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  1. We present an approach to selectively examine an asymmetric potential in the buried layer of solar cell devices by means of nonlinear x-ray spectroscopy. Detecting second harmonic generation signals while resonant to the SiO2 core level, we directly observe existence of the band bending effect in the SiO2 nanolayer, buried in the heterostructures of Al/LiF/SiO2/Si, TiO2/SiO2/Si, and Al2O3/SiO2/Si. The results demonstrate high sensitivity of the method to the asymmetric potential that determines performance of functional materials for photovoltaics or other optoelectronic devices.

     
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    Free, publicly-accessible full text available July 17, 2024
  2. Abstract

    Solid-state electrolytes overcome many challenges of present-day lithium ion batteries, such as safety hazards and dendrite formation1,2. However, detailed understanding of the involved lithium dynamics is missing due to a lack of in operando measurements with chemical and interfacial specificity. Here we investigate a prototypical solid-state electrolyte using linear and nonlinear extreme-ultraviolet spectroscopies. Leveraging the surface sensitivity of extreme-ultraviolet-second-harmonic-generation spectroscopy, we obtained a direct spectral signature of surface lithium ions, showing a distinct blueshift relative to bulk absorption spectra. First-principles simulations attributed the shift to transitions from the lithium 1 sstate to hybridized Li-s/Ti-dorbitals at the surface. Our calculations further suggest a reduction in lithium interfacial mobility due to suppressed low-frequency rattling modes, which is the fundamental origin of the large interfacial resistance in this material. Our findings pave the way for new optimization strategies to develop these electrochemical devices via interfacial engineering of lithium ions.

     
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  3. Although ultrafast manipulation of magnetism holds great promise for new physical phenomena and applications, targeting specific states is held back by our limited understanding of how magnetic correlations evolve on ultrafast timescales. Using ultrafast resonant inelastic X-ray scattering we demonstrate that femtosecond laser pulses can excite transient magnons at large wavevectors in gapped antiferromagnets and that they persist for several picoseconds, which is opposite to what is observed in nearly gapless magnets. Our work suggests that materials with isotropic magnetic interactions are preferred to achieve rapid manipulation of magnetism. 
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