Ultrafast exciton fluid flow in an atomically thin MoS2 semiconductor.

Excitons (coupled electron-hole pairs) in semiconductors can form collective states that sometimes exhibit spectacular nonlinear properties. Here, we show experimental evidence of a collective state of short-lived excitons in a direct-bandgap, atomically thin MoS2 semiconductor whose propagation resembles that of a classical liquid as suggested by the nearly uniform photoluminescence through the MoS2 monolayer regardless of crystallographic defects and geometric constraints. The exciton fluid flows over ultralong distances (at least 60 µm) at a speed of ~1.8 × 107 m s-1 (~6% the speed of light). The collective phase emerges above a critical laser power, in the absence of free charges and below a critical temperature (usually Tc ≈ 150 K) approaching room temperature in hexagonal-boron-nitride-encapsulated devices. Our theoretical simulations suggest that momentum is conserved and local equilibrium is achieved among excitons; both these features are compatible with a fluid dynamics description of the exciton transport.

Optimizing Hot Electron Harvesting at Planar Metal-Semiconductor Interfaces with Titanium Oxynitride Thin Films.

Understanding metal-semiconductor interfaces is critical to the advancement of photocatalysis and sub-bandgap solar energy harvesting where electrons in the metal can be excited by sub-bandgap photons and extracted into the semiconductor. In this work, we compare the electron extraction efficiency across Au/TiO2 and titanium oxynitride (TiON)/TiO2-x interfaces, where in the latter case the spontaneously forming oxide layer (TiO2-x) creates a metal-semiconductor contact. Time-resolved pump-probe spectroscopy is used to study the electron recombination rates in both cases. Unlike the nanosecond recombination lifetimes in Au/TiO2, we find a bottleneck in the electron relaxation in the TiON system, which we explain using a trap-mediated recombination model. Using this model, we investigate the tunability of the relaxation dynamics with oxygen content in the parent film. The optimized film (TiO0.5N0.5) exhibits the highest carrier extraction efficiency (NFC ≈ 2.8 × 1019 m-3), slowest trapping, and an appreciable hot electron population reaching the surface oxide (NHE ≈ 1.6 × 1018 m-3). Our results demonstrate the productive role oxygen can play in enhancing electron harvesting and prolonging electron lifetimes, providing an optimized metal-semiconductor interface using only the native oxide of titanium oxynitride.

Zero-field quantum beats and spin decoherence mechanisms in CsPbBr3 perovskite nanocrystals.

Coherent optical manipulation of exciton states provides a fascinating approach for quantum gating and ultrafast switching. However, their coherence time for incumbent semiconductors is highly susceptible to thermal decoherence and inhomogeneous broadening effects. Here, we uncover zero-field exciton quantum beating and anomalous temperature dependence of the exciton spin lifetimes in CsPbBr3 perovskite nanocrystals (NCs) ensembles. The quantum beating between two exciton fine-structure splitting (FSS) levels enables coherent ultrafast optical control of the excitonic degree of freedom. From the anomalous temperature dependence, we identify and fully parametrize all the regimes of exciton spin depolarization, finding that approaching room temperature, it is dominated by a motional narrowing process governed by the exciton multilevel coherence. Importantly, our results present an unambiguous full physical picture of the complex interplay of the underlying spin decoherence mechanisms. These intrinsic exciton FSS states in perovskite NCs present fresh opportunities for spin-based photonic quantum technologies.