arXiv subjects

Junqiao Wu

Publications and source records attributed to Junqiao Wu.

At least 19 recordsLinked to original sources

arXiv2023

Proton Collective Quantum Tunneling Induces Anomalous Thermal Conductivity of Ice under Pressure

Proton tunneling is believed to be non-local in ice but has never been shown experimentally. Here we measured thermal conductivity of ice under pressure up to 50 GPa and found it to increase with pressure until 20 GPa but decrease at higher pressures. We attribute this anomalous drop of thermal conductivity to the collective tunneling of protons at high pressures, supported by large-scale quantum molecular dynamics simulations. The collective tunneling loops span several picoseconds in time and are as large as nanometers in space, which match the phonon periods and wavelengths, leading to strong phonon scattering at high pressures. Our results show direct evidence of collective quantum motion existing in high-pressure ice and provide a new perspective to understanding the coupling between phonon propagation and atomic tunneling.

physics.chem-ph↗

arXiv2022

Ultrafast optical nanoscopy of carrier dynamics in silicon nanowires

Carrier distribution and dynamics in semiconductor materials often govern their physical properties that are critical to functionalities and performance in industrial applications. The continued miniaturization of electronic and photonic devices calls for tools to probe carrier behavior in semiconductors simultaneously at the picosecond time and nanometer length scales. Here, we report pump-probe optical nanoscopy in the visible-near-infrared spectral region to characterize the carrier dynamics in silicon nanostructures. By coupling experiments with the point-dipole model, we resolve the size-dependent photoexcited carrier lifetime in individual silicon nanowires. We further demonstrate local carrier decay time mapping in silicon nanostructures with a sub-50 nm spatial resolution. Our study enables the nanoimaging of ultrafast carrier kinetics, which will find promising applications in the future design of a broad range of electronic, photonic, and optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2022

Vapor-liquid-solid growth of highly-mismatched semiconductor nanowires with high-fidelity van der Waals layer stacking

Nanobelts, nanoribbons and other quasi-one-dimensional nanostructures formed from layered, so-called, van der Waals semiconductors have garnered much attention due to their high-performance, tunable optoelectronic properties. For layered alloys made from the gallium monochalcogenides GaS, GaSe, and GaTe, near-continuous tuning of the energy bandgap across the full composition range has been achieved in GaSe1-xSx and GaSe1-xTex alloys. Gold-catalyzed vapor-liquid-solid (VLS) growth of these alloys yields predominantly nanobelts, nanoribbons and other nanostructures for which the fast crystal growth front consists of layer edges in contact with the catalyst. We demonstrate that in the S-rich, GaS1-xTex system, unlike GaSe1-xSx and GaSe1-xTex, the Au-catalyzed VLS process yields van der Waals nanowires for which the fast growth direction is normal to the layers. The high mismatch between S and Te leads to extraordinary bowing of the GaS1-xTex alloy's energy bandgap, decreasing by at least 0.6 eV for x as small as 0.03. Calculations using density functional theory confirm the significant decrease in bandgap in S-rich GaS1-xTex. The nanowires can exceed fifty micrometers in length, consisting of tens of thousands of van der Waals-bonded layers with triangular or hexagonal cross-sections of uniform dimensions along the length of the nanowire. We propose that the low solubility of Te in GaS results in an enhancement in Te coverage around the Au catalyst-nanowire interface, confining the catalyst to the chalcogen-terminated basal plane (rather than the edges) and thereby enabling layer-by-layer, c-axis growth.

cond-mat.mtrl-sci↗

arXiv2022

Incoherent phonon transport dominates heat conduction across van der Waals superlattices

Heat conduction mechanisms in superlattices could be different across different types of interfaces. Van der Waals superlattices are structures physically assembled through weak van der Waals interactions by design, and may host properties beyond the traditional limits of lattice matching and processing compatibility, offering new types of interfaces. In this work, natural van der Waals (SnS)1.17(NbS2)n superlattices are synthesized, and their thermal conductivities are measured by time-domain thermoreflectance as a function of interface density. Our results show that heat conduction of (SnS)1.17(NbS2)n superlattices is dominated by interface scattering when the coherent length of phonons is larger than the superlattice period, indicating incoherent phonon transport dominates cross-plane heat conduction in van der Waals superlattices even when the period is atomically thin and abrupt. Moreover, our result suggests that the widely accepted heat conduction mechanism for conventional superlattices that coherent phonons dominate when the period is short, is not applicable due to symmetry breaking in most van der Waals superlattices. Our findings provide new insight for understanding the thermal behavior of van der Waals superlattices, and devise approaches for effective thermal management of superlattices depending on the distinct types of interfaces.

cond-mat.mtrl-sci↗

arXiv2021

Charge Carrier Transport in Iron Pyrite Thin Films: Disorder Induced Variable Range Hopping

The origin of p-type conductivity and the mechanism responsible for low carrier mobility was investigated in pyrite (FeS2) thin films. Temperature dependent resistivity measurements were performed on polycrystalline and nanostructured thin films prepared by three different methods. Films have a high hole density and low mobility regardless of the method used for their preparation. The charge transport mechanism is determined to be nearest neighbour hopping (NNH) at near room temperature with Mott-type variable range hopping (VRH) of holes via localized states occurring at lower temperatures. Density functional theory (DFT) predicts that sulfur vacancy induced localized defect states will be situated within the band gap with the charge remaining localized around the defect. The data indicate that the electronic properties including hopping transport in pyrite thin films can be correlated to sulfur vacancy related defect. The results provide insights on electronic properties of pyrite thin films and its implications for charge transport

cond-mat.mtrl-sci↗

arXiv2020

Chemical trends of deep levels in van der Waals semiconductors

Properties of semiconductors are largely defined by crystal imperfections including native defects. Van der Waals (vdW) semiconductors, a newly emerged class of materials, are no exception: defects exist even in the purest materials and strongly affect their electrical, optical, magnetic, catalytic and sensing properties. However, unlike conventional semiconductors where energy levels of defects are well documented, they are experimentally unknown in even the best studied vdW semiconductors, impeding the understanding and utilization of these materials. Here, we directly evaluate deep levels and their chemical trends in the bandgap of MoS2, WS2 and their alloys by transient spectroscopic study. One of the deep levels is found to follow the conduction band minimum of each host, attributed to the native sulfur vacancy. A switchable, DX center - like deep level has also been identified, whose energy lines up instead on a fixed level across different hosts, explaining a persistent photoconductivity above 400K.

cond-mat.mtrl-sci↗

arXiv2020

Nanoscale-femtosecond dielectric response of Mott insulators captured by two-colour near-field ultrafast electron microscopy

Characterizing and controlling the out-of-equilibrium state of nanostructured Mott insulators hold great promises for emerging quantum technologies while providing an exciting playground for investigating fundamental physics of strongly-correlated systems. Here, we use two-colour near-field ultrafast electron microscopy to photo-induce the insulator-to-metal transition in a single VO2 nanowire and probe the ensuing electronic dynamics with combined nanometer-femtosecond resolution. We take advantage of a femtosecond temporal gating of the electron pulse mediated by an infrared laser pulse, and exploit the sensitivity of inelastic electron-light scattering to changes in the material dielectric function. By spatially mapping the near-field dynamics of an individual nanowire of VO2, we observe that ultrafast photo-doping drives the system into a metallic state on a time scale of about 150 fs without yet perturbing the crystalline lattice. Due to the high versatility and sensitivity of the electron probe, our method would allow capturing the electronic dynamics of a wide range of nanoscale materials with ultimate spatio-temporal resolution.

physics.app-ph↗

arXiv2019

Synthesis and electronic structure characterization of diamane

Atomically thin graphite, known as graphene, has been a marvel in material science because of its exceptional properties, novel physics and promising applications. Atomically thin diamond, called diamane, has also attracted considerable scientific interest due to its potential physical and mechanical properties. However, until now there has been no reports of successful synthesis of a free-standing pristine diamane film. Here, we report the synthesis and electronic structure characterization of diamane. Electrical measurements, x-ray diffraction and theoretical simulations reveal that trilayer and thicker graphene transform to hexagonal diamane (h-diamane) when compressed to above 20 GPa, which can be preserved down to few GPa. Raman studies indicate that the sample quenched from high pressure and high temperature also has a h-diamane structure, i.e., h-diamane is recovered back to ambient conditions. Optical absorption and band structure calculations reveal an indirect energy gap of 2.8 eV in the diamane film. Compared to gapless graphene, diamane with sizable bandgap may open up new applications of carbon semiconductors.

cond-mat.mtrl-sci↗

arXiv2018

Black Arsenic: A Layered Semiconductor with Extreme in-plane Anisotropy

Two-dimensional (2D) layered materials emerge in recent years as a new platform to host novel electronic, optical or excitonic physics and develop unprecedented nanoelectronic and energy applications. By definition, these materials are strongly anisotropic between within the basal plane and cross the plane. The structural and property anisotropies inside their basal plane, however, are much less investigated. Herein, we report a rare chemical form of arsenic, called black-arsenic (b-As), as an extremely anisotropic layered semiconductor. We have performed systematic characterization on the structural, electronic, thermal and electrical properties of b-As single crystals, with particular focus on its anisotropies along two in-plane principle axes, armchair (AC) and zigzag (ZZ). Our analysis shows that b-As exhibits higher or comparable electronic, thermal and electric transport anisotropies between the AC and ZZ directions than any other known 2D crystals. Such extreme in-plane anisotropies are able to potentially implement novel ideas for scientific research and device applications.

cond-mat.mtrl-sci↗

arXiv2017

Subcycle insulator-to-metal transition in vanadium dioxide by terahertz-field-driven tunneling

In vanadium dioxide, the interplay between coherent lattice transformation and electronic correlation drives an insulator-to-metal transition (IMT). This phase commutation can be triggered by temperature, pressure, doping or deposition of optical energy. Here we demonstrate that an atomically-strong terahertz electric field initiates a metastable ultrafast IMT in vanadium dioxide without a concomitant lattice transformation. The free-space terahertz field acts as off-resonant excitation with photon energy below the lattice phonons and the interband transitions. Differently from optical and infrared excitation, terahertz interaction leads to a full IMT by interband Zener tunneling with a negligible entropy deposition. In previous experiments the temporal dynamics of IMT in VO2 could be only indirectly inferred. We disentangle the electronic and lattice contributions to the IMT on a sub-picosecond timescale. Near the critical temperature the IMT becomes dissipative and the terahertz field concludes the lattice-assisted metallic nucleation initiated by heating. The method of strong-field induced phase transition presented here is applicable to a wide class of strongly correlated systems and will enable the discovery of novel metastable phases.

cond-mat.str-el↗

arXiv2017

Pressure-Temperature Phase Diagram of Vanadium Dioxide

The complexity of strongly correlated electron physics in vanadium dioxide is exemplified as its rich phase diagrams of all kinds, which in turn shed light on the mechanisms behind its various phase transitions. In this work, we map out the hydrostatic pressure - temperature phase diagram of vanadium dioxide nanobeams by independently varying pressure and temperature with a diamond anvil cell. In addition to the well-known insulating M1 (monoclinic) and metallic R (tetragonal) phases, the diagram identifies the existence at high pressures of the insulating M1' (monoclinic, more conductive than M1) phase, and two metallic phases of X (monoclinic) and O (orthorhombic, at high temperature only). Systematic optical and electrical measurements combined with density functional calculations allow us to delineate their phase boundaries as well as reveal some basic features of the transitions.

cond-mat.mtrl-sci↗

arXiv2016

Pressurizing Field-Effect Transistors of Few-Layer MoS2 in a Diamond Anvil Cell

Hydrostatic pressure applied using diamond anvil cells (DAC) has been widely explored to modulate physical properties of materials by tuning their lattice degree of freedom. Independently, electrical field is able to tune the electronic degree of freedom of functional materials via, for example, the field-effect transistor (FET) configuration. Combining these two orthogonal approaches would allow discovery of new physical properties and phases going beyond the known phase space. Such experiments are, however, technically challenging and have not been demonstrated. Herein, we report a feasible strategy to prepare and measure FETs in a DAC by lithographically patterning the nanodevices onto the diamond culet. Multiple-terminal FETs were fabricated in the DAC using few-layer MoS2 and BN as the channel semiconductor and dielectric layer, respectively. It is found that the mobility, conductance, carrier concentration, and contact conductance of MoS2 can all be significantly enhanced with pressure. We expect that the approach could enable unprecedented ways to explore new phases and properties of materials under coupled mechano-electrostatic modulation.

cond-mat.mtrl-sci↗

arXiv2015

Electronic structure, spin-orbit coupling, and interlayer interaction in bulk MoS2 and WS2

We present in-depth measurements of the electronic band structure of the transition-metal dichalcogenides (TMDs) MoS2 and WS2 using angle-resolved photoemission spectroscopy, with focus on the energy splittings in their valence bands at the K point of the Brillouin zone. Experimental results are interpreted in terms of our parallel first-principles computations. We find that interlayer interaction only weakly contributes to the splitting in bulk WS2, resolving previous debates on its relative strength. We additionally find that across a range of TMDs, the band gap generally decreases with increasing magnitude of the valence-band splitting, molecular mass, or ratio of the out-of-plane to in-plane lattice constant. Our results provide an important reference for future studies of electronic properties of MoS2 and WS2 and their applications in spintronics and valleytronics devices.

cond-mat.mes-hall↗

arXiv2014

Ultrafast Charge Transfer in Atomically Thin MoS2/WS2 Heterostructures

Van der Waals heterostructures have recently emerged as a new class of materials, where quantum coupling between stacked atomically thin two-dimensional (2D) layers, including graphene, hexagonal-boron nitride, and transition metal dichalcogenides (MX2), give rise to fascinating new phenomena. MX2 heterostructures are particularly exciting for novel optoelectronic and photovoltaic applications, because 2D MX2 monolayers can have an optical bandgap in the near-infrared to visible spectral range and exhibit extremely strong light-matter interactions. Theory predicts that many stacked MX2 heterostructures form type-II semiconductor heterojunctions that facilitate efficient electron-hole separation for light detection and harvesting. Here we report the first experimental observation of ultrafast charge transfer in photo-excited MoS2/WS2 heterostructures using both photoluminescence mapping and femtosecond (fs) pump-probe spectroscopy. We show that hole transfer from the MoS2 layer to the WS2 layer takes place within 50 fs after optical excitation, a remarkable rate for van der Waals coupled 2D layers. Such ultrafast charge transfer in van der Waals heterostructures can enable novel 2D devices for optoelectronics and light harvesting.

cond-mat.mes-hall↗

arXiv2014

Elastic Properties of Chemical-Vapor-Deposited Monolayer MoS2, WS2, and Their Bilayer Heterostructures

Elastic properties of materials are an important factor in their integration in applications. Chemical vapor deposited (CVD) monolayer semiconductors are proposed as key components in industrial-scale flexible devices and building blocks of 2D van der Waals heterostructures. However, their mechanical and elastic properties have not been fully characterized. Here we report high 2D elastic moduli of CVD monolayer MoS2 and WS2 (~ 170 N/m), which is very close to the value of exfoliated MoS2 monolayers and almost half the value of the strongest material, graphene. The 2D moduli of their bilayer heterostructures are lower than the sum of 2D modulus of each layer, but comparable to the corresponding bilayer homostructure, implying similar interactions between the hetero monolayers as between homo monolayers. These results not only provide deep insight to understanding interlayer interactions in 2D van der Waals structures, but also potentially allow engineering of their elastic properties as desired.

cond-mat.mtrl-sci↗

arXiv2014

Gate-dependent Pseudospin Mixing in Graphene/Boron Nitride Moire Superlattices

Electrons in graphene are described by relativistic Dirac-Weyl spinors with a two-component pseudospin1-12. The unique pseudospin structure of Dirac electrons leads to emerging phenomena such as the massless Dirac cone2, anomalous quantum Hall effect2, 3, and Klein tunneling4, 5 in graphene. The capability to manipulate electron pseudospin is highly desirable for novel graphene electronics, and it requires precise control to differentiate the two graphene sub-lattices at atomic level. Graphene/boron nitride (graphene/BN) Moire superlattice, where a fast sub-lattice oscillation due to B-N atoms is superimposed on the slow Moire period, provides an attractive approach to engineer the electron pseudospin in graphene13-18. This unusual Moire superlattice leads to a spinor potential with unusual hybridization of electron pseudospins, which can be probed directly through infrared spectroscopy because optical transitions are very sensitive to excited state wavefunctions. Here, we perform micro-infrared spectroscopy on graphene/BN heterostructure and demonstrate that the Moire superlattice potential is dominated by a pseudospin-mixing component analogous to a spatially varying pseudomagnetic field. In addition, we show that the spinor potential depends sensitively on the gate-induced carrier concentration in graphene, indicating a strong renormalization of the spinor potential from electron-electron interactions. Our study offers deeper understanding of graphene pseudospin structure under spinor Moire potential, as well as exciting opportunities to control pseudospin in two-dimensional heterostructures for novel electronic and photonic nanodevices.

cond-mat.mes-hall↗

arXiv2014

Temperature Gated Thermal Rectifier

Heat flow control is essential for widespread applications of heating, cooling, energy conversion and utilization. Here we demonstrate the first observation of temperature-gated thermal rectification in vanadium dioxide beams, in which an environment temperature actively modulates asymmetric heat flow. In this three terminal device, there are two switchable states, which can be accessed by global heating: Rectifier state and Resistor state. In the Rectifier state, up to 28% thermal rectification is observed. In the Resistor state, the thermal rectification is significantly suppressed (below 4%). This temperature-gated rectifier can have substantial implications ranging from autonomous thermal management of micro/nanoscale devices to thermal energy conversion and storage.

cond-mat.mtrl-sci↗

arXiv2013

Mechanically Modulated Tunneling Resistance in Monolayer MoS2

We report on the modulation of tunneling resistance in MoS2 monolayers by nano-indentation using an atomic force microscope (AFM). The resistance between the conductive AFM tip and the bottom electrode separated by a monolayer MoS2 is reversibly reduced by up to 4 orders of magnitude, which is attributed to enhanced quantum tunneling when the monolayer is compressed by the tip force. Under the WKB approximation, the experimental data is quantitatively explained by using the metal-insulator-metal tunneling diode model. As an ideal tunneling medium, the defect-free, nanometer-thick MoS2 monolayer can serve as the active layer for non-impacting nano-electro-mechanical switches.

cond-mat.mtrl-sci↗