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Register a new userPolymer Thin Films as Universal Substrates for Extreme Ultraviolet Absorption Spectroscopy of Molecular Transition Metal Complexes
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Polystyrene and polyvinyl chloride thin films are explored as sample supports for extreme ultraviolet (XUV) spectroscopy of molecular transition metal complexes. Thin polymer films prepared by slip-coating are flat, smooth, and transmit much more XUV light than silicon nitride windows. Analytes can be directly cast onto the polymer surface, or codeposited within it. The M-edge x-ray absorption near-edge (XANES) spectra (40-90 eV) of eight archetypal transition metal complexes (M=Mn, Fe, Co, Ni) are presented to demonstrate the versatility of this method. The films are suitable for pump/probe transient absorption spectroscopy, as shown by the excited-state spectra of Fe(bpy)$_3^{2+}$ in two different polymer supports.
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Nonlinear spectroscopy in the extreme ultraviolet (EUV) and soft x-ray spectral range offers the opportunity for element selective probing of ultrafast dynamics using core-valence transitions (Mukamel et al., Acc. Chem. Res. 42, 553 (2009)). We demonstrate a step on this path showing core-valence sensitivity in transient grating spectroscopy with EUV probing. We study the optically induced insulator-to-metal transition (IMT) of a VO2 film with EUV diffraction from the optically excited sample. The VO2 exhibits a change in the 3p-3d resonance of V accompanied by an acoustic response. Due to the broadband probing we are able to separate the two features.
Metal halide perovskites single-crystalline thin films (SCTFs) have recently emerged as promising materials for the next generation of optoelectronic devices due to their superior intrinsic properties. However, it is still challenging to transfer and integrate them with other functional materials for hybrid multilayer devices because of their substrate-dependent growth. Herein, a method that allows the SCTFs to be transferred with high quality onto arbitrary substrates has been reported. By introducing hydrophobic treatment to the growth substrates, the adhesion between SCTFs and growth substrates is reduced. Meanwhile, anti-solvent intercalation technique is used to peel off SCTFs from the growth substrates intactly. Finally, centimeter-scale perovskite SCTF has been successfully transferred to target substrate. This work opens up a new route to transfer large-scale perovskite SCTFs, providing a platform to widen the applications of perovskite SCTFs in large-scale hybrid multilayer optoelectronic devices.
Implicit electron-density solvation models based on joint density-functional theory offer a computationally efficient solution to the problem of calculating thermodynamic quantities of solvated systems from firstprinciples quantum mechanics. However, despite much recent interest in such models, to date the applicability of such models in the plane-wave context to non-aqueous solvents has been limited because the determination of the model parameters requires fitting to a large database of experimental solvation energies for each new solvent considered. This work presents an alternate approach which allows development of new iso-density models for a large class of protic and aprotic solvents from only simple, single-molecule ab initio calculations and readily available bulk thermodynamic data.
We have synthesized epitaxial NdNiO$_{3}$ ultra-thin films in a layer-by-layer growth mode under tensile and compressive strain on SrTiO$_{3}$ (001) and LaAlO$_3$ (001), respectively. A combination of X-ray diffraction, temperature dependent resistivity, and soft X-ray absorption spectroscopy has been applied to elucidate electronic and structural properties of the samples. In contrast to the bulk NdNiO$_{3}$, the metal-insulator transition under compressive strain is found to be completely quenched, while the transition remains under the tensile strain albeit modified from the bulk behavior.
Coherent light pulses of few to hundreds of femtoseconds (fs) duration have prolifically served the field of ultrafast phenomena. While fs pulses address mainly dynamics of nuclear motion in molecules or lattices in the gas, liquid or condensed matter phase, the advent of attosecond pulses has in recent years provided direct experimental access to ultrafast electron dynamics. However, there are processes involving nuclear motion in molecules and in particular coupled electronic and nuclear motion that possess few fs or even sub-fs dynamics. In the present work we have succeeded in addressing simultaneously vibrational and electronic dynamics in molecular Hydrogen. Utilizing a broadband extreme-ultraviolet (XUV) continuum the entire, Frank-Condon allowed spectrum of H2 is coherently excited. Vibrational, electronic and ionization 1fs scale dynamics are subsequently tracked by means of XUV-pump-XUV-probe measurements. These reflect the intrinsic molecular behavior as the XUV probe pulse hardly distorts the molecular potential.
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