arXiv subjects

Shawna M. Hollen

Publications and source records attributed to Shawna M. Hollen.

3 recordsLinked to original sources

arXiv2026

Direct Evidence for Robust Bulk Band Gap Across the Charge Density Wave Transition in TiSe2

The mechanism driving the charge density wave (CDW) transition in TiSe2 has been debated for decades, with proposals ranging from an excitonic insulator to a lattice-driven instability. A central question remains whether the transition involves an opening or enhancement of the bulk band gap. Using high-resolution angle-resolved photoemission spectroscopy, we directly track the temperature evolution of the bulk band edges across the CDW transition at TCDW = 200 K. Contrary to the expectation of a gap-opening transition, we find that the size of the fundamental band gap remains constant from the high-temperature normal phase down to 160 K. While the CDW induces clear band-folding signatures and spectral weight redistribution, the underlying band extrema are unperturbed. These results demonstrate that TiSe2 does not undergo a temperature-driven electronic gap opening. Instead, they support a scenario where the transition is governed by a lattice symmetry-breaking reconstruction that folds, but does not gap, the electronic structure of a pre-existing band insulator.

cond-mat.str-el↗

arXiv2026

Emergent surface resonance from charge density wave symmetry breaking in TiSe2

Surface confined electronic states provide a fertile ground for discovering emergent phenomena that have no counterpart in the bulk, offering new routes to manipulate correlations, symmetry breaking, and dimensionality at the atomic scale. Here, we show that charge density wave (CDW) symmetry breaking can yield a surface states in 1T-TiSe2. Micro angle resolved photoemission spectroscopy resolves a sharp, two dimensional surface resonant state (SRS) that emerges within the CDW reconstructed low energy spectrum. The SRS exhibits notable temperature dependence and its spectral weight collapses around 160 K, while CDW transition temperature TCDW is commonly reported as 202 K. Slab DFT+U calculations reproduce a surface localized resonance when CDW folding brings valence and conduction states into near degeneracy, suggesting a correlation tuned, surface selective origin. These results point to a form of correlation-tuned surface resonance in a layered CDW compound and suggest a framework for engineering low dimensional quantum states in van der Waals materials via symmetry breaking and electronic structure tuning.

cond-mat.mtrl-sci↗

arXiv2023

Elucidating the Mechanism of Large Phosphate Molecule Intercalation Through Graphene Heterointerfaces

Intercalation is a process of inserting chemical species into the heterointerfaces of two-dimensional (2D) layered materials. While much research has focused on intercalating metals and small gas molecules into graphene, the intercalation of larger molecules through the basal plane of graphene remains highly unexplored. In this work, we present a new mechanism for intercalating large molecules through monolayer graphene to form confined oxide materials at the graphene-substrate heterointerface. We investigate the intercalation of phosphorus pentoxide (P2O5) molecules directly from the vapor phase and confirm the formation of confined P2O5 at the graphene heterointerface using various techniques. Density functional theory (DFT) corroborate the experimental results and reveal the intercalation mechanism, whereby P2O5 dissociates into small fragments catalyzed by defects in the graphene that then permeates through lattice defects and reacts at the heterointerface to form P2O5. This process can also be used to form new confined metal phosphates (e.g., 2D InPO4). While the focus of this study is on P2O5 intercalation, the possibility of intercalation from pre-dissociated molecules catalyzed by defects in graphene may exist for other types of molecules as well. This study is a significant milestone in advancing our understanding of intercalation routes of large molecules via the basal plane of graphene, as well as heterointerface chemical reactions leading to the formation of distinctive confined complex oxide compounds.

cond-mat.mtrl-sci↗