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Creators/Authors contains: "Plumb, K W"

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  1. It is undeniable that novel 2D devices and heterostructures will have a lasting impact on the advancement of future technologies. However, the inherent instability of many exfoliated van der Waals (vdW) materials is a well-known hurdle yet to be overcome. Thus, the sustained interest in exfoliated vdW materials underscores the importance of understanding the mechanisms of sample degradation to establish proactive protective measures. Here, the impact of prolonged synchrotron-based X-ray beam exposure on exfoliated flakes of two contemporary vdW materials, N i P S 3 and α - R u C l 3 , is explored using resonant inelastic X-ray scattering (RIXS) and total fluorescence yield X-ray absorption spectroscopy (XAS). In N i P S 3 , the resulting RIXS and XAS spectra show a suppression, then vanishing, of NiS6multiplet excitations coupled with an upward shift of the peak energy of the XAS as a function of X-ray dose. In α - R u C l 3 , the signs of beam damage from the RIXS spectra are less evident. However, the post-experiment characterization of both materials using Raman spectroscopy exhibits signals of an amorphous and disordered system compared to pristine flakes; in addition, energy-dispersive X-ray spectroscopy of N i P S 3 shows evidence of ligand vacancies. As synchrotron radiation is fast becoming a required probe to study 2D vdW materials, these findings lay the groundwork for the development of future protective measures for synchrotron-based prolonged X-ray beam exposure, as well as for X-ray free electron laser. 
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    Free, publicly-accessible full text available June 25, 2026
  2. Abstract Understanding the interplay between the inherent disorder and the correlated fluctuating-spin ground state is a key element in the search for quantum spin liquids. H3LiIr2O6is considered to be a spin liquid that is proximate to the Kitaev-limit quantum spin liquid. Its ground state shows no magnetic order or spin freezing as expected for the spin liquid state. However, hydrogen zero-point motion and stacking faults are known to be present. The resulting bond disorder has been invoked to explain the existence of unexpected low-energy spin excitations, although data interpretation remains challenging. Here, we use resonant X-ray spectroscopies to map the collective excitations in H3LiIr2O6and characterize its magnetic state. In the low-temperature correlated state, we reveal a broad bandwidth of magnetic excitations. The central energy and the high-energy tail of the continuum are consistent with expectations for dominant ferromagnetic Kitaev interactions between dynamically fluctuating spins. Furthermore, the absence of a momentum dependence to these excitations are consistent with disorder-induced broken translational invariance. Our low-energy data and the energy and width of the crystal field excitations support an interpretation of H3LiIr2O6as a disordered topological spin liquid in close proximity to bond-disordered versions of the Kitaev quantum spin liquid. 
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