Sunryu Ryu

We report the chemical reaction of single-layer graphene with hydrogen atoms, generated in situ by electron-induced dissociation of hydrogen silsesquioxane (HSQ). Hydrogenation, forming sp3 C--H functionality on the basal plane of graphene, proceeds at a higher rate for single than for double layers, demonstrating the enhanced chemical reactivity of single sheet graphene. The net H atom sticking probability on single layers at 300 K is at least 0.03, which exceeds that of double layers by at lea

We report on the existence of water-gated charge doping of graphene deposited on atomically flat mica substrates. Molecular films of water in units of ~0.4 nm thick bilayers were found to be present in regions of the interface of graphene/mica heterostacks prepared by micromechanical exfoliation of kish graphite. The spectral variation of the G and 2D bands, as visualized by Raman mapping, shows that mica substrates induce strong p-type doping in graphene with hole densities of (9 ± 2) × 10(12)

Nanometer-scale graphene objects are attracting much research interest because of newly emerging properties originating from quantum confinement effects. We present Raman spectroscopy studies of graphene nanoribbons (GNRs), which are known to have nonzero electronic bandgap. GNRs of width ranging from 15 to 100 nm have been prepared by e-beam lithographic patterning of mechanically exfoliated graphene followed by oxygen plasma etching. Raman spectra of narrow GNRs can be characterized by an upsh

Atomically thin binary two-dimensional (2D) semiconductors exhibit diverse physical properties depending on their composition, structure, and thickness. By adding another element in these materials, which will lead to formation of ternary 2D materials, the property and structure would greatly change and significantly expanded applications could be explored. In this work, we report structural and optical properties of atomically thin chromium thiophosphate (CrPS 4 ), a ternary antiferromagnetic s

Ultrathin black phosphorus (BP) is one of the promising two-dimensional (2D) materials for future optoelectronic devices. Its chemical instability in ambient conditions and lack of a bottom-up approach for its synthesis necessitate efficient etching methods that generate BP films of designed thickness with stable and high-quality surfaces. Herein, reporting a photochemical etching method, we demonstrate a controlled layer-by-layer thinning of thick BP films down to a few layers or a single layer

Chemical transformation of existing two-dimensional (2D) materials can be crucial in further expanding the 2D crystal palette required to realize various functional heterostructures. In this work, we demonstrate a 2D 'on-stack' chemical conversion of single-layer crystalline MoS2 into MoO3 with a precise layer control that enables truly 2DMoO(3) and MoO3/MoS2 heterostructures. To minimize perturbation of the 2D morphology, a nonthermal oxidation using O-2 plasma was employed. T

Even weak van der Waals (vdW) adhesion between two-dimensional solids may perturb their various materials properties owing to their low dimensionality. Although the electronic structure of graphene has been predicted to be modified by the vdW interaction with other materials, its optical characterization has not been successful. In this report, we demonstrate that Raman spectroscopy can be utilized to detect a few percent decrease in the Fermi velocity (v(F)) of graphene caused by the vdW intera

Many two-dimensional (2D) semiconductors represented by transition metal dichalcogenides have tunable optical bandgaps in the visible or near IR-range standing as a promising candidate for optoelectronic devices. Despite this potential, however, their photoreactions are not well understood or controversial in the mechanistic details. In this work, we report a unique thickness-dependent photoreaction sensitivity and a switchover between two competing reaction mechanisms in atomically thin chromiu

Second-harmonic generation (SHG) is a nonlinear optical process that converts two identical photons into a new one with doubled frequency. Two-dimensional semiconductors represented by transition-metal dichalcogenides are highly efficient SHG media because of their excitonic resonances. Using spectral phase interferometry, here we directly show that SHG in heterobilayers of MoS₂ and WS₂ is governed by optical interference between two coherent SH fields that are phase-delaye

Abstract Controlling extra charge carriers is pivotal in manipulating electronic, optical, and magnetic properties of various two-dimensional materials. Nonetheless, the ubiquitous hole doping of two-dimensional materials in the air and acids has been controversial in its mechanistic details. Here we show their common origin is an electrochemical reaction driven by redox couples of oxygen and water molecules. Using real-time photoluminescence imaging of WS 2 and Raman spectroscopy of graphene, w

Despite their importance, chemical reactions confined in a low dimensional space are elusive and experimentally intractable. In this work, we report doubly anisotropic, in-plane and out-of-plane, oxidation reactions of two-dimensional crystals, by resolving interface-confined thermal oxidation of a single and multilayer MoS 2 supported on silica substrates from their conventional surface reaction. Using optical second-harmonic generation spectroscopy of artificially stacked multilayers, we direc

Chromium thiophosphate (CrPS4), a monoclinic crystal of C23 space group, is a ternary-layered semiconductor with an optical band gap of 1.4 eV and exhibits antiferromagnetism below 36 K. Despite its potential in optoelectronic and magnetic applications, the symmetry of its lattice vibrations has not been systematically studied. In this work, we performed polarized Raman spectroscopy of bulk CrPS4 using three different excitation wavelengths of 457, 514, and 633 nm. High-quality crystals grown by

Solvation and transfer dynamics of photoinjected electrons in thin ice film coadsorbed with CFCl3 were investigated by two-photon photoemission spectroscopy. Water molecules were found to solvate the photoinjected electrons within the first several hundred femtoseconds, thus stabilizing the electron with a lifetime of ca. 120 fs for 5 ML ice film grown on Ag(111). The significant lifetime decrease upon adsorption of CFCl3 on the ice film was attributed to dissociative electron transfer of the so