arXiv subjects

Tom Barnowsky

Publications and source records attributed to Tom Barnowsky.

4 recordsLinked to original sources

arXiv2025

Exfoliation and Cleavage of Crystals from a Universal Potential

Exfoliation and cleavage create two-dimensional (2D) materials and surfaces with physical and chemical properties distinct from their bulk parents. The rising class of non-van der Waals (non-vdW) 2D materials derived from non-layered crystals provides a fascinating new platform - greatly expanding the landscape of low-dimensional materials. Current computational models, however, provide limited guidance: existing descriptors are largely tailored to vdW layered systems. Here, we introduce a general framework predicting crystal cleavage and exfoliable 2D subunits directly from bulk structures. At its core is a universal eXfoliation and Cleavage Potential (XCP) enabling large-scale screening of diverse materials at negligible computational cost. Applying this approach, we obtain 37,208 cleavable surfaces and candidate non-vdW 2D materials from which we investigate 2,377 likely exfoliable ones using high-throughput density functional theory. We identify sheets with square and rectangular lattices, semiconducting systems exhibiting an indirect-to-direct band-gap transition upon exfoliation, and first non-vdW 2D metals. Our study thus opens a systematic route to explore and design new 2D materials with unprecedented chemical and structural diversity.

cond-mat.mtrl-sci↗

arXiv2025

Non-van der Waals Heterostructures

Beyond the study of individual materials, their interfaces and arising functionality are crucial enablers of fundamental science and technological progress. Recently, the arena of two-dimensional (2D) materials was extended to so-called non-van der Waals (non-vdW) compounds derived from strongly bonded non-layered bulk crystals. These nanosystems have advantageous active surfaces and thus now complement - through their chemically bonded heterostructure (HS) interfaces - the established space of weakly interacting vdW HSs. Here, we study a wide range of 55 candidate non-vdW HSs with extensive density functional calculations and find that the resulting interfacial chemical hybridization and bonding is the key factor determining their electronic and magnetic properties. It gives rise to the formation of unique hybrid interface bands, strong magnetic coupling, and substantial electronic as well as magnetic moire surface property modulations upon twisting. Our work thus provides a valuable platform for charting the new interface class of non-vdW HSs.

cond-mat.mtrl-sci↗

arXiv2023

Magnetic State Control of Non-van der Waals 2D Materials by Hydrogenation

Controlling the magnetic state of two-dimensional (2D) materials is crucial for spintronic applications. By employing data-mining and autonomous density functional theory calculations, we demonstrate the switching of magnetic properties of 2D non-van der Waals materials upon hydrogen passivation. The magnetic configurations are tuned to states with flipped and enhanced moments. For 2D CdTiO$_3$ - a nonmagnetic compound in the pristine case - we observe an onset of ferromagnetism upon hydrogenation. Further investigation of the magnetization density of the pristine and passivated systems provides a detailed analysis of modified local spin symmetries and the emergence of ferromagnetism. Our results indicate that selective surface passivation is a powerful tool for tailoring magnetic properties of nanomaterials such as non-vdW 2D compounds.

cond-mat.mtrl-sci↗

arXiv2022

A New Group of Two-Dimensional Non-van der Waals Materials with Ultra Low Exfoliation Energies

The exfoliation energy - quantifying the energy required to extract a two-dimensional (2D) sheet from the surface of a bulk material - is a key parameter determining the synthesizability of 2D compounds. Here, using ab initio calculations, we present a new group of non-van der Waals 2D materials derived from non-layered crystals which exhibit ultra low exfoliation energies. In particular for sulfides, surface relaxations are essential to correctly describe the associated energy gain needed to obtain reliable results. Taking into account long-range dispersive interactions has only a minor effect on the energetics and ultimately proves that the exfoliation energies are close to the ones of traditional van der Waals bound 2D compounds. The candidates with the lowest energies, 2D SbTlO$_3$ and MnNaCl$_3$, exhibit appealing electronic, potential topological, and magnetic features as evident from the calculated band structures making these systems an attractive platform for fundamental and applied nanoscience.

cond-mat.mtrl-sci↗