Physics Commons^™

Atom-Specific Probing Of Electron Dynamics In An Atomic Adsorbate By Time-Resolved X-Ray Spectroscopy, Simon Schreck, Elias Diesen, Martina Dell'angela, Chang Liu, Matthew Weston, Flavio Capotondi, Hirohito Ogasawara, Jerry Larue, Roberto Costantini, Martin Beye, Piter S. Miedema, Joakim Halldin Stenlid, Jörgen Gladh, Boyang Liu, Hsin-Yi Wang, Fivos Perakis, Filippo Cavalca, Sergey Koroidov, Peter Amann, Emanuele Pedersoli, Denys Naumenko, Ivaylo Nikolov, Lorenzo Raimondi, Frank Abild-Pedersen, Tony F. Heinz, Johannes Voss, Alan C. Luntz, Anders Nilsson

Biology, Chemistry, and Environmental Sciences Faculty Articles and Research

The electronic excitation occurring on adsorbates at ultrafast timescales from optical lasers that initiate surface chemical reactions is still an open question. Here, we report the ultrafast temporal evolution of x-ray absorption spectroscopy (XAS) and x-ray emission spectroscopy (XES) of a simple well-known adsorbate prototype system, namely carbon (C) atoms adsorbed on a nickel [Ni(100)] surface, following intense laser optical pumping at 400 nm. We observe ultrafast (∼100  fs) changes in both XAS and XES showing clear signatures of the formation of a hot electron-hole pair distribution on the adsorbate. This is followed by slower changes on a few picoseconds …

Turning Density Functional Theory Calculations Into Molecular Mechanics Simulations : Establishing The Fluctuating Density Model For Rna Nucleobases, Christopher A. Myers

Legacy Theses & Dissertations (2009 - 2024)

Molecular mechanics (MD) simulations and density functional theory (DFT) have been the backbone of computational chemistry for decades. Due to its accuracy and computational feasibility, DFT has become the go-to method for theoretically predicting interaction energies, polarizability, and other electronic properties of small molecules at the quantum mechanical level. Although less fundamental than DFT, molecular mechanics (MM) algorithms have been just as influential in the fields of biology and chemistry, owing their success to the ability to compute measurable, macroscopic quantities for systems with tens of thousands to hundreds of thousands of atoms at a time. Nevertheless, MD simulations would …

Hydrogen Behavior At Crystalline/Amorphous Interface Of Transparent Oxide Semiconductor And Its Effects On Carrier Transport And Crystallization, Julia E. Medvedeva, Kapil Sharma, Bishal Bhattarai, Mariana I. Bertoni

Physics Faculty Research & Creative Works

The role of disorder and particularly of the interfacial region between crystalline and amorphous phases of indium oxide in the formation of hydrogen defects with covalent (In-OH) or ionic (In-H-In) bonding are investigated using ab initio molecular dynamics and hybrid density-functional approaches. The results reveal that disorder stabilizes In-H-In defects even in the stoichiometric amorphous oxide and also promotes the formation of deep electron traps adjacent to In-OH defects. Furthermore, below-room-temperature fluctuations help switch interfacial In-H-In into In-OH, creating a new deep state in the process. This H-defect transformation limits not only the number of free carriers but also the …

Tuning Properties Of Topological Insulators: An Ab-Initio Approach, Karunya Shailesh Shirali

LSU Doctoral Dissertations

This thesis develops a first-principles based approach to explore the tuning of topological properties of the tetradymite topological insulators. We begin by setting up a framework to systematically obtain the bulk and surface properties of topological insulators, treating the structural and electronic properties on an equal footing. We determine a consistent method for including the van der Waals interactions, which are responsible for the weak coupling between sets of atomic layers in this family of layered materials, which is important in obtaining accurate structural properties. We obtain close agreement with experimental values for both the bulk and surface states.

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