arXiv subjects

Yung-Chang Lin

Publications and source records attributed to Yung-Chang Lin.

At least 19 recordsLinked to original sources

arXiv2025

Defect migration and phase transformations in 2D iron chloride inside bilayer graphene

The intercalation of metal chlorides, and particularly iron chlorides, into graphitic carbon structures has recently received lots of attention, as it can not only protect this two-dimensional (2D) magnetic system from the effects of the environment, but also substantially alter the magnetic, electronic, and optical properties of both intercalant and host material. At the same time, the intercalation can result in the formation of structural defects, or defects can appear under external stimuli, which can affect materials performance. These aspects have received so far little attention in the dedicated experiments. In this study, we investigate the behavior of atomic-scale defects in iron chlorides intercalated into bilayer graphene (BLG) by using scanning transmission electron microscopy (STEM) and first-principles calculations. We observe transformations between the FeCl2 and FeCl3 phases and elucidate the role of defects in the transformations. Specifically, three types of defects are identified: Fe vacancies in FeCl2 domains, Fe adatoms and interstitials in FeCl3 domains, each exhibiting distinct dynamic behaviors. We also observed a crystalline phase with an unusual stoichiometry of Fe5Cl18 which has not been reported before. Our findings not only advance the understanding of intercalation mechanism of 2D materials but also highlight the profound impact of atomic-scale defects on their properties and potential technological applications.

cond-mat.mtrl-sci↗

arXiv2025

Bilayer graphene as a template for manufacturing novel 2D materials

Recent intensive research on two-dimensional materials (2DMs) rekindle the interest in the intercalation of various atoms and molecules into layered compounds as a tool to manufacture 2DMs and tune their optoelectronic, magnetic and catalytic properties. Intercalation into free-standing bilayer graphene (BLG) has received special attention, as graphene is stable, chemically inert and enables one to study the atomic structure of the intercalated 2DM using high-resolution transmission electron microscopy. It was also discovered that the protecting action of graphene sheets makes it possible to not only stabilize the encapsulated single sheets of marginally stable layered materials, but also synthesize completely new 2D systems inside BLG, which in comparison to the bulk graphite allows for easier intercalation and much larger increase in the inter-layer separation of the sheets. In this review, we summarize the recent progress in this area, with a special focus on new materials created inside BLG. We compare the experimental findings to the theoretical predictions, pay special attention to the discrepancies and outline the challenges in the field. Finally, we discuss unique opportunities offered by the intercalation into 2DMs beyond graphene and their heterostructures.

cond-mat.mes-hall↗

arXiv2025

Direct observation of locally modified excitonic effect within a moir\'e unit cell in twisted bilayer graphene

Bilayer graphene, forming moir\'e superlattices, possesses distinct electronic and optical properties derived from the hybridization of energy band and the emergence of van Hove singularities depending on its twist angle. Extensive research has been conducted on the global characteristics of moir\'e superlattice induced by long-range periodicity. However, limited attention has been given to the local properties within a moir\'e unit cell, which undoubtedly differ due to the variations in three-dimensional atomic arrangement. Here we demonstrate the highly localized excitations of carbon 1s electrons to unoccupied van Hove singularities in a twisted bilayer graphene using an electron energy loss spectroscopy based on a monochromated transmission electron microscope. The core-level excitations associated with the van Hove singularities show a systematic twist angle dependence which is analogous to the optical excitations. Furthermore, local variations in those core-level van Hove singularity peaks within a moir\'e unit cell have been corroborated for the first time, which can originate from core-exciton lifetimes and band modifications influenced by the local stacking geometry.

cond-mat.mes-hall↗

arXiv2024

Lattice-guided growth of dense arrays of aligned transition metal dichalcogenide nanoribbons with high catalytic reactivity

Transition metal dichalcogenides (TMDs) exhibit unique properties and potential applications when reduced to one-dimensional (1D) nanoribbons (NRs), owing to quantum confinement and high edge densities. However, effective growth methods for self-aligned TMD NRs are still lacking. We demonstrate a versatile approach for lattice-guided growth of dense, aligned MoS2 NR arrays via chemical vapor deposition (CVD) on anisotropic sapphire substrates, without tailored surface steps. This method enables the synthesis of NRs with widths below 10 nm and longitudinal axis parallel to the zigzag direction, being also extensible to the growth of WS2 NRs and MoS2-WS2 hetero-nanoribbons. Growth is influenced by both substrate and CVD temperature, indicating the role of anisotropic precursor diffusion and substrate interaction. The 1D nature of the NRs was asserted by the observation of Coulomb blockade at low temperature. Pronounced catalytic activity was observed at the edges of the NRs, indicating their promise for efficient catalysis.

cond-mat.mes-hall↗

arXiv2024

Direct observation of the vanishing EELS cross section in graphene

In transmission electron energy-loss spectroscopy, the cross section in 2D is quenched by kinematic effects once the momentum transfer becomes smaller than a critical value set by $q_z$, the momentum loss parallel to the beam. Our highly momentum ($\Delta q = 0.02$~\r{A}$^{-1}$) and energy ($\Delta E = 45$~meV) resolved setup is instrumental on delivering the unprecedented experimental verification of quenched 2D EEL spectra on freestanding graphene at momentum transfers $q$ below $0.06$\r{A}$^{-1}$. We retrieve the intrinsic uniform dielectric response of graphene from measured spectra by quantifying the kinematic suppression.

cond-mat.mes-hall↗

arXiv2023

One-Dimensional Crystallographic Etching of Few-Layer WS$_2$

Layer number-dependent band structures and symmetry are vital for the electrical and optical characteristics of two-dimensional (2D) transition metal dichalcogenides (TMDCs). Harvesting 2D TMDCs with tunable thickness and properties can be achieved through top-down etching and bottom-up growth strategies. In this study, we report a pioneering technique that utilizes the migration of in-situ generated Na-W-S-O droplets to etch out one-dimensional (1D) nanotrenches in few-layer WS$_2$. 1D WS$_2$ nanotrenches were successfully fabricated on the optically inert bilayer WS$_2$, showing pronounced photoluminescence and second harmonic generation signals. Additionally, we demonstrate the modulation of inkjet-printed Na$_2$WO$_4$-Na$_2$SO$_4$ particles to switch between the etching and growth modes by manipulating the sulfur supply. This versatile approach enables the creation of 1D nanochannels on 2D TMDCs. Our research presents exciting prospects for the top-down and bottom-up fabrication of 1D-2D mixed-dimensional TMDC nanostructures, expanding their use for photonic and optoelectronic applications.

physics.app-ph↗

arXiv2023

Coupling and decoupling of bilayer graphene monitored by electron energy loss spectroscopy

We studied the interlayer coupling and decoupling of bilayer graphene (BLG) by using spatially resolved electron energy loss spectroscopy (EELS) with a monochromated electron source. We correlated the twist-angle-dependent energy band hybridization with Moire superlattices and the corresponding optical absorption peaks. The optical absorption peak originates from the excitonic transition between the hybridized van Hove singularities (vHSs), which shifts systematically with the twist angle. We then proved that the BLG decouples when a monolayer of metal chloride is intercalated in its van der Waals (vdW) gap, and results in the elimination of the vHS peak.

cond-mat.mtrl-sci↗

arXiv2023

Imaging of isotope diffusion using atomic-scale vibrational spectroscopy

The spatial resolutions of even the most sensitive isotope analysis techniques based on light or ion probes are limited to a few hundred nanometres. Although vibration spectroscopy using electron probes has achieved higher spatial resolution, the detection of isotopes at the atomic level has been challenging so far. Here we show the unambiguous isotopic imaging of 12C carbon atoms embedded in 13C graphene and the monitoring of their self-diffusion via atomic level vibrational spectroscopy. We first grow a domain of 12C carbon atoms in a preexisting crack of 13C graphene, which is then annealed at 600C for several hours. Using scanning transmission electron microscopy electron energy loss spectroscopy, we obtain an isotope map that confirms the segregation of 12C atoms that diffused rapidly. The map also indicates that the graphene layer becomes isotopically homogeneous over 100 nanometre regions after 2 hours. Our results demonstrate the high mobility of carbon atoms during growth and annealing via selfdiffusion. This imaging technique can provide a fundamental methodology for nanoisotope engineering and monitoring, which will aid in the creation of isotope labels and tracing at the nanoscale.

physics.atom-ph↗

arXiv2023

Excitonic effects in energy loss spectra of freestanding graphene

In this work we perform electron energy-loss spectroscopy (EELS) of freestanding graphene with high energy and momentum resolution to disentangle the quasielastic scattering from the excitation gap of Dirac electrons close to the optical limit. We show the importance of many-body effects on electronic excitations at finite transferred momentum by comparing measured EELS with ab initio calculations at increasing levels of theory. Quasi-particle corrections and excitonic effects are addressed within the GW approximation and Bethe-Salpeter equation, respectively. Both effects are essential in the description of the EEL spectra to obtain a quantitative agreement with experiments, with the position, dispersion, and shape of both the excitation gap and the $\pi$ plasmon being significantly affected by excitonic effects.

cond-mat.mtrl-sci↗

arXiv2021

Mixed-Salt Enhanced Chemical Vapor Deposition of Two-Dimensional Transition Metal Dichalcogenides

The usage of molten salts, e.g., Na2MoO4 and Na2WO4, has shown great success in the growth of two-dimensional (2D) transition metal dichalcogenides (TMDCs) by chemical vapor deposition (CVD). In comparison with the halide salt (i.e., NaCl, NaBr, KI)-assisted growth (Salt 1.0), the molten salt-assisted vapor-liquid-solid (VLS) growth technique (Salt 2.0) has improved the reproducibility, efficiency and scalability of synthesizing 2D TMDCs. However, the growth of large-area MoSe2 and WTe2 is still quite challenging with the use Salt 2.0 technique. In this study, a renewed Salt 2.0 technique using mixed salts (e.g., Na2MoO4-Na2SeO3 and Na2WO4-Na2TeO3) is developed for the enhanced CVD growth of 2D MoSe2 and WTe2 crystals with large grain size and yield. Continuous monolayer MoSe2 film with grain size of 100-250 μm or isolated flakes up to ~ 450 μm is grown on a halved 2-inch SiO2/Si wafer. Our study further confirms the synergistic effect of Na+ and SeO32- in the enhanced CVD growth of wafer-scale monolayer MoSe2 film. And thus, the addition of Na2SeO3 and Na2TeO3 into the transition metal salts could be a general strategy for the enhanced CVD growth of many other 2D selenides and tellurides.

cond-mat.mtrl-sci↗

arXiv2021

Tunable Doping of Rhenium and Vanadium into Transition Metal Dichalcogenides for Two-Dimensional Electronics

Two-dimensional (2D) transition metal dichalcogenides (TMDCs) with unique electrical properties are fascinating materials used for future electronics. However, the strong Fermi level pinning effect at the interface of TMDCs and metal electrodes always leads to high contact resistance, which seriously hinders their application in 2D electronics. One effective way to overcome this is to use metallic TMDCs or transferred metal electrodes as van der Waals (vdW) contacts. Alternatively, using highly conductive doped TMDCs will have a profound impact on the contact engineering of 2D electronics. Here, a novel chemical vapor deposition using mixed molten salts is established for vapor-liquid-solid growth of high-quality rhenium (Re) and vanadium (V)-doped TMDC monolayers with high controllability and reproducibility. A tunable semiconductor to metal transition is observed in the Re and V-doped TMDCs. Electrical conductivity increases up to a factor of 108 in the degenerate V-doped WS2 and WSe2. Using V-doped WSe2 as vdW contact, the on-state current and on/off ratio of WSe2-based field-effect transistors have been substantially improved (from ~10-8 to 10-5 A; ~104 to 108), compared to metal contacts. Future studies on lateral contacts and interconnects using doped TMDCs will pave the way for 2D integrated circuits and flexible electronics.

cond-mat.mtrl-sci↗

arXiv2019

Does the metallic 1T phase WS2 really exist?

The electronic and optical properties of transition metal dichalcogenides (TMDCs) in distinctive phases, such as 1H, 1T, and 1T' phases, are of fundamental importance for variety of applications. The 1H phase has been understood as a direct bandgap semiconductor. On the other hand, the electronic properties of the 1T and 1T' phases remain controversy in the theoretical and experimental perspectives. In this study, we explore the optical properties of monolayer WS2 in 1H, 1T, and 1T' phases using Raman and photoluminescence, corroborated with the atomic structure identified by scanning transmission electron microscopy. Despite of earlier theoretical investigations which all predict the metallic 1T phase, we experimentally discovered that the 1T-phase WS2 is a direct band gap semiconductor and optically indistinguishable from the 1H phase. In a sharp contrast, the 1T'-phase WS2 shows a gapless nature in its bandstructure with the quenched exciton transition as expected. Our experimental findings may give an interesting twist on the existing literatures reporting the metallic nature of 1T phase because the 1T phase has a strong tendency to co-exist with the metallic 1T' phase.

cond-mat.mtrl-sci↗

arXiv2019

Wafer-Scale and Deterministic Patterned Growth of Monolayer MoS2 via Vapor-Liquid-Solid Method

Vapor transportation is the core process in growing transition-metal dichalcogenides (TMDCs) by chemical vapor deposition (CVD). One inevitable problem is the spatial inhomogeneity of the vapors. The non-stoichiometric supply of transition-metal precursors and chalcogen leads to poor control in products' location, morphology, crystallinity, uniformity and batch to batch reproducibility. While vapor-liquid-solid (VLS) growth involves molten precursors at the growth temperatures higher than their melting points. The liquid sodium molybdate can precipitate solid MoS2 monolayers when saturated with sulfur vapor. Taking advantage of the VLS growth, we achieved three kinds of important achievements: (a) 4-inch-wafer-scale uniform growth of MoS2 flakes on SiO2/Si substrates, (b) 2-inch-wafer-scale growth of continuous MoS2 film with a grain size exceeding 100 um on sapphire substrates, and (c) pattern (site-controlled) growth of MoS2 flakes and film. We clarified that the VLS growth thus pave the new way for the high-efficient, scalable synthesis of two-dimensional TMDC monolayers.

cond-mat.mtrl-sci↗

arXiv2019

Exciton mapping at subwavelength scales in two-dimensional materials

Spatially resolved EELS has been performed at diffuse interfaces between MoS$_2$ and MoSe$_2$ single layers. With a monochromated electron source (20 meV) we have successfully probed excitons near the interface by obtaining the low loss spectra at the nanometer scale. The exciton maps clearly show variations even with a 10 nm separation between measurements; consequently the optical bandgap can be measured with nanometer-scale resolution, which is 50 times smaller than the wavelength of the emitted photons. By performing core-loss EELS at the same regions, we observe that variations in the excitonic signature follow the chemical composition. The exciton peaks are observed to be broader at interfaces and heterogeneous regions, possibly due to interface roughness and alloying effects. Moreover, we do not observe shifts of the exciton peak across the interface, possibly because the interface width is not much larger than the exciton Bohr radius.

cond-mat.mes-hall↗

arXiv2019

Momentum Conserved Ultrafast Charge Transfer Dynamics of Interlayer Excitons in vdW Heterostructures

Heterostructures comprising van der Waals (vdW) stacked transition metal dichalcogenide (TMDC) monolayers are a fascinating class of two-dimensional (2D) materials with unique properties. The presence of interlayer excitons, where the electron and the hole remain spatially separated in the two layers due to ultrafast charge transfer, is an intriguing feature of these heterostructures. Inevitably, the efficiency of 2D heterostructure devices is critically dependent on the charge transfer dynamics. However, the role of the relative rotation angle of the constituent layers on this charge transfer dynamics is hitherto unknown. Here, we investigate MoS$_2$/WSe$_2$ vdW heterostructures (hMWs) using monochromated low-loss electron energy loss (EEL) spectroscopy combined with aberration-corrected scanning transmission electron microscopy (STEM), and report that momentum conservation is a critical factor in the charge transfer dynamics of TMDC vdW heterostructures. The low-loss EEL spectra of the heterostructures with various rotation angles reveal that the charge transfer rate can be about one order-of-magnitude faster in the aligned (or anti-aligned) case than the misaligned cases. These results provide a deeper insight into the role of the fundamental principle of momentum conservation in 2D vdW heterostructure charge transfer dynamics.

cond-mat.mes-hall↗

arXiv2018

Vapor-Liquid-Solid Growth of Monolayer MoS2 Nanoribbons

Chemical vapor deposition (CVD) of two-dimensional (2D) materials such as monolayer MoS2 typically involves the conversion of vapor-phase precursors to a solid product in a process that may be described as a vapor-solid-solid (VSS) mode. Here, we report the first demonstration of vapor-liquid-solid (VLS) growth of monolayer MoS2 yielding highly crystalline ribbon-shaped structures with a width of a few tens of nanometers to a few micrometers. The VLS growth mode is triggered by the reaction between molybdenum oxide and sodium chloride, which results in the formation of molten Na-Mo-O droplets. These droplets mediate the growth of MoS2 ribbons in the "crawling mode" when saturated with sulfur on a crystalline substrate. Our growth yields straight and kinked ribbons with a locally well-defined orientation, reflecting the regular horizontal motion of the liquid droplets during growth. Using atomic-resolution scanning transmission electron microscopy (STEM) and second harmonic generation (SHG) microscopy, we show that the ribbons are homoepitaxially on monolayer MoS2 surface with predominantly 2H- or 3R-type stacking. These findings pave the way to novel devices with structures of mixed dimensionalities.

cond-mat.mtrl-sci↗

arXiv2017

Towards atomically precise manipulation of 2D nanostructures in the electron microscope

Despite decades of research, the ultimate goal of nanotechnology--top-down manipulation of individual atoms--has been directly achieved with only one technique: scanning probe microscopy. In this Review, we demonstrate that scanning transmission electron microscopy (STEM) is emerging as an alternative method for the direct assembly of nanostructures, with possible applications in plasmonics, quantum technologies, and materials science. Atomically precise manipulation with STEM relies on recent advances in instrumentation that have enabled non-destructive atomic-resolution imaging at lower electron energies. While momentum transfer from highly energetic electrons often leads to atom ejection, interesting dynamics can be induced when the transferable kinetic energies are comparable to bond strengths in the material. Operating in this regime, very recent experiments have revealed the potential for single-atom manipulation using the Angstrom-sized electron beam. To truly enable control, however, it is vital to understand the relevant atomic-scale phenomena through accurate dynamical simulations. Although excellent agreement between experiment and theory for the specific case of atomic displacements from graphene has been recently achieved using density functional theory molecular dynamics, in many other cases quantitative accuracy remains a challenge. We provide a comprehensive reanalysis of available experimental data on beam-driven dynamics in light of the state-of-the-art in simulations, and identify important targets for improvement. Overall, the modern electron microscope has great potential to become an atom-scale fabrication platform, especially for covalently bonded 2D nanostructures. We review the developments that have made this possible, argue that graphene is an ideal starting material, and assess the main challenges moving forward.

cond-mat.mtrl-sci↗

arXiv2014

The structure and local chemical properties of boron-terminated tetravacancies in hexagonal boron-nitride

Imaging and spectroscopy performed in a low-voltage scanning transmission electron microscope (LV-STEM) are used to characterize the structure and chemical properties of boron-terminated tetravacancies in hexagonal boron nitride (h-BN). We confirm earlier theoretical predictions about the structure of these defects and identify new features in the electron energy-loss spectra (EELS) of B atoms using high resolution chemical maps, highlighting differences between these areas and pristine sample regions. We correlate our experimental data with calculations which help explain our observations.

cond-mat.mtrl-sci↗