arXiv subjects

Daniel Rhodes

Publications and source records attributed to Daniel Rhodes.

33 records · Page 2Linked to original sources

arXiv2019

Magnetic field mixing and splitting of bright and dark excitons in monolayer MoSe2

Monolayers of semiconducting transition metal dichalcogenides (TMDCs) with unique spin-valley contrasting properties and remarkably strong excitonic effects continue to be a subject of intense research interests. These model 2D semiconductors feature two fundamental intravalley excitons species - optically accessible ' bright' excitons with anti-parallel spins and optically inactive 'dark' excitons with parallel spins. For applications exploiting radiative recombination of bright excitons or long lifetime dark excitons, it is essential to understand the radiative character of the exciton ground state and establish the energy separation between the lowest energy bright and dark excitons. Here, we report a direct spectroscopic measure of dark excitons in monolayer MoSe$_2$ encapsulated in hexagonal boron nitride. By applying strong in-plane magnetic field, we induce mixing and splitting of bright and dark exciton branches, which enables an accurate spectroscopic determination of their energies. We confirm the bright character of the exciton ground state separated by a 1.5~meV gap from the higher energy dark exciton state, much smaller compared to the previous theoretical expectations. These findings provide critical information for further improvement of the accurate theoretical description of TMDCs electronic structure.

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arXiv2018

Shedding light on the monolayer-WSe2 exciton's nature by optical effective-mass measurements

Two-dimensional excitons formed in quantum materials such as monolayer transition-metal dichalcogenides and their strong light-matter interaction have attracted unrivalled attention by the research community due to their extraordinarily large oscillator strength as well as binding energy, and the inherent spin-valley locking. Semiconducting few-layer and monolayer materials with their sharp optical resonances such as WSe2 have been extensively studied and envisioned for applications in the weak as well as strong light-matter coupling regimes, for effective nano-laser operation with various different structures, and particularly for valleytronic nanophotonics motivated by the circular dichroism. Many of these applications, which may benefit heavily from the two-dimensional electronic quasiparticle's properties in such films, require controlling, manipulating and first of all understanding the nature of the optical resonances that are attributed to exciton modes. While theory and previous experiments have provided unique methods to the characterization and classification efforts regarding the band structure and optical modes in 2D materials, here, we directly measure the quasiparticle energy-momentum dispersion for the first time. Our results for single-layer WSe2 clearly indicate an emission regime predominantly governed by free excitons, i.e. Coulomb-bound electron-hole pairs with centre-of-mass momentum and corresponding effective mass. Besides uniquely evidencing the existence of free excitons at cryogenic temperatures optically, the fading of the dispersive character for increased temperatures or excitation densities reveals a transition to a regime with profound role of charge-carrier plasma or localized excitons regarding its emission, debunking the myth of free-exciton emission at elevated temperatures.

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arXiv2018

Phase Modulators Based on High Mobility Ambipolar ReSe2 Field-Effect Transistors

We fabricated ambipolar field-effect transistors (FETs) from multi-layered triclinic ReSe2, mechanically exfoliated onto a SiO2 layer grown on p-doped Si. In contrast to previous reports on thin layers (~2 to 3 layers), we extract field-effect carrier mobilities in excess of 10^2 cm^2/Vs at room temperature in crystals with nearly ~10 atomic layers. These thicker FETs also show nearly zero threshold gate voltage for conduction and high ON to OFF current ratios when compared to the FETs built from thinner layers. We also demonstrate that it is possible to utilize this ambipolarity to fabricate logical elements or digital synthesizers. For instance, we demonstrate that one can produce simple, gate-voltage tunable phase modulators with the ability to shift the phase of the input signal by either 90^o or nearly 180^o. Given that it is possible to engineer these same elements with improved architectures, for example on h-BN in order to decrease the threshold gate voltage and increase the carrier mobilities, it is possible to improve their characteristics in order to engineer ultra-thin layered logic elements based on ReSe2.

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arXiv2018

Giant Anisotropic Magnetoresistance due to Purely Orbital Rearrangement in the Quadrupolar Heavy Fermion Superconductor PrV$_2$Al$_{20}$

We report the discovery of giant and anisotropic magnetoresistance due to the orbital rearrangement in a non-magnetic correlated metal. In particular, we measured the magnetoresistance under fields up to 31.4 T in the cubic Pr-based heavy fermion superconductor PrV$_2$Al$_{20}$ with a non-magnetic $Γ_3$ doublet ground state, exhibiting antiferro-quadrupole ordering below 0.7 K. For the [100] direction, we find that the high-field phase appears between 12 T and 25 T, accompanied by a large jump at 12 T in the magnetoresistance ($ΔMR \sim $ 100 $\% $) and in the anisotropic magnetoresistivity (AMR) ratio by $\sim $ 20 $\% $. These observations indicate that the strong hybridization between the conduction electrons and anisotropic quadrupole moments leads to the Fermi surface reconstruction upon crossing the field-induced antiferro-quadrupole (orbital) rearrangement.

cond-mat.str-el↗

arXiv2018

Via Method for Lithography Free Contact and Preservation of 2D Materials

Atomically thin 2D materials span the common components of electronic circuits as metals, semi-conductors, and insulators, and can manifest correlated phases such as superconductivity, charge density waves, and magnetism. An ongoing challenge in the field is to incorporate these 2D materials into multi-layer hetero-structures with robust electrical contacts while preventing disorder and degradation. In particular, preserving and studying air-sensitive 2D materials has presented a significant challenge since they readily oxidize under atmospheric conditions. We report a new technique for contacting 2D materials, in which metal via contacts are integrated into flakes of insulating hexagonal boron nitride, and then placed onto the desired conducting 2D layer, avoiding direct lithographic patterning onto the 2D conductor. The metal contacts are planar with the bottom surface of the boron nitride and form robust contacts to multiple 2D materials. These structures protect air-sensitive 2D materials for months with no degradation in performance. This via contact technique will provide the capability to produce atomic printed circuit boards that can form the basis of more complex multi-layer heterostructures.

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arXiv2017

Ambipolar Landau levels and strong band-selective carrier interactions in monolayer WSe$_2$

Monolayers (MLs) of transition metal dichalcogenides (TMDs) exhibit unusual electrical behavior under magnetic fields due to their intrinsic spin-orbit coupling and lack of inversion symmetry. While recent experiments have also identified the critical role of carrier interactions within these materials, a complete mapping of the ambipolar Landau level (LL) sequence has remained elusive. Here, we use single-electron transistors to perform LL spectroscopy in ML WSe$_2$, for the first time providing a comprehensive picture of the electronic structure of a ML TMD for both electrons and holes. We find that the LLs differ notably between the two bands, and follow a unique sequence in the valence band (VB) that is dominated by strong Zeeman effects. The Zeeman splitting in the VB is several times higher than the cyclotron energy, far exceeding the predictions of a single-particle model, and moreover tunes significantly with doping. This implies exceptionally strong many-body interactions, and suggests that ML WSe$_2$ can serve as a host for new correlated-electron phenomena.

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arXiv2017

Van der Waals Schottky barriers as interface probes of the correlation between chemical potential shifts and charge density wave formation in 1T-TiSe$_2$ and 2H-NbSe$_2$

Layered transition metal dichalcogenide (TMD) materials, i.e. 1T-TiSe$_2$ and 2H-NbSe$_2$, harbor a second order charge density wave (CDW) transition where phonons play a key role for the periodic modulations of conduction electron densities and associated lattice distortions. We systematically study the transport and capacitance characteristics over a wide temperature range of Schottky barriers formed by intimately contacting freshly exfoliated flakes of 1T-TiSe$_2$ and 2H-NbSe$_2$ to \textit{n}-type GaAs semiconductor substrates. The extracted temperature-dependent parameters (zero-bias barrier height, ideality and built-in potential) reflect changes at the TMD/GaAs interface induced by CDW formation for both TMD materials. The measured built-in potential reveals chemical-potential shifts relating to CDW formation. With decreasing temperature a peak in the chemical-potential shifts during CDW evolution indicates a competition between electron energy re-distributions and a combination of lattice strain energies and Coulomb interactions. These modulations of chemical potential in CDW systems, such as 1T-TiSe$_2$ and 2H-NbSe$_2$ harboring second-order phase transitions, reflect a corresponding conversion from short to long-range order.

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arXiv2016

Photoconductivity of few-layered p-WSe2 phototransistors via multi-terminal measurements

Recently, two-dimensional materials and in particular transition metal dichalcogenides (TMDs) were extensively studied because of their strong light-matter interaction and the remarkable optoelectronic response of their field-effect transistors (FETs). Here, we report a photoconductivity study from FETs built from few-layers of p-WSe2 measured in a multi-terminal configuration under illumination by a 532 nm laser source. The photogenerated current was measured as a function of the incident optical power, of the drain-to-source bias and of the gate voltage. We observe a considerably larger photoconductivity when the phototransistors were measured via a four-terminal configuration when compared to a two-terminal one. For an incident laser power of 248 nW, we extract 18 A/W and ~4000% for the two-terminal responsivity (R) and the concomitant external quantum efficiency (EQE) respectively, when a bias voltage Vds = 1 V and a gate voltage Vbg = 10 V are applied to the sample. R and EQE are observed to increase by 370% to ~85 A/W and ~20000% respectively, when using a four-terminal configuration. Thus, we conclude that previous reports have severely underestimated the optoelectronic response of transition metal dichalcogenides, which in fact reveals a remarkable potential for photosensing applications.

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arXiv2015

Non-stoichiometry and Defects in the Weyl Semimetals TaAs, TaP, NbP, and NbAs

We report a structural study of the Weyl semimetals TaAs, TaP, NbP, and NbAs, utilizing diffraction techniques (single crystal x-ray diffraction and energy dispersive spectroscopy) and imaging techniques (transmission electron microscopy/scanning transmission electron microscopy). We observe defects of various degrees, leading to non-stoichiometric single crystals of all four semimetals. While TaP displays a large pnictide deficiency with composition TaP$_{0.83(3)}$, and stacking faults accompanied by anti-site disorder and site vacancies, TaAs displays transition metal deficiency with composition Ta$_{0.92(2)}$As and a high density of stacking faults. NbP also displays pnictide deficiency, yielding composition NbP$_{0.95(2)}$, and lastly, NbAs display very little deviation from a 1:1 composition, NbAs$_{1.00(3)}$, and is therefore recommended to serve as the model compound for these semimetals.

cond-mat.mtrl-sci↗

arXiv2015

Pronounced photovoltaic response from multi-layered transition-metal dichalcogenides PN-junctions

Transition metal dichalcogenides (TMDs) are layered semiconductors with indirect band gaps comparable to Si. These compounds can be grown in large area, while their gap(s) can be tuned by changing their chemical composition or by applying a gate voltage. The experimental evidence collected so far, points towards a strong interaction with light, which contrasts with the small photovoltaic efficiencies $η\geq 1$ % extracted from bulk crystals or exfoliated monolayers. Here, we evaluate the potential of these compounds by studying the photovoltaic response of electrostatically generated PN-junctions composed of approximately ten atomic-layers of MoSe$_2$ stacked onto the dielectric $h$-BN. In addition to ideal diode-like response, we find that these junctions can yield, under AM-1.5 illumination, photovoltaic efficiencies $η$ exceeding 14 %, with fill-factors of ~ 70 %. Given the available strategies for increasing $η$ such as gap tuning, improving the quality of the electrical contacts, or the fabrication of tandem cells, our study suggests a remarkable potential for photovoltaic applications based on TMDs.

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arXiv2015

Metal to insulator quantum-phase transition in few-layered ReS$_2$

In ReS$_2$ a layer-independent direct band-gap of 1.5 eV implies a potential for its use in optoelectronic applications. ReS$_2$ crystallizes in the 1T$^{\prime}$-structure which leads to anisotropic physical properties and whose concomitant electronic structure might host a non-trivial topology. Here, we report an overall evaluation of the anisotropic Raman response and the transport properties of few-layered ReS$_2$ field-effect transistors. We find that ReS$_2$ exfoliated on SiO$_2$ behaves as an $n$-type semiconductor with an intrinsic carrier mobility surpassing $μ_i$ ~30 cm$^2$/Vs at $T = 300$ K which increases up to ~350 cm$^2$/Vs at 2 K. Semiconducting behavior is observed at low electron densities $n$, but at high values of n the resistivity decreases by a factor > 7 upon cooling to 2 K and displays a metallic $T^2$-dependence. This indicates that the band structure of 1T$^{\prime}$-ReS$_2$ is quite susceptible to an electric field applied perpendicularly to the layers. The electric-field induced metallic state observed in transition metal dichalcogenides was recently claimed to result from a percolation type of transition. Instead, through a scaling analysis of the conductivity as a function of $T$ and $n$, we find that the metallic state of ReS$_2$ results from a second-order metal to insulator transition driven by electronic correlations. This gate-induced metallic state offers an alternative to phase engineering for producing ohmic contacts and metallic interconnects in devices based on transition metal dichalcogenides.

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arXiv2015

Optoelectronic switch based on intrinsic dual Schottky diodes in ambipolar MoSe$_2$ field-effect transistors

Here, we report the observation of a hitherto unreported optoelectronic effect, namely a light-induced diode-like response in multi-layered MoSe$_2$ field-effect transistors whose sense of current rectification is controllable through a gate voltage. We argue, through numerical simulations, that this behavior results from the difference in the size of the Schottky barriers between drain and source metal contacts. Each barrier can be modeled as a Schottky diode but with opposite senses of current rectification between them, with the diode response resulting from the light induced promotion of photo-generated carriers across the smaller barrier. The back gate voltage controls the sense of current rectification by modulating the relative amplitude between them. This effect, which gives rise to a novel type of optoelectronic switch, also yields a photovoltaic response. Hence, it could provide an alternative to PN-junctions when harvesting photovoltaic currents from transition metal dichalcogenides. We argue that the photovoltaic efficiency associated to this effect could be increased by just increasing the relative asymmetry between both Schottky barriers. We also suggest that this new electro-optical effect has potential for technological applications.

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arXiv2015

High Photoresponsivity and Short Photo Response Times in Few-Layered WSe$_2$ Transistors

Here, we report the photoconducting response of field-effect transistors based on three atomic layers of chemical vapor transport grown WSe$_2$ crystals mechanically exfoliated onto SiO$_2$. We find that tri-layered WSe$_2$ field-effect transistors, built with the simplest possible architecture, can display high hole mobilities ranging from 350 cm$^2$/Vs at room temperature (saturating at a value of ~500 cm$^2$/Vs below 50 K) displaying a strong photocurrent response which leads to exceptionally high photo responsivities up to 7 A/W under white light illumination of the entire channel for power densities p < 10$^2$ W/m$^2$. Under a fixed wavelength of $λ$ = 532 nm and a laser spot size smaller than the conducting channel area we extract photo responsitivities approaching 100 mA/W with concomitantly high external quantum efficiencies up to ~ 40 % at room temperature. These values surpass values recently reported from more complex architectures, such as graphene and transition metal dichalcogenides based heterostructures. Also, tri-layered WSe$_2$ photo-transistors display photo response times in the order of 10 microseconds. Our results indicate that the addition of a few atomic layers considerably decreases the photo response times, probably by minimizing the interaction with the substrates, while maintaining a very high photo-responsivity.

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arXiv2015

Gate-modulated conductance of few-layer WSe_2 field-effect transistors in the subgap regime: Schottky barrier transistor and subgap impurity states

Two key subjects stand out in the pursuit of semiconductor research: material quality and contact technology. The fledging field of atomically thin transition metal dichalcogenides (TMDCs) faces a number of challenges in both efforts. This work attempts to establish a connection between the two by examining the gate-dependent conductance of few-layer (1-5L) WSe2 field effect devices. Measurements and modeling of the subgap regime reveal Schottky barrier transistor behavior. We show that transmission through the contact barrier is dominated by thermionic field emission (TFE) at room temperature, despite the lack of intentional doping. The TFE process arises due to a large number of subgap impurity states, the presence of which also leads to high mobility edge carrier densities. The density of states of such impurity states is self-consistently determined to be approximately 1-2x10^13 /cm^2/eV in our devices. We demonstrate that substrate is unlikely to be a major source of the impurity states and suspect that lattice defects within the material itself are primarily responsible. Our experiments provide key information to advance the quality and understanding of TMDC materials and electrical devices.

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arXiv2014

Field-Effect Transistors Based on Few-Layered alpha-MoTe_2

Here we report the properties of field-effect transistors based on few layers of chemical vapor transport grown alpha- MoTe_2 crystals mechanically exfoliated onto SiO_2. We performed field-effect and Hall mobility measurements, as well as Raman scattering and transmission electron microscopy. In contrast to both MoS_2 and MoSe_2, our MoTe_2 field-effect transistors (FETs) are observed to be hole-doped, displaying on/off ratios surpassing 106 and typical sub-threshold swings of ~ 140 mV per decade. Both field-effect and Hall mobilities indicate maximum values approaching or surpassing 10 cm^2/Vs which are comparable to figures previously reported for single or bi-layered MoS_2 and/or for MoSe_2 exfoliated onto SiO_2 at room temperature and without the use of dielectric engineering. Raman scattering reveals sharp modes in agreement with previous reports, whose frequencies are found to display little or no dependence on the number of layers. Given that both MoS_2 is electron doped, the stacking of MoTe_2 onto MoS_2 could produce ambipolar field-effect transistors and a gap modulation. Although the overall electronic performance of MoTe_2 is comparable to those of MoS_2 and MoSe_2, the heavier element Te should lead to a stronger spin orbit-coupling and possibly to concomitantly longer decoherence times for exciton valley and spin indexes.

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