arXiv subjects

Oscar Custance

Publications and source records attributed to Oscar Custance.

5 recordsLinked to original sources

arXiv2026

Reconstruction-Dependent Imaging, Reactivity and Local Reduction of the CeO$_2$(100) surface

The possibility of mapping the local reactivity and reduction state to the atomic structure of chemically active oxide surfaces opens new avenues for further understanding of catalysis. Here, we combine scanning tunnelling (STM) and atomic force microscopy (AFM) with first-principles modelling to explore this possibility on the CeO2(100) surface. While STM reveals the periodicity of cerium-terminated and oxygen-terminated CeO$_2$(100) reconstructions coexisting on the same surface, AFM imaging and force spectroscopy provide direct identification of the exposed atomic species and their reactivity as the chemical interaction with the probe. Density functional theory based STM and AFM simulations reproduce the main experimental observations and show that STM contrast cannot be in general assigned to the atomic positions of certain chemical species, as traditionally assumed from previous studies. Simulated STM contrast of the two reconstructions across different reduction states associated with the removal of oxygen atoms in deeper layers, evidence that STM alone does not offer a robust fingerprint of the local reduction state for the cerium-terminated reconstruction, but it is sensitive to the reduced state in the case of the oxygen-terminated one, being able to provide information on a mixed distribution of Ce$^{3+}$ and Ce$^{4+}$ ions on the first sub-surface Ce layer.

cond-mat.mtrl-sci↗

arXiv2026

A low-temperature ultra-high-vacuum scanning probe microscope with in situ electronic transport capabilities: from macro to nano in 10 minutes

We have developed a low temperature (LT), ultra-high-vacuum (UHV) system that combines two complementary techniques, scanning probe microscopy (SPM) and electrical transport measurements, within a single platform. By providing simultaneous access to the atomic-scale surface landscape and the macroscopic device response of the same sample, the setup enables direct correlations between local structural/spectroscopic signatures and global electronic transport behavior in two-dimensional (2D) devices. The system allows experiments where atomic-scale modifications or controlled manipulations are performed while continuously monitoring their impact on device-scale performance. The setup consists of two interconnected UHV chambers: a dedicated preparation chamber and a separate measurement chamber that houses a liquid-helium cryostat and the SPM/transport stage. Base pressure is 1x10^-11 Torr. A key feature is direct optical access to the sample, enabling rapid and reliable tip positioning with an accuracy of 5 microns x 5 microns within 10 minutes. The SPM, operated using custom-built electronics, can track the exact same sample region across a temperature range from 2.9 K to 400 K, with mechanical stability below 1 pm. System performance is demonstrated on graphene devices, and bulk Pb is used to determine energy resolution. Using superconducting tips, scanning tunneling spectroscopy measures the superconducting gap with an energy resolution of 30 microV. Transport measurements track the temperature dependence of both resistivity and critical current across the superconducting transition of an in-situ prepared Pb nanowire.

cond-mat.mes-hall↗

arXiv2025

Near-surface Defects Break Symmetry in Water Adsorption on CeO$_{2-x}$(111)

Water interactions with oxygen-deficient cerium dioxide (CeO$_2$) surfaces are central to hydrogen production and catalytic redox reactions, but the atomic-scale details of how defects influence adsorption and reactivity remain elusive. Here, we unveil how water adsorbs on partially reduced CeO$_{2-x}$(111) using atomic force microscopy (AFM) with chemically sensitive, oxygen-terminated probes, combined with first-principles calculations. Our AFM imaging reveals water molecules as sharp, asymmetric boomerang-like features radically departing from the symmetric triangular motifs previously attributed to molecular water. Strikingly, these features localize near subsurface defects. While the experiments are carried out at cryogenic temperature, water was dosed at room temperature, capturing configurations relevant to initial adsorption events in catalytic processes. Density functional theory identifies Ce$^{3+}$ sites adjacent to subsurface vacancies as the thermodynamically favored adsorption sites, where defect-induced symmetry breaking governs water orientation. Force spectroscopy and simulations further distinguish Ce$^{3+}$ from Ce$^{4+}$ centers through their unique interaction signatures. By resolving how subsurface defects control water adsorption at the atomic scale, this work demonstrates the power of chemically selective AFM for probing site-specific reactivity in oxide catalysts, laying the groundwork for direct investigations of complex systems such as single-atom catalysts, metal-support interfaces, and defect-engineered oxides.

cond-mat.mtrl-sci↗

arXiv2023

Local Probe Structure Isomerization in a One-Dimensional Molecular Array

Synthesis of one-dimensional molecular arrays with tailored stereoisomers is challenging yet has a great potential for application in molecular opto-, electronic- and magnetic-devices, where the local array structure plays a decisive role in the functional properties. Here, we demonstrate construction and characterization of dehydroazulene isomer and diradical units in three-dimensional organometallic compounds on Ag(111) with a combination of low-temperature scanning tunneling microscopy and density functional theory calculations. Tip-induced voltage pulses firstly result in the formation of a diradical species via successive homolytic fission of two C-Br bonds in the naphthyl groups, which are subsequently transformed into chiral dehydroazulene moieties. The delicate balance of the reaction rates among the diradical and two stereoisomers, arising from an in-line configuration of tip and molecular unit, allows directional azulene-to-azulene and azulene-to-diradical local probe structural isomerization in a controlled manner. Furthermore, our theoretical calculations suggest that the diradical moiety hosts an open-shell singlet with antiferromagnetic coupling between the unpaired electrons, which can undergo an inelastic spin transition of 91 meV to the ferromagnetically coupled triplet state.

cond-mat.mtrl-sci↗

arXiv2020

Machine-learning Based Extraction of the Short-Range Part of the Interaction in Non-contact Atomic Force Microscopy

A machine-learning method for extracting the short-range part of the probe-surface interaction from force spectroscopy curves is presented. Our machine-learning algorithm consists of two stages: the first stage determines a boundary that separates the region where the short-range interaction is dominantly acting on the probe, and a second stage that finds the parameters to fit the interaction over the long-range region. We successfully applied this method to force spectroscopy maps acquired over the Si(111)-(7x7) surface and found, as a result, a faint structure on the short-range interaction for one of the probes used in the experiments that would have probably been obviated using human-supervised fitting strategies.

cond-mat.mes-hall↗