arXiv subjects

Ing-Shouh Hwang

Publications and source records attributed to Ing-Shouh Hwang.

17 recordsLinked to original sources

arXiv2024

Crystalline Water Structure in Room-Temperature Clathrate State: Hydrogen-Bonded Pentagonal Rings

Water hydrogen bonding is extremely versatile; approximately 20 ice structures and several types of clathrate hydrate structures have been identified. These crystalline water structures form at temperatures below room temperature and/or at high pressure. We used transmission electron microscopy to study a new crystalline water structure in a clathrate state that is prepared by sandwiching gas-supersaturated water between graphene layers under ambient conditions. In this clathrate state, water molecules form a three-dimensional hydrogen bonding network that encloses gas-filled cages 2-4 nm in size. We derived the crystalline water structure by recording and analyzing electron diffraction patterns and performing first-principles calculations. The structure consists purely of pentagonal rings and has a topology similar to that of water ice XVII. The study proposed a mechanism for the formation of the clathrate state. The present results improve the understanding of interactions among water and small nonpolar molecules and offer novel insights into the local structures of ambient liquid water.

cond-mat.mtrl-sci↗

arXiv2024

Formation of highly stable interfacial nitrogen gas hydrate overlayers under ambient conditions

Surfaces (interfaces) dictate many physical and chemical properties of solid materials and adsorbates considerably affect these properties. Nitrogen molecules, which are the most abundant constituent in ambient air, are considered to be inert. Our study combining atomic force microscopy (AFM), X-ray photoemission spectroscopy (XPS), and thermal desorption spectroscopy (TDS) revealed that nitrogen and water molecules can self-assemble into two-dimensional domains, forming ordered stripe structures on graphitic surfaces in both water and ambient air. The stripe structures of this study were composed of approximately 90% and 10% water and nitrogen molecules, respectively, and survived in ultra-high vacuum (UHV) conditions at temperatures up to approximately 350 K. Because pure water molecules completely desorb from graphitic surfaces in a UHV at temperatures lower than 200 K, our results indicate that the incorporation of nitrogen molecules substantially enhanced the stability of the crystalline water hydrogen bonding network. Additional studies on interfacial gas hydrates can provide deeper insight into the mechanisms underlying formation of gas hydrates.

cond-mat.mtrl-sci↗

arXiv2022

Superconducting Niobium Tip Electron Beam Source

Modern electron microscopy and spectroscopy is a key technology for studying the structure and composition of quantum and biological materials in fundamental and applied sciences. High-resolution spectroscopic techniques and aberration-corrected microscopes are often limited by the relatively large energy distribution of currently available beam sources. This can be improved by a monochromator, with the significant drawback of losing most of the beam current. Here, we study the field emission properties of a monocrystalline niobium tip electron field emitter at 5.2 K, well below the superconducting transition temperature. The emitter fabrication process can generate two tip configurations, with or without a nano-protrusion at the apex, strongly influencing the field-emission energy distribution. The geometry without the nano-protrusion has a high beam current, long-term stability, and an energy width of around 100 meV. The beam current can be increased by two orders of magnitude by xenon gas adsorption. We also studied the emitter performance up to 82 K and demonstrated the beam's energy width can be below 40 meV even at liquid nitrogen cooling temperatures when an apex nano-protrusion is present. Furthermore, the spatial and temporal electron-electron correlations of the field emission are studied at normal and superconducting temperatures and the influence of Nottingham heating is discussed. This new monochromatic source will allow unprecedented accuracy and resolution in electron microscopy, spectroscopy, and high-coherence quantum applications.

physics.app-ph↗

arXiv2022

Observation of Mesoscopic Clathrate Structures in Ethanol-Water Mixtures

Water-alcohol mixtures exhibit many abnormal physicochemical properties, the origins of which remain controversial. Here we use transmission electron microscopy (TEM), nanoparticle tracking analysis (NTA), and atomic force microscopy (AFM) to study ethanol-water mixtures. TEM reveals mesoscopic clathrate structures with water molecules forming a crystalline matrix hosting a high density of tiny cells. The presence of these mesoscopic clathrate structures is further supported by a refractive index of 1.27+-0.02 at 405 nm measured via NTA and the hydrophilic nature of the mesoscopic structures implied by AFM observations, explaining many long-standing puzzles related to water-alcohol mixtures.

cond-mat.mes-hall↗

arXiv2017

Coherent properties of a tunable low energy electron matter wave source

A general challenge in various quantum experiments and applications is to develop suitable sources for coherent particles. In particular, recent progress in microscopy, interferometry, metrology, decoherence measurements and chip based applications rely on intensive, tunable, coherent sources for free low energy electron matter waves. In most cases, the electrons get field emitted from a metal nanotip where its radius and geometry towards a counter electrode determines the field distribution and the emission voltage. A higher emission is often connected to faster electrons with smaller de Broglie wavelengths, requiring larger pattern magnification after matter wave diffraction or interferometry. This can be prevented with a well-known setup consisting of two counter electrodes that allow independent setting of the beam intensity and velocity. However, it needs to be tested if the coherent properties of such a source are preserved after the acceleration and deceleration of the electrons. Here, we study the coherence of the beam in a biprism interferometer with a single atom tip electron field emitter if the particle velocity and wavelength varies after emission. With a Wien filter measurement and a contrast correlation analysis we demonstrate that the intensity of the source at a certain particle wavelength can be enhanced up to a factor of 33 without changing the transverse and longitudinal coherence of the electron beam. In addition, the energy width of the single atom tip emitter was measured to be 377 meV, corresponding to a longitudinal coherence length of 82 nm. The design has potential applications in interferometry, microscopy and sensor technology

quant-ph↗

arXiv2017

Adsorption and dynamics of Si atoms at the monolayer Pb/Si(111) surface

In this work, we studied the adsorption behavior of deposited Si atoms along with their diffusion and other dynamic processes on a Pb monolayer-covered Si(111) surface from 125-230 K using a variable-temperature scanning tunneling microscope (STM). The Pb-covered Si(111) surface form a low-symmetry row-like structure in this temperature range and the Si atoms bind favorably to two specific on-top sites (T1A and T1B) on the trimer row after deposition at the sample temperature of 125 K. The Si atoms were immobile at low temperatures and started to switch between the two neighboring T1A and T1B sites within the same trimer when the temperature was raised to 150 K. When the temperature was raised above 160 K, the adsorbed Si atoms could hop to other trimers along the same trimer row. Below 170 K, short hops to adjacent trimers dominated, but long hops dominated at temperatures above 170 K. The activation energy and prefactor for the Si atoms diffusion were derived through analysis of continuous-time imaging at temperatures from 160-174 K. In addition, irreversible aggregation of single Si atoms into Si clusters started to occur at the phase boundaries or defective sites at temperatures above 170 K. This study provides crucial information for understanding the very initial stage of nucleation and growth behavior of epitaxial Si layers on a Pb-covered Si(111) surface. In addition, our study provides strong evidence for breaking in the mirror symmetry in the Pb-covered structure, which has implication for the atomic model of this controversial structure.

cond-mat.mes-hall↗

arXiv2017

Vibrational dephasing in matter-wave interferometers

Matter-wave interferometry is a highly sensitive tool to measure small perturbations in a quantum system. This property allows the creation of precision sensors for dephasing mechanisms such as mechanical vibrations. They are a challenge for phase measurements under perturbing conditions that cannot be perfectly decoupled from the interferometer, e.g. for mobile interferometric devices or vibrations with a broad frequency range. Here, we demonstrate a method based on second-order correlation theory in combination with Fourier analysis, to use an electron interferometer as a sensor that precisely characterizes the mechanical vibration spectrum of the interferometer. Using the high spatial and temporal single-particle resolution of a delay line detector, the data allows to reveal the original contrast and spatial periodicity of the interference pattern from "washed-out" matter-wave interferograms that have been vibrationally disturbed in the frequency region between 100 and 1000 Hz. Other than with electromagnetic dephasing, due to excitations of higher harmonics and additional frequencies induced from the environment, the parts in the setup oscillate with frequencies that can be different to the applied ones. The developed numerical search algorithm is capable to determine those unknown oscillations and corresponding amplitudes. The technique can identify vibrational dephasing and decrease damping and shielding requirements in electron, ion, neutron, atom and molecule interferometers that generate a spatial fringe pattern on the detector plane.

quant-ph↗

arXiv2017

Three-dimensional surface topography of graphene by divergent beam electron diffraction

There is only a handful of scanning techniques that can provide surface topography at nanometre resolution. At the same time, there are no methods that are capable of non-invasive imaging of the three-dimensional surface topography of a thin free-standing crystalline material. Here we propose a new technique - the divergent beam electron diffraction (DBED) and show that it can directly image the inhomogeneity in the atomic positions in a crystal. Such inhomogeneities are directly transformed into the intensity contrast in the first order diffraction spots of DBED patterns and the intensity contrast linearly depends on the wavelength of the employed probing electrons. Three-dimensional displacement of atoms as small as 1 angstrom can be detected when imaged with low-energy electrons (50 - 250 eV). The main advantage of DBED is that it allows visualisation of the three-dimensional surface topography and strain distribution at the nanometre scale in non-scanning mode, from a single shot diffraction experiment.

physics.ins-det↗

arXiv2016

Preferential Gas Adsorption at the Graphene-Water interface

The contact of water with graphene is of fundamental importance and of great interest for numerous promising applications, but how graphene interacts with water remains unclear. Here we used atomic force microscopy to investigate hydrophilic mica substrates with some regions covered by mechanically exfoliated graphene layers in water. In water containing air gas close to the saturation concentration (within ~40%), cap-shaped nanostructures and ordered stripe domains were observed on graphene-covered regions, but not on pure mica regions. These structures did not appear on graphene when samples were immersed in highly degassed water, indicating that their formation was caused by adsorption of gas dissolved in water. Thus, atomically thin graphene, even at a narrow width of 20 nm, changes the local surface chemistry of a highly hydrophilic substrate. Further, surface hydrophobicity significantly affects gas adsorption, which has broad implications for diverse phenomena in water.

cond-mat.mes-hall↗

arXiv2016

Proximity Scanning Transmission Electron Microscopy/Spectroscopy

Here a new microscopic method is proposed to image and characterize very thin samples like few-layer materials, organic molecules, and nanostructures with nanometer or sub-nanometer resolution using electron beams of energies lower than 20 eV. The microscopic technique achieves high resolution through the proximity (or near-field) effect, as in scanning tunneling microscopy (STM), while it also allows detection of transmitted electrons for imaging and spectroscopy, as in scanning transmission electron microscopy (STEM). This proximity transmission electron microscopy (PSTEM) does not require any lens to focus the electron beam. It also allows detailed characterization of the interaction of low-energy electron with materials. PSTEM can operate in a way very similar to scanning tunneling microscopy, which provides high-resolution imaging of geometric and electronic structures of the sample surface. In addition, it allows imaging and characterization of the interior structures of the sample based on the detected transmission electron signals. PSTEM comprises a family of spectroscopies that address the transport and scattering of low-energy electrons in materials. Thus rich information can be extracted from the measurements. PSTEM offers a fundamentally new and powerful way to investigate thin materials. New analysis methods of thin materials and new physics may be uncovered by this method.

physics.ins-det↗

arXiv2015

Low-voltage coherent electron imaging based on a single-atom electron

It has been a general trend to develop low-voltage electron microscopes due to their high imaging contrast of the sample and low radiation damage. Atom-resolved transmission electron microscopes with voltages as low as 15-40 kV have been demonstrated. However, achieving atomic resolution at voltages lower than 10 kV is extremely difficult. An alternative approach is coherent imaging or phase retrieval imaging, which requires a sufficiently coherent source and an adequately small detection area on the sample as well as the detection of high-angle diffracted patterns with a sufficient resolution. In this work, we propose several transmission-type schemes to achieve coherent imaging of thin materials (less than 5 nm thick) with atomic resolution at voltages lower than 10 kV. Experimental schemes of both lens-less and lens-containing designs are presented and the advantages and challenges of these schemes are discussed. Preliminary results based on a highly coherent single-atom electron source are presented. The image plate is designed to be retractable to record the transmission patterns at different positions along the beam propagation direction. In addition, reflection-type coherent electron imaging schemes are also proposed as novel methods for characterizing surface atomic and electronic structures of materials.

physics.ins-det↗

arXiv2015

How Nanobubbles Nucleate at a Hydrophobic/Water Interface

Experimental investigations of hydrophobic/water interfaces often return controversial results, possibly due to the unknown role of gas accumulation at the interfaces. Here, during advanced atomic force microscopy of the initial evolution of gas-containing structures at a highly ordered pyrolytic graphite/water interface, a fluid phase first appeared as a circular wetting layer ~0.3 nm in thickness and was later transformed into a cap-shaped nanostructure (an interfacial nanobubble). Two-dimensional ordered domains were nucleated and grew over time outside or at the perimeter of the fluid regions, eventually confining growth of the fluid regions to the vertical direction. We determined that interfacial nanobubbles and fluid layers have very similar mechanical properties, suggesting low interfacial tension with water and a liquid-like nature, explaining their high stability and their roles in boundary slip and bubble nucleation. These ordered domains may be the interfacial hydrophilic gas hydrates and/or the long-sought chemical surface heterogeneities responsible for contact line pinning and contact angle hysteresis. The gradual nucleation and growth of hydrophilic ordered domains renders the original homogeneous hydrophobic/water interface more heterogeneous over time, which would have great consequence for interfacial properties that affect diverse phenomena, including interactions in water, chemical reactions, and the self-assembly and function of biological molecules.

cond-mat.mes-hall↗

arXiv2015

Nucleation and Growth Mechanism of a Covalent Material: Magic Clusters and Chemical Reactions

With scanning tunneling microscopy, we study the very early stage of Si deposition on a Pb monolayer covered Si(111) surface. We find a special type of Si magic clusters which are highly mobile on the defect-free surface but may be trapped temporarily at certain boundary or defect sites. They may also aggregate and a special aggregate arrangement is found to be stable for one to two days at room temperature. Adding more Si on the cluster aggregate can transform it into a metastable structure. A scenario based on magic clusters and their chemical reactions is proposed to describe the nucleation and growth processes of covalent materials.

cond-mat.mtrl-sci↗

arXiv2014

Interface-Induced Ordering of Gas Molecules Confined in a Small Space

The thermodynamic properties of gases have been understood primarily through phase diagrams of bulk gases. However, observations of gases confined in a nanometer space have posed a challenge to the principles of classical thermodynamics. Here, we investigated interfacial structures comprising either O2 or N2 between water and a hydrophobic solid surface by using advanced atomic force microscopy techniques. Ordered epitaxial layers and cap-shaped nanostructures were observed. In addition, pancake-shaped disordered layers that had grown on top of the epitaxial base layers were observed in oxygen-supersaturated water. We propose that hydrophobic solid surfaces provide low-chemical-potential sites at which gas molecules dissolved in water can be adsorbed. The structures are further stabilized by interfacial water. Gas molecules can agglomerate into a condensed form when confined in a sufficiently small space under ambient conditions. The ordering and thermodynamic properties of the confined gases are determined primarily according to interfacial interactions. The crystalline solid surface may even induce a solid-gas state.

cond-mat.soft↗

arXiv2014

Correction of dephasing oscillations in matter wave interferometry

Vibrations, electromagnetic oscillations and temperature drifts are among the main reasons for dephasing in matter-wave interferometry. Sophisticated interferometry experiments, e.g. with ions or heavy molecules, often require integration times of several minutes due to the low source intensity or the high velocity selection. Here we present a scheme to suppress the influence of such dephasing mechanisms - especially in the low-frequency regime - by analyzing temporal and spatial particle correlations available in modern detectors. Such correlations can reveal interference properties that would otherwise be washed out due to dephasing by external oscillating signals. The method is shown experimentally in a biprism electron interferometer where a perturbing oscillation is artificially introduced by a periodically varying magnetic field. We provide a full theoretical description of the particle correlations where the perturbing frequency and amplitude can be revealed from the disturbed interferogram. The original spatial fringe pattern without the perturbation can thereby be restored. The technique can be applied to lower the general noise requirements in matter-wave interferometers. It allows for the optimization of electromagnetic shielding and decreases the efforts for vibrational or temperature stabilization.

quant-ph↗

arXiv2013

Biprism Electron Interferometry with a Single Atom Tip Source

Experiments with electron or ion matter waves require a coherent, monochromatic and long-term stable source with high brightness. These requirements are best fulfilled by single atom tip (SAT) field emitters. The performance of an iridium covered W(111) SAT is demonstrated and analyzed for electrons in a biprism interferometer. Furthermore we characterize the emission of the SAT in a separate field electron and field ion microscope and compare it with other emitter types. A new method is presented to fabricate the electrostatic charged biprism wire that separates and combines the matter wave. In contrast to other biprism interferometers the source and the biprism size are well defined within a few nanometers. The setup has direct applications in ion interferometry and Aharonov-Bohm physics.

physics.optics↗

arXiv2012

Evidence of Epitaxial Growth of Molecular Layers of Dissolved Gas at a Hydrophobic/Water Interface

The non-wetting phenomena of water on certain solid surfaces have been under intensive study for decades, but the nature of hydrophobic/water interfaces remains controversial. Here a water/graphite interface is investigated with high-sensitivity atomic force microscopy. We show evidence of nucleation and growth of an epitaxial monolayer on the graphite surface, probably caused by adsorption of nitrogen molecules dissolved in water. The subsequent adsorption process resembles the layer-plus-island, or Stranski-Krastanov, growth mode in heteroepitaxy. This finding underlines the importance of gas segregation at various water interfaces and may unravel many puzzles, especially the nature and the high stability of so-called nanobubbles at solid/water interfaces and in bulk water. Based on the hydrophobic effect, we propose that gas molecules dissolved in water may aggregate into clusters in bulk water as well as at solid/water interfaces. As a cluster grows above a critical size, it undergoes a transition into a gas bubble, which can explain formation or nucleation of gas bubbles in water.

cond-mat.soft↗