arXiv subjects

Luis Sandoval

Publications and source records attributed to Luis Sandoval.

8 recordsLinked to original sources

arXiv2026

Towards Atom-by-Atom Fabrication: Mechanosynthetic donation and abstraction

Enabled by inverted-mode scanning tunneling microscopy (IM-STM) and the use of functionalized molecular tools, we demonstrate positionally-controlled mechanosynthetic addition (donation) of carbon and subtraction (abstraction) of silicon atoms on a model build site: atomically clean and crystalline Si(100). The resulting structures represent the first demonstrations of an emerging ability to manipulate radical chemistry with positional control of specific atoms and moieties in 3D. Furthermore, by comparing the behavior of molecular tools designed for atomic donation versus abstraction, we highlight general principles governing molecular tool design for selective and reliable mechanosynthetic functionality.

cond-mat.mtrl-sci↗

arXiv2026

Atomically precise mechanosynthesis of carbon structures on hydrogenated Si(100) by inverted-mode STM

The ability to build atomically precise structures on surfaces with complete control over both atomic placement and chemical bonding remains a central challenge in nanoscale fabrication. Here, we demonstrate simultaneous spatial and chemical control over the mechanosynthetic fabrication of carbon structures. Using inverted-mode STM, C$_2$ units are donated from surface-deposited molecules to pre-patterned reactive sites on a hydrogen-passivated Si(100) surface. We demonstrate single-site C$_2$ donation, spatially patterned multi-site C$_2$ donation, and the stepwise assembly of polyyne structures through successive C-C bond formation. Together, these results establish controlled mechanosynthetic donation as a foundational capability for programmable atomically precise fabrication.

cond-mat.mtrl-sci↗

arXiv2025

Inverted-Mode Scanning Tunneling Microscopy for Atomically Precise Fabrication

Scanning Tunneling Microscopy (STM) enables fabrication of atomically precise structures with unique properties and growing technological potential. However, reproducible manipulation of covalently bonded atoms requires control over the atomic configuration of both sample and probe - a longstanding challenge in STM. Here, we introduce inverted-mode STM, an approach that enables mechanically controlled chemical reactions for atomically precise fabrication. Tailored molecules on a Si(100) surface image the probe apex, and the usual challenge of understanding the probe structure is effectively solved. The molecules can also react with the probe, with the two sides of the tunnel junction acting as reagents positioned with sub-angstrom precision. This allows abstraction or donation of atoms from or to the probe apex. We demonstrate this by using a novel alkynyl-terminated molecule to reproducibly abstract hydrogen atoms from the probe. The approach is expected to extend to other elements and moieties, opening a new avenue for scalable atomically precise fabrication.

cond-mat.mes-hall↗

arXiv2025

Molecular Tools for Non-Planar Surface Chemistry

Scanning probe microscopy (SPM) investigations of on-surface chemistry on passivated silicon have only shown in-plane chemical reactions, and studies on bare silicon are limited in facilitating additional reactions post-molecular-attachment. Here, we enable subsequent reactions on Si(100) through selectively adsorbing 3D, silicon-specific "molecular tools". Following an activation step, the molecules present an out-of-plane radical that can function both to donate or accept molecular fragments, thereby enabling applications across multiple scales, e.g., macroscale customizable silicon-carbon coatings or nanoscale tip-mediated mechanosynthesis. Creation of many such molecular tools is enabled by broad molecular design criteria that facilitate reproducibility, surface specificity, and experimental verifiability. These criteria are demonstrated using a model molecular tool tetrakis(iodomethyl)germane ($Ge(CH_{2}I)_{4}$; TIMe-Ge), with experimental validation by SPM and X-ray photoelectron spectroscopy (XPS), and theoretical support by density functional theory (DFT) investigations. With this framework, a broad and diverse range of new molecular engineering capabilities are enabled on silicon.

cond-mat.mtrl-sci↗

arXiv2025

Multiscale Microscopy via Automation: Dual Magnification ESEM Imaging by Frame Alternation

In Environmental Scanning Electron Microscopy (ESEM) experiments, the acquisition parameters are generally kept constant throughout the collection of a data set. This limits data collection to one data set at a time, and frequent human interaction is required to maintain the image quality. Here, we use a custom-designed automation interface to minimize such supervision and allow for the collection of multiple interlaced data sets simultaneously. The oscillatory modes of an example catalytic system (hydrogen oxidation over Co foil) were employed as a tunable spatiotemporal test case. Using our automation interface, we can implement more advanced acquisition programs into the microscope that allow dual imaging - effectively bridging reaction monitoring between different length scales. By using automation to change the settings of the acquisition after each frame, we are able to capture alternating magnifications of the same process and sample location. Both a low magnification overview of the mesoscopic surface dynamics and a high magnification field of view of the ongoing structural changes of a selected surface motif were acquired. Using such truly correlative data captured with the dual magnification method, cross-scale correlations about catalytic systems including phase information can be established.

physics.ins-det↗

arXiv2013

Thermodynamic interpretation of reactive processes in Ni-Al nanolayers from atomistic simulations

Metals which can form intermetallic compounds by an exothermic reaction constitute a class of reactive materials with multiple applications. Ni-Al laminates of thin alternating layers are being considered as model nanometric metallic multilayers for studying various reaction processes. However, the reaction kinetics at short timescales after mixing are not entirely understood. In this work, we calculate the free energies of Ni-Al alloys as a function of composition and temperature for different solid phases using thermodynamic integration based on state-of-the-art interatomic potentials. We use this information to interpret molecular dynamics (MD) simulations of bilayer systems at 800 K and zero pressure, both in isothermal and isenthalpic conditions. We find that a disordered phase always forms upon mixing as a precursor to a more stable nano crystalline B2 phase. We construe the reactions observed in terms of thermodynamic trajectories governed by the state variables computed. Simulated times of up to 30 ns were achieved, which provides a window to phenomena not previously observed in MD simulations. Our results provide insight into the early experimental reaction timescales and suggest that the path (segregated reactants)$\rightarrow$(disordered phase)$\rightarrow$(B2 structure) is always realized irrespective of the imposed boundary conditions.

cond-mat.mtrl-sci↗

arXiv2013

Mesoscale computational study of the nano-crystallization of amorphous Ge via a self-consistent atomistic - phase field coupling

Germanium is the base element in many phase-change materials, i.e. systems that can undergo reversible transformations between their crystalline and amorphous phases. They are widely used in current digital electronics and hold great promise for the next generation of non-volatile memory devices. However, the ultra fast phase transformations required for these applications can be exceedingly complex even for single component systems, and a full physical understanding of these phenomena is still lacking. In this paper we study nucleation and growth of crystalline Ge from amorphous thin films at high temperature using phase field models informed by atomistic calculations of fundamental material properties. The atomistic calculations capture the full anisotropy of the Ge crystal lattice, which results in orientation dependences for interfacial energies and mobilities. These orientation relations are then exactly recovered by the phase field model at finite thickness via a novel parametrization strategy based on invariance solutions of the Allen-Cahn equations. By means of this multiscale approach, we study the interplay between nucleation and growth and find that the relation between the mean radius of the crystallized Ge grains and the nucleation rate follows simple Avrami-type scaling laws. We argue that these can be used to cover a wide region of the nucleation rate space, hence facilitating comparison with experiments.

cond-mat.mtrl-sci↗

arXiv2006

Semiclassical propagator of the Wigner function

Propagation of the Wigner function is studied on two levels of semiclassical propagation, one based on the van-Vleck propagator, the other on phase-space path integration. Leading quantum corrections to the classical Liouville propagator take the form of a time-dependent quantum spot. Its oscillatory structure depends on whether the underlying classical flow is elliptic or hyperbolic. It can be interpreted as the result of interference of a \emph{pair} of classical trajectories, indicating how quantum coherences are to be propagated semiclassically in phase space. The phase-space path-integral approach allows for a finer resolution of the quantum spot in terms of Airy functions.

quant-ph↗