We report on an element-selective study of the fate of charge carriers in photoexcited inorganic CsPbBr3 and CsPb(ClBr)3 perovskite nanocrystals in toluene solutions using time-resolved X-ray absorption spectroscopy with 80 ps time resolution. Probing the Br K-edge, the Pb L3-edge, and the Cs L2-edge, we find that holes in the valence band are localized at Br atoms, forming small polarons, while electrons appear as delocalized in the conduction band. No signature of either electronic or structural changes is observed at the Cs L2-edge. The results at the Br and Pb edges suggest the existence of a weakly localized exciton, while the absence of signatures at the Cs edge indicates that the Cs+ cation plays no role in the charge transport, at least beyond 80 ps. This first, time-resolved element-specific study of perovskites helps understand the rather modest charge carrier mobilities in these materials.

Hypothesis: Enteric leakage is a significant complication of the Roux-en-Y gastric bypass (RYGB) procedure that can be treated successfully.

The measurement of chirality and its temporal evolution are crucial for the understanding of a large range of biological functions and chemical reactions. Steady-state circular dichroism (CD) is a standard analytical tool for measuring chirality in chemistry and biology. Nevertheless, its push into the ultrafast time domain and in the deep-ultraviolet has remained a challenge, with only some isolated reports of subnanosecond CD. Here, we present a broadband time-resolved CD spectrometer in the deep ultraviolet (UV) spectral range with femtosecond time resolution. The setup employs a photoelastic modulator to achieve shot-to-shot polarization switching of a 20 kHz pulse train of broadband femtosecond deep-UV pulses (250-370 nm). The resulting sequence of alternating left-and right-circularly polarized probe pulses is employed in a pump-probe scheme with shot-to-shot dispersive detection and thus allows for the acquisition of broadband CD spectra of ground-and excited-state species. Through polarization scrambling of the probe pulses prior to detection, artifact-free static and transient CD spectra of enantiopure Rubpy 3 2 are successfully recorded with a sensitivity of <2 × 10 −5 OD (≈0.7 mdeg). Due to its broadband deep-UV detection with unprecedented sensitivity, the measurement of ultrafast chirality changes in biological systems with amino-acid residues and peptides and of DNA oligomers is now feasible.

Ultrafast interfacial electron transfer in sensitized solar cells has mostly been probed by visible-to-terahertz radiation, which is sensitive to the free carriers in the conduction band of the semiconductor substrate. Here, we demonstrate the use of deep-ultraviolet continuum pulses to probe the interfacial electron transfer, by detecting a specific excitonic transition in both N719-sensitized anatase TiO and wurtzite ZnO nanoparticles. Our results are compared to those obtained on bare nanoparticles upon above-gap excitation. We show that the signal upon electron injection from the N719 dye into TiO is dominated by long-range Coulomb screening of the final states of the excitonic transitions, whereas in sensitized ZnO it is dominated by phase-space filling. The present approach offers a possible route to detecting interfacial electron transfer in a broad class of systems, including other transition metal oxides or sensitizers.

The development of next-generation perovskitebased optoelectronic devices relies critically on the understanding of the interaction between charge carriers and the polar lattice in out-of-equilibrium conditions. While it has become increasingly evident for CsPbBr 3 perovskites that the Pb−Br framework flexibility plays a key role in their light-activated functionality, the corresponding local structural rearrangement has not yet been unambiguously identified. In this work, we demonstrate that the photoinduced lattice changes in the system are due to a specific polaronic distortion, associated with the activation of a longitudinal optical phonon mode at 18 meV by electron−phonon coupling, and we quantify the associated structural changes with atomic-level precision. Key to this achievement is the combination of timeresolved and temperature-dependent studies at Br K and Pb L 3 X-ray absorption edges with refined ab initio simulations, which fully account for the screened core-hole final state effects on the X-ray absorption spectra. From the temporal kinetics, we show that carrier recombination reversibly unlocks the structural deformation at both Br and Pb sites. The comparison with the temperaturedependent XAS results rules out thermal effects as the primary source of distortion of the Pb−Br bonding motif during photoexcitation. Our work provides a comprehensive description of the CsPbBr 3 perovskites' photophysics, offering novel insights on the light-induced response of the system and its exceptional optoelectronic properties.