arXiv subjects

Nathan Guisinger

Publications and source records attributed to Nathan Guisinger.

7 recordsLinked to original sources

arXiv2026

Visualization of Defect Electronic States in Layered Semiconductor CrSBr

Chromium sulfur bromide (CrSBr) is a layered magnetic semiconducting material combining a rich magnetic phase diagram with axis-dependent electronic and optical properties. While defects in CrSBr have been shown to affect magnetic order and excitonic responses, their microscopic nature, atomic structure, and electronic properties are not yet fully understood. In this work, we use scanning tunneling microscopy/spectroscopy (STM/STS) to explore the structure and electronic signatures of two prominent defects in bulk CrSBr. Their structure reflects the symmetries of the underlying lattice, with electronic features near the valence band edge. By comparing experimental data with ab initio simulated STM images, we infer that a common defect corresponds to a b-axis-aligned double sulfur vacancy, in line with findings from a recent growth analysis study. This result advances our understanding of the role of intrinsic defects in shaping the electronic structure of CrSBr.

cond-mat.mes-hall↗

arXiv2025

Bright hybrid excitons in molecularly tunable bilayer crystals

Bilayer crystals, built by stacking crystalline monolayers, generate interlayer potentials that govern excitonic phenomena but are constrained by fixed covalent lattices and orientations. Replacing one layer with an atomically thin molecular crystal overcomes this limitation, as diverse functional groups enable tunable molecular lattices and interlayer potentials, tailoring a wide range of excitonic properties. Here, we report hybrid excitons in four-atom-thick hybrid bilayer crystals (HBCs), directly synthesized with single-crystalline perylene diimide (PDI) molecular crystal atop WS2 monolayers. These excitons arise from a hybridized bilayer band structure, revealed by lattice-scale first-principles calculations, inheriting properties from both monolayers. They exhibit bright photoluminescence with near-unity polarization above and below the WS2 bandgap, along with spectral signatures of exciton delocalization, supported by theory, while their energies and intensities are tuned by modifying the HBC composition by synthesis. Our work introduces a molecule-based 2D quantum materials platform for bottom-up design and control of optoelectronic properties.

cond-mat.mtrl-sci↗

arXiv2024

Molecular tuning of excitons in four-atom-thick hybrid bilayer crystals

Bilayer crystals, formed by stacking monolayers of two-dimensional (2D) crystals, create interlayer potentials that govern excitonic phenomena but are constrained by their fixed covalent lattices. Replacing one layer with an atomically thin molecular crystal overcomes this limitation, as precise control of functional groups enables tunable 2D molecular lattices and, consequently, electronic structures. Here, we report molecular tuning of lattices and excitons in four-atom-thick hybrid bilayer crystals (HBCs), synthesized as monolayers of perylene-based molecular and transition metal dichalcogenide (TMD) single crystals. In HBCs, we observe an anisotropic photoluminescence signal exhibiting characteristics of both molecular and TMD excitons, directly tuned by molecular geometry and HBC composition. Ab initio calculations reveal that this anisotropic emission arises from hybrid excitons, which inherit properties from both layers through a hybridized bilayer band structure. Our work establishes a synthetically derived, molecule-based 2D quantum materials platform with the potential for engineering interlayer potentials.

cond-mat.mtrl-sci↗

arXiv2013

Chiral Pinwheel Heterojunctions Self Assembled from C60 and Pentacene

We demonstrate the self-assembly of C$_{60}$ and pentacene (Pn) molecules into acceptor-donor heterostructures which are well-ordered and -- despite the high degree of symmetry of the constituent molecules -- {\it chiral}. Pn was deposited on Cu(111) to monolayer coverage, producing the random-tiling ($R$) phase as previously described. Atop $R$-phase Pn, post-deposited C$_{60}$ molecules cause rearrangement of the Pn molecules into domains based on chiral supramolecular `pinwheels'. These two molecules are the highest-symmetry achiral molecules so far observed to coalesce into chiral heterostructures. Also, the chiral pinwheels (composed of 1 C$_{60}$ and 6 Pn each) may share Pn molecules in different ways to produce structures with different lattice parameters and degree of chirality. High-resolution scanning tunneling microscopy (STM) results and knowledge of adsorption sites allow the determination of these structures to a high degree of confidence. The measurement of chiral angles identical to those predicted is a further demonstration of the accuracy of the models. Van der Waals density functional theory calculations reveal that the Pn molecules around each C$_{60}$ are torsionally flexed around their long molecular axes and that there is charge transfer from C$_{60}$ to Pn in each pinwheel.

cond-mat.mes-hall↗

arXiv2011

Monolayer and bilayer pentacene on Cu(111)

The morphology and electronic structure of pentacene (Pn) deposited on Cu(111) was studied using scanning tunneling microscopy (STM) and spectroscopy (STS). Deposition of a multilayer followed by annealing to reduce coverage to a monolayer results in the formation of either of two unique phases: a 2D herringbone structure previously unobserved for any linear acene, or a 'random- tiling' structure. Coverage greater than a monolayer promotes the formation of a bilayer phase similar to that observed for Pn/Ag(111). STS shows that the electronic structure of the first layer is strongly modified due to its proximity to the substrate while the second layer exhibits nearly bulk-like electronic structure.

cond-mat.mes-hall↗

arXiv2011

Ultrathin BaTiO3 templates for multiferroic nanostructures

Structural, electronic and dielectric properties of high-quality ultrathin BaTiO3 films are investigated. The films, which are grown by ozone-assisted molecular beam epitaxy on Nb-doped SrTiO3 (001) substrates and having thicknesses as thin 8 unit cells (3.2 nm), are unreconstructed and atomically smooth with large crystalline terraces. A strain-driven transition to 3D island formation is observed for films of of 13 unit cells thickness (5.2 nm). The high structural quality of the surfaces, together with the dielectric properties similar to bulk BaTiO3 and dominantly TiO2 surface termination, make these films suitable templates for the synthesis of high-quality metal-oxide multiferroic heterostructures for the fundamental study and exploitation of magneto-electric effects, such as a recently proposed interface effect in Fe/BaTiO3 heterostructures based on Fe-Ti interface bonds.

cond-mat.mtrl-sci↗

arXiv2011

Control and Characterization of Individual Grains and Grain Boundaries in Graphene Grown by Chemical Vapor Deposition

The strong interest in graphene has motivated the scalable production of high quality graphene and graphene devices. Since large-scale graphene films synthesized to date are typically polycrystalline, it is important to characterize and control grain boundaries, generally believed to degrade graphene quality. Here we study single-crystal graphene grains synthesized by ambient CVD on polycrystalline Cu, and show how individual boundaries between coalescing grains affect graphene's electronic properties. The graphene grains show no definite epitaxial relationship with the Cu substrate, and can cross Cu grain boundaries. The edges of these grains are found to be predominantly parallel to zigzag directions. We show that grain boundaries give a significant Raman "D" peak, impede electrical transport, and induce prominent weak localization indicative of intervalley scattering in graphene. Finally, we demonstrate an approach using pre-patterned growth seeds to control graphene nucleation, opening a route towards scalable fabrication of single-crystal graphene devices without grain boundaries.

cond-mat.mes-hall↗