Spin blockades to relaxation of hot multi-excitons in nanocrystals

The rates of elementary photophysical processes in nanocrystals, such as carrier cooling, multiexciton generation, Auger recombination etc., are determined by monitoring the transient occupation of the lowest exciton band. The underlying assumption is that hot carriers relax rapidly to their lowest quantum level. Using femtosecond transient absorption spectroscopy in CdSe/CdS nanodots we challenge this assumption. Results show, that in nanodots containing a preexisting cold exciton "spectator", \emph{only half of the photoexcited electrons}relax directly to the band-edge and the complementary half is blocked in an excited state level due to Pauli exclusion. Full relaxation occurs only after \textasciitilde 15 ps, as the blocked electrons flip spin. This novel spin-blockade effect may offer the key for the long-sought-for bottleneck mechanism for multiexciton energy dissipation

Global wealth disparities drive adherence to COVID-safe pathways in head and neck cancer surgery

Peer reviewe

A phase-field approach to model evaporation in porous media: Upscaling from pore to Darcy scale

We develop a phase-field model for evaporation in a porous medium by explicitly considering a vapor component together with the liquid and gas phases in the system. The phase-field model consists of the conservation of mass (for phases and vapor component), momentum, and energy. In addition, the evolution of the phase field is described by the Allen-Cahn equation. In the limit of vanishing interface width, matched asymptotic expansions reveal that the phase-field model reduces to the sharp-interface model with all the relevant transmission conditions at the moving interface. An energy estimate is derived, which suggests that for the diffusion-dominated regime, energy always decreases with time. However, this is not always the case for other regimes. The phase-field model is upscaled to the Darcy scale using periodic homogenization for the diffusion-dominated regime. The effective parameters at the Darcy scale are connected to the pore scale through corresponding cell problems.Comment: 33 pages, 5 figure

White-Light Emission from Unmodified Graphene Oxide Quantum Dots

We report herein the synthesis and characterization of unmodified graphene oxide quantum dots (GOQDs) with white-light-emitting properties, upon photoexcitation at 340 nm. The Commission International de l’Éclairage (CIE) 1931 chromaticity coordinates for GOQDs (<i>x</i> = 0.29, <i>y</i> = 0.34) suggest that highly pure white-light emission was achieved. A detailed mechanistic study was carried out utilizing UV–visible absorption, steady-state and time-resolved fluorescence spectroscopy, and dynamic light scattering (DLS) techniques to understand the origin of the white-light emission. The results taken together suggest that GOQDs could self-assemble in solution and thus transform the luminescence behavior. Furthermore, the results indicate that the pH of the medium also plays a crucial role in assisting the aggregation to generate the white-light emission. The concentration-dependent DLS measurements support a cooperative mechanism for the aggregation kinetics in the system. More importantly, the study suggests that white-light emission can be generated from unmodified graphene oxide quantum dots by tuning their nanoscopic aggregation properties

Monitoring hot exciton dissociation in hybrid lead halide perovskite films with sub-10 fs pulses

Sub-10 fs pump-probe experiments on methylammonium lead halide (MAPbI3) perovskite films show hot exciton dissociation in 20 fs after photo-excitation with ~0.7 eV excess energy compared to its optical band gap (BG). Coherent wave packets were also detected in the form of spectral modulation, revealing electron-phonon coupling in these materials. The estimated electron-phonon coupling strengths from the frequency and amplitude of the detected spectral modulation are in the weak regime, suggesting formation of large polaron