. We excite the first-order phase transition of vanadium dioxide with laser pulses of sufficient frequency to overcome the band gap but with insufficient pulse energy to overcome the latent heat. According to Maxwell's equations and Bloch theory, no transition should occur, because nowhere in the material is enough energy. Nevertheless, we observe with ultrafast electron diffraction a disordered crystal geometry with nanometer-sized spots of switched material that grow and diminish with time. The amount of localized spots matches approximately to the number of photons in the absorbed laser wave. Two optical experiments substantiate this phenomenon, and simulations reproduce all measurements results. We discuss whether crystals defects, temperature, or a genuine wavefunction collapse can explain the discovered phenomenon. Practically, the reported absorption mechanism enables local consequences at substantially higher energy than average and provides insight into symmetry breaks and non-thermal fluctuations within complex materials.

physics.optics

Prospects for Direct Electron Detectors in Ultrafast Electron Diffraction and Scattering Experiments

Ultrafast electron diffraction and phonon-diffuse scattering [UED(S)] experiments make use of photo-induced changes to electron scattering intensity across 2D detectors to report on a very wide range of dynamic structural phenomena in molecules and materials. Hybrid pixel counting detectors (HPCDs) are a promising technology for improved sensitivity and signal-to-noise in UED(S) experiments, as they offer near-zero readout noise and dark counts with the possibility of new acquisition modalities (e.g., shot-to-shot normalization) due to their high frame rates. However, it is well known that HPCDs suffer from count losses at high electron fluxes even in CW beam applications. How this translates to ultrashort electron pulse exposures has yet to be determined and is critical to understanding the application of this technology to ultrafast electron scattering experiments. Here we show that count losses are significantly exacerbated in ultrafast (pulsed) experiments and that HPCDs require unconventional data handling and saturate above $\approx\!2$ electrons per pixel per pulse. This count-rate limitation presents a severe constraint on electron bunch charge when interrogating single crystal samples. Normalization strategies to optimize signal-to-noise in UED(S) and a complete model for measurement uncertainties using HPCDs are developed and tested using a large dataset. Finally, we suggest ways HPCDs could be better adapted to ultrashort pulsed beam experiments.

physics.ins-det