arXiv subjects

Judy J. Cha

Publications and source records attributed to Judy J. Cha.

At least 37 records · Page 2Linked to original sources

arXiv2021

Effects of Steric Factors on Molecular Doping to MoS$_2$

Surface functionalization of two-dimensional (2D) materials with organic electron donors (OEDs) is a powerful method to modulate the electronic properties of the material. However, our fundamental understanding of the doping mechanism is largely limited to the categorization of molecular dopants as n- or p-type based on the relative position of the molecule's redox potential in relation to the Fermi level of the 2D host. Our limited knowledge about the impact of factors other than the redox properties of the molecule on doping makes it challenging to controllably use molecules to dope 2D materials and design new OEDs. Here, we functionalize monolayer MoS$_2$ using two molecular dopants, Me- and $^t$Bu-OED, which have the same redox potential but different steric properties to probe the effects of molecular size on the doping level of MoS$_2$. We show that, for the same functionalization conditions, the doping powers of Me- and $^t$Bu-OED are 0.22 - 0.44 and 0.11 electrons per molecule, respectively, demonstrating that the steric properties of the molecule critically affect doping levels. Using the stronger dopant, Me-OED, a carrier density of 1.10 +/- 0.37 x 10$^{14}$ cm$^{-2}$ is achieved in MoS$_2$, the highest doping level to date for MoS$_2$ using surface functionalization. Overall, we establish that tuning of the steric properties of the dopant is essential in the rational design of molecular dopants.

cond-mat.mtrl-sci↗

arXiv2021

Heterointerface control over lithium-induced phase transitions in MoS2 heterostructures

Phase transitions of two-dimensional materials and their heterostructures enable many applications including electrochemical energy storage, catalysis, and memory; however, the nucleation pathways by which these transitions proceed remain underexplored, prohibiting engineering control for these applications. Here, we demonstrate that the lithium intercalation-induced 2H-1T' phase transition in MoS2 proceeds via nucleation of the 1T' phase at a heterointerface by monitoring the phase transition of MoS2/graphene and MoS2/hexagonal boron nitride (hBN) heterostructures with Raman spectroscopy in situ during intercalation. We observe that graphene-MoS2 heterointerfaces require an increase of 0.8 V in applied electrochemical potential to nucleate the 1T' phase in MoS2 compared to hBN-MoS2 heterointerfaces. The increased nucleation barrier at graphene-MoS2 heterointerfaces is due to the reduced charge transfer from lithium to MoS2 at the heterointerface as lithium also dopes graphene based on ab initio calculations. Further, we show that the growth of the 1T' domain propagates along the heterointerface, rather than through the interior of MoS2. Our results provide the first experimental observations of the heterogeneous nucleation and growth of intercalation-induced phase transitions in two-dimensional materials and heterointerface effects on their phase transition.

cond-mat.mtrl-sci↗

arXiv2021

Thickness Dependence of Magneto-transport Properties in Tungsten Ditelluride

We investigate the electronic structure of tungsten ditelluride (WTe$_2$) flakes with different thicknesses in magneto-transport studies. The temperature-dependent resistance and magnetoresistance (MR) measurements both confirm the breaking of carrier balance induced by thickness reduction, which suppresses the `turn-on' behavior and large positive MR. The Shubnikov-de-Haas oscillation studies further confirm the thickness-dependent change of electronic structure of WTe$_2$ and reveal a possible temperature-sensitive electronic structure change. Finally, we report the thickness-dependent anisotropy of Fermi surface, which reveals that multi-layer WTe$_2$ is an electronic 3D material and the anisotropy decreases as thickness decreases.

cond-mat.mtrl-sci↗

arXiv2020

Heterointerface effects on lithium-induced phase transitions in intercalated MoS2

The intercalation-induced phase transition of MoS2 from the semiconducting 2H to the semimetallic 1T' phase has been studied in detail for nearly a decade; however, the effects of a heterointerface between MoS2 and other two-dimensional (2D) crystals on the phase transition have largely been overlooked. Here, ab initio calculations show that intercalating Li at a MoS2-hexagonal boron nitride (hBN) interface stabilizes the 1T phase over the 2H phase of MoS2 by ~ 100 mJ m-2, suggesting that encapsulating MoS2 with hBN may lower the electrochemical energy needed for the intercalation-induced phase transition. However, in situ Raman spectroscopy of hBN-MoS2-hBN heterostructures during electrochemical intercalation of Li+ shows that the phase transition occurs at the same applied voltage for the heterostructure as for bare MoS2. We hypothesize that the predicted thermodynamic stabilization of the 1T'-MoS2-hBN interface is counteracted by an energy barrier to the phase transition imposed by the steric hindrance of the heterointerface. The phase transition occurs at lower applied voltages upon heating the heterostructure, which supports our hypothesis. Our study highlights that interfacial effects of 2D heterostructures can go beyond modulating electrical properties and can modify electrochemical and phase transition behaviors.

cond-mat.mtrl-sci↗

arXiv2020

Cm2 Scale Synthesis of MoTe2 Thin Films with Large Grains and Layer Control David

Owing to the small energy differences between its polymorphs, MoTe2 can access a full spectrum of electronic states, from the 2H semiconducting state to the 1T semimetallic state, and from the Td Weyl semimetallic state to the superconducting state in the 1T and Td phase at low temperature. Thus, it is a model system for phase transformation studies as well as quantum phenomena such as the quantum spin Hall effect and topological superconductivity. Careful studies of MoTe2 and its potential applications require large area MoTe2 thin films with high crystallinity and thickness control. Here, we present cm2 scale synthesis of 2H MoTe2 thin films with layer control and large grains that span several microns. Layer control is achieved by controlling the initial thickness of the precursor MoOx thin films, which are deposited on sapphire substrates by atomic layer deposition and subsequently tellurized. Despite the van der Waals epitaxy, the precursor-substrate interface is found to critically determine the uniformity in thickness and grain size of the resulting MoTe2 films: MoTe2 grown on sapphire show uniform films while MoTe2 grown on amorphous SiO2 substrates form islands. This synthesis strategy decouples the layer control from the variabilities of growth conditions for robust growth results, and is applicable to grow other transition metal dichalcogenides with layer control.

cond-mat.mtrl-sci↗

arXiv2020

Synthesis of narrow SnTe nanowires using alloy nanoparticles

Topological crystalline insulator tin telluride (SnTe) provides a rich playground to examine interactions of correlated electronic states, such as ferroelectricity, topological surface states, and superconductivity. Making SnTe into nanowires further induces novel electronic states due to one-dimensional (1D) confinement effects. Thus, for transport measurements, SnTe nanowires must be made narrow in their diameters to ensure the 1D confinement and phase coherence of the topological surface electrons. This study reports a facile growth method to produce narrow SnTe nanowires with a high yield using alloy nanoparticles as growth catalysts. The average diameter of the SnTe nanowires grown using the alloy nanoparticles is 85 nm, nearly a factor of three reduction from the previous average diameter of 240 nm using gold nanoparticles as growth catalysts. Transport measurements reveal the effect of the nanowire diameter on the residual resistance ratio and magnetoresistance. Particularly, the ferroelectric transition temperature for SnTe is observed to change systematically with the nanowire diameter. In situ cryogenic cooling of narrow SnTe nanowires in a transmission electron microscope directly reveals the cubic to rhombohedral structural transition, which is associated with the ferroelectric transition. Thus, these narrow SnTe nanowires represent a model system to study electronic states arising from the 1D confinement, such as 1D topological superconductivity as well as a potential multi-band superconductivity.

cond-mat.mtrl-sci↗

arXiv2020

The Effect of Mechanical Strain on Lithium Staging in Graphene

Lithium intercalation into graphite is the foundation for the lithium-ion battery, and the thermodynamics of the lithiation of graphitic electrodes have been heavily investigated. Intercalated lithium in bulk graphite undergoes structural ordering known as staging to minimize electrostatic repulsions within the crystal lattice. While this process is well-understood for bulk graphite, confinement effects become important at the nanoscale, which can significantly impact the electrochemistry of nanostructured electrodes. Therefore, graphene offers a model platform to study intercalation dynamics at the nanoscale by combining on-chip device fabrication and electrochemical intercalation with in situ characterization. We show that microscale mechanical strain significantly affects the formation of ordered lithium phases in graphene. In situ Raman spectroscopy of graphene microflakes mechanically constrained at the edge during lithium intercalation reveals a thickness-dependent increase of up to 1.26 V in the electrochemical potential that induces lithium staging. While the induced mechanical strain energy increases with graphene thickness to the fourth power, its magnitude is small compared to the observed increase in electrochemical energy. We hypothesize that the mechanical strain energy increases a nucleation barrier for lithium staging, greatly delaying the formation of ordered lithium phases. Our results indicate that electrode assembly can critically impact lithium staging dynamics important for cycling rates and power generation for batteries. We demonstrate strain engineering in two-dimensional nanomaterials as an approach to manipulate phase transitions and chemical reactivity.

cond-mat.mtrl-sci↗

arXiv2020

Near Unity Molecular Doping Efficiency in Monolayer MoS2

Surface functionalization with organic electron donors (OEDs) is an effective doping strategy for two-dimensional (2D) materials, which can achieve doping levels beyond those possible with conventional electric field gating. While the effectiveness of surface functionalization has been demonstrated in many 2D systems, the doping efficiencies of OEDs have largely been unmeasured, which is in stark contrast to their precision syntheses and tailored redox potentials. Here, using monolayer MoS2 as a model system and an organic reductant based on 4,4-bipyridine (DMAP-OED) as a strong organic dopant, we establish that the doping efficiency of DMAP-OED to MoS2 is in the range of 0.63 to 1.26 electrons per molecule. We also achieve the highest doping level to date in monolayer MoS2 by surface functionalization and demonstrate that DMAP-OED is a stronger dopant than benzyl viologen, which was the previous best OED dopant. The measured range of the doping efficiency is in good agreement with the values predicted from first-principles calculations. Our work provides a basis for the rational design of OEDs for high-level doping of 2D materials.

cond-mat.mtrl-sci↗

arXiv2020

Crossover Between Weak Antilocalization and Weak Localization and Electron-Electron Interaction in Few-Layer WTe$_2$

We report electron transport studies in an encapsulated few-layer WTe$_2$ at low temperatures and high magnetic fields. The magnetoconductance reveals a temperature-induced crossover between weak antilocalization (WAL) and weak localization (WL) in quantum diffusive regime. We show that the crossover clearly manifests coexistence and competition among several characteristic lengths, including the dephasing length, the spin-flip length, and the mean free path. In addition, low temperature conductance increases logarithmically with the increase of temperature indicating an interplay of electron-electron interaction (EEI) and spin-orbit coupling (SOC). We demonstrate the existences and quantify the strengths of EEI and SOC which are considered to be responsible for gap opening in the quantum spin hall state in WTe2 at the monolayer limit.

cond-mat.mtrl-sci↗

arXiv2016

Efficient Electrical Control of Thin-Film Black Phosphorus Bandgap

Recently rediscovered black phosphorus is a layered semiconductor with promising electronic and photonic properties. Dynamic control of its bandgap can enable novel device applications and allow for the exploration of new physical phenomena. However, theoretical investigations and photoemission spectroscopy experiments performed on doped black phosphorus through potassium adsorption indicate that in its few-layer form, an exceedingly large electric field in the order of several volts per nanometer is required to effectively tune its bandgap, making the direct electrical control unfeasible. Here we demonstrate the tuning of bandgap in intrinsic black phosphorus using an electric field directly and reveal the unique thickness-dependent bandgap tuning properties, arising from the strong interlayer electronic-state coupling. Furthermore, leveraging a 10-nm-thick black phosphorus in which the field-induced potential difference across the film dominates over the interlayer coupling, we continuously tune its bandgap from ~300 to below 50 milli-electron volts, using a moderate displacement field up to 1.1 volts per nanometer. Such dynamic tuning of bandgap may not only extend the operational wavelength range of tunable black phosphorus photonic devices, but also pave the way for the investigation of electrically tunable topological insulators and topological nodal semimetals.

cond-mat.mes-hall↗

arXiv2016

Anisotropic Black Phosphorus Synaptic Device for Neuromorphic Applications

Synapses are functional links between neurons, through which "information" flows in the neural network. These connections vary significantly in strength, typically resulting from the intrinsic heterogeneity in their chemical and biological properties. Such heterogeneity is fundamental to the diversity of neural activities, which together with other features of the brain enables functions ranging from perception and recognition, to memory and reasoning. Realizing such heterogeneity in synaptic electronics is critical towards building artificial neural network with the potential for achieving the level of complexity in biological systems. However, such intrinsic heterogeneity has been very challenging to realize in current synaptic devices. Here, we demonstrate the first black phosphorus (BP) synaptic device, which offers intrinsic anisotropy in its synaptic characteristics directly resulting from its low crystal symmetry. The charge transfer between the 2-nm native oxide of BP and the BP channel is utilized to achieve the synaptic behavior. Key features of biological synapses such as long-term plasticity with heterogeneity, including long-term potentiation/depression and spike-timing-dependent plasticity, are mimicked. With the anisotropic BP synaptic devices, we also realize a simple compact heterogeneous axon-multi-synapses network. This demonstration represents an important step towards introducing intrinsic heterogeneity to artificial neuromorphic systems.

cond-mat.mtrl-sci↗

arXiv2016

Structural Phase Transition and Carrier Density Tuning in SnSexTe1-x Nanoplates for Topological Crystalline Insulators

For topological insulators and topological crystalline insulators (TCIs), their exotic surface states are promising for fundamental condensed matter physics research as well as future electronics such as low-dissipation electronics and spintronics. However, the high bulk carrier density that often dominates the transport property is the major materials challenge, critically hindering our ability to study and manipulate the surface states. In this manuscript, we demonstrate an alloying strategy, SnSexTe1-x, to effectively reduce the bulk carrier density. As long as SnSexTe1-x remains in the cubic crystal structure, it is predicted to be a TCI. We show systematic decrease of the bulk carrier density with the increasing Se concentration, demonstrating that the alloying principle works. In addition, we map out the phase diagram of the cubic to the orthorhombic structural transition as a function of the Se concentration. This was made possible by studying alloy nanoplates which remain single-crystalline and is either in the cubic or the orthorhombic phase, in contrast to bulk alloys that would exhibit polycrystalline grains. Lastly, we investigate systematically the ferroelectric transition associated with the structural transition from the cubic to the rhombohedral phase for SnSexTe1-x. This is the first ferroelectric transition study of the alloy system SnSexTe1-x.

cond-mat.mtrl-sci↗

arXiv2015

Revealing surface states in In-doped SnTe superconducting nanoplates with low bulk mobility

Indium (In) doping in topological crystalline insulator SnTe induces superconductivity, making In-doped SnTe a candidate for a topological superconductor. SnTe nanostructures offer well-defined nanoscale morphology and high surface-to-volume ratios to enhance surface effects. Here, we study In-doped SnTe nanoplates, InxSn1-xTe, with x ranging from 0 to 0.1 and show they superconduct. More importantly, we show that In doping reduces the bulk mobility of InxSn1-xTe such that the surface states are revealed in magnetotransport despite the high bulk carrier density. This is manifested by two-dimensional linear magnetoresistance in high magnetic fields, which is independent of temperature up to 10 K. Aging experiments show that the linear magnetoresistance is sensitive to ambient conditions, further confirming its surface origin. We also show that the weak antilocalization observed in InxSn1-xTe nanoplates is a bulk effect. Thus, we show that nanostructures and reducing the bulk mobility are effective strategies to reveal the surface states and test for topological superconductors.

cond-mat.mes-hall↗

arXiv2014

Topological Crystalline Insulator Nanostructures

Topological crystalline insulators are topological insulators whose surface states are protected by the crystalline symmetry, instead of the time reversal symmetry. Similar to the first generation of three-dimensional topological insulators such as Bi2Se3 and Bi2Te3, topological crystalline insulators also possess surface states with exotic electronic properties such as spin-momentum locking and Dirac dispersion. Experimentally verified topological crystalline insulators to date are SnTe, Pb1-xSnxSe, and Pb1-xSnxTe. Because topological protection comes from the crystal symmetry, magnetic impurities or in-plane magnetic fields are not expected to open a gap in the surface states in topological crystalline insulators. Additionally, because they are cubic structure instead of layered structure, branched structures or strong coupling with other materials for large proximity effects are possible, which are difficult with layered Bi2Se3 and Bi2Te3. Thus, additional fundamental phenomena inaccessible in three-dimensional topological insulators can be pursued. In this review, topological crystalline insulator SnTe nanostructures will be discussed. For comparison, experimental results based on SnTe thin films will be covered. Surface state properties of topological crystalline insulators will be discussed briefly.

cond-mat.mtrl-sci↗

arXiv2014

Synthesis of SnTe Nanoplates with {100} and {111} Surfaces

SnTe is a topological crystalline insulator that possesses spin-polarized, Dirac-dispersive surface states protected by crystal symmetry. Multiple surface states exist on the {100}, {110}, and {111} surfaces of SnTe, with the band structure of surface states depending on the mirror symmetry of a particular surface. Thus, to access surface states selectively, it is critical to control the morphology of SnTe such that only desired crystallographic surfaces are present. Here, we grow SnTe nanostructures using vapor-liquid-solid and vapor-solid growth mechanisms. Previously, SnTe nanowires and nanocrystals have been grown.1-4 In this report, we demonstrate synthesis of SnTe nanoplates with lateral dimensions spanning tens of microns and thicknesses of a hundred nanometers. The top and bottom surfaces are either (100) or (111), maximizing topological surface states on these surfaces. Magnetotransport on these SnTe nanoplates shows high bulk carrier density, consistent with bulk SnTe crystals arising due to defects such as Sn vacancies. In addition, we observe a structural phase transition in these nanoplates from the high temperature rock salt to low temperature rhombohedral structure. For nanoplates with very high carrier density, we observe a slight upturn in resistance at low temperatures, indicating electron-electron interactions.

cond-mat.mes-hall↗

arXiv2014

One-dimensional helical transport in topological insulator nanowire interferometers

The discovery of three-dimensional (3D) topological insulators opens a gateway to generate unusual phases and particles made of the helical surface electrons, proposing new applications using unusual spin nature. Demonstration of the helical electron transport is a crucial step to both physics and device applications of topological insulators. Topological insulator nanowires, of which spin-textured surface electrons form 1D band manipulated by enclosed magnetic flux, offer a unique nanoscale platform to realize quantum transport of spin-momentum locking nature. Here, we report an observation of a topologically protected 1D mode of surface electrons in topological insulator nanowires existing at only two values of half magnetic quantum flux ($\pm$h/2e) due to a spin Berry's phase ($π$). The helical 1D mode is robust against disorder but fragile against a perpendicular magnetic field breaking time-reversal-symmetry. This result demonstrates a device with robust and easily accessible 1D helical electronic states from 3D topological insulators, a unique nanoscale electronic system to study topological phenomena.

cond-mat.mes-hall↗

arXiv2011

Ultra-low carrier concentration and surface dominant transport in Sb-doped Bi2Se3 topological insulator nanoribbons

A topological insulator is a new state of matter, possessing gapless spin-locking surface states across the bulk band gap which has created new opportunities from novel electronics to energy conversion. However, the large concentration of bulk residual carriers has been a major challenge for revealing the property of the topological surface state via electron transport measurement. Here we report surface state dominated transport in Sb-doped Bi2Se3 nanoribbons with very low bulk electron concentrations. In the nanoribbons with sub-10nm thickness protected by a ZnO layer, we demonstrate complete control of their top and bottom surfaces near the Dirac point, achieving the lowest carrier concentration of 2x10^11/cm2 reported in three-dimensional (3D) topological insulators. The Sb-doped Bi2Se3 nanostructures provide an attractive materials platform to study fundamental physics in topological insulators, as well as future applications.

cond-mat.mes-hall↗

arXiv2011

Ambipolar Field Effect in Topological Insulator Nanoplates of (BixSb1-x)2Te3

Topological insulators represent a new state of quantum matter attractive to both fundamental physics and technological applications such as spintronics and quantum information processing. In a topological insulator, the bulk energy gap is traversed by spin-momentum locked surface states forming an odd number of surface bands that possesses unique electronic properties. However, transport measurements have often been dominated by residual bulk carriers from crystal defects or environmental doping which mask the topological surface contribution. Here we demonstrate (BixSb1-x)2Te3 as a tunable topological insulator system to manipulate bulk conductivity by varying the Bi/Sb composition ratio. (BixSb1-x)2Te3 ternary compounds are confirmed as topological insulators for the entire composition range by angle resolved photoemission spectroscopy (ARPES) measurements and ab initio calculations. Additionally, we observe a clear ambipolar gating effect similar to that observed in graphene using nanoplates of (BixSb1-x)2Te3 in field-effect-transistor (FET) devices. The manipulation of carrier type and concentration in topological insulator nanostructures demonstrated in this study paves the way for implementation of topological insulators in nanoelectronics and spintronics.

cond-mat.str-el↗