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Description, Strong hybridization of two-magnon scattering with phonons is observed in 2D antiferromagnet MnPSe3., Magnetic excitations in van der Waals (vdW) materials, especially in the two-dimensional (2D) limit, are an exciting research topic from both the fundamental and applied perspectives. Using temperature-dependent, magneto-Raman spectroscopy, we identify the hybridization of two-magnon excitations with two phonons in manganese phosphorus triselenide (MnPSe3), a magnetic vdW material that hosts in-plane antiferromagnetism. Results from first-principles calculations of the phonon and magnon spectra further support our identification. The Raman spectra’s rich temperature dependence through the magnetic transition displays an avoided crossing behavior in the phonons’ frequency and a concurrent decrease in their lifetimes. We construct a model based on the interaction between a discrete level and a continuum that reproduces these observations. Our results imply a strong hybridization between each phonon and a two-magnon continuum. This work demonstrates that the magnon-phonon interactions can be observed directly in Raman scattering and provides deep insight into these interactions in 2D magnetic materials.

The interest in two-dimensional and layered materials continues to expand, driven by the compelling properties of individual atomic layers that can be stacked and/or twisted into synthetic heterostructures. The plethora of electronic properties as well as the emergence of many different quasiparticles, including plasmons, polaritons, trions and excitons with large, tunable binding energies that all can be controlled and modulated through electrical means has given rise to many device applications. In addition, these materials exhibit both room-temperature spin and valley polarization, magnetism, superconductivity, piezoelectricity that are intricately dependent on the composition, crystal structure, stacking, twist angle, layer number and phases of these materials. Initial results on graphene exfoliated from single bulk crystals motivated the development of wide-area, high purity synthesis and heterojunctions with atomically clean interfaces. Now by opening this design space to new synthetic two-dimensional materials "beyond graphene", it is possible to explore uncharted opportunities in designing novel heterostructures for electrical tunable devices. To fully reveal the emerging functionalities and opportunities of these atomically thin materials in practical applications, this review highlights several representative and noteworthy research directions in the use of electrical means to tune these aforementioned physical and structural properties, with an emphasis on discussing major applications of beyond graphene 2D materials in tunable devices in the past few years and an outlook of what is to come in the next decade.

Efficient doping of 2D materials, including carrier type, concentration and mobility, is challenging but essential for enabling their future electronic and photonic applications. We are developing substitutional n- and p- doping of InSe semiconductor by introducing Sn and Zn, respectively, in the Bridgman bulk crystal growth. Electrical transport properties of undoped vs. n- and p- doped InSe crystals are compared by conducting Hall measurements on bulk crystals and FET transport measurements on exfoliated thin layers. Undoped InSe is intrinsically n-type in both bulk and thin-film forms, with [n]~3.5E14 cm-3 and mu values of up to 1,400 cm2 V-1 s-1 for thick layers at 300K. Carrier concentration in Sn-doped thick layers increases approximately two-fold, while the corresponding mobility reduces ~2 times at 300 K. Zn-doped InSe shows p- behavior for bulk InSe with [p]~7.9E13 cm-3 and mu~43 cm2 V-1 s-1 at 300 K, which reverts to ambipolar/n- type behavior for thin layers in FET devices.

Recently it was discovered that van der Waals bonded magnetic materials retain long range magnetic ordering down to a single layer, opening many avenues in fundamental physics and potential applications of these fascinating materials. One such material is $\mathrm{FeP}{\mathrm{S}}_{3}$, a large spin $(S=2)$ Mott insulator where the Fe atoms form a honeycomb lattice. In the bulk, $\mathrm{FeP}{\mathrm{S}}_{3}$ has been shown to be a quasi-two-dimensional-Ising antiferromagnet, with additional features in the Raman spectra emerging below the N\'eel temperature $({T}_{\mathrm{N}})$ of approximately 120 K. Using magneto-Raman spectroscopy as an optical probe of magnetic structure, we show that one of these Raman-active modes in the magnetically ordered state is actually a magnon with a frequency of $\ensuremath{\approx}3.7\phantom{\rule{0.16em}{0ex}}\mathrm{THz}\phantom{\rule{4pt}{0ex}}(122\phantom{\rule{0.16em}{0ex}}\mathrm{c}{\mathrm{m}}^{\ensuremath{-}1})$. Contrary to previous work, which interpreted this feature as a phonon, our Raman data shows the expected frequency shifting and splitting of the antiferromagnetic magnon as a function of temperature and magnetic field, respectively, where we determine the $g$ factor to be $\ensuremath{\approx}2$. In addition, the symmetry behavior of the magnon is studied by polarization-dependent Raman spectroscopy and explained using the magnetic point group of $\mathrm{FeP}{\mathrm{S}}_{3}$.

The discovery of 2-dimensional (2D) materials, such as CrI3, that retain magnetic ordering at monolayer thickness has resulted in a surge of both pure and applied research in 2D magnetism. Here, we report a magneto-Raman spectroscopy study on multilayered CrI3, focusing on two additional features in the spectra that appear below the magnetic ordering temperature and were previously assigned to high frequency magnons. Instead, we conclude these modes are actually zone-folded phonons. We observe a striking evolution of the Raman spectra with increasing magnetic field applied perpendicular to the atomic layers in which clear, sudden changes in intensities of the modes are attributed to the interlayer ordering changing from antiferromagnetic to ferromagnetic at a critical magnetic field. Our work highlights the sensitivity of the Raman modes to weak interlayer spin ordering in CrI3., Thin samples CrI3 exhibit a phase transition under an applied magnetic field from layered antiferromagnetism to ferromagnetism. Here the authors observe an associated abrupt change in the magneto-Raman spectra, illustrating the sensitivity of Raman spectra to magnetic ordering.

The strong in-plane anisotropy of rhenium disulfide (ReS2) offers an additional physical parameter that can be tuned for advanced applications such as logic circuits, thin-film polarizers, and polarization-sensitive photodetectors. ReS2 also presents advantages for optoelectronics, as it is both a direct-gap semiconductor for few-layer thicknesses (unlike MoS2 or WS2) and stable in air (unlike black phosphorus). Raman spectroscopy is one of the most powerful characterization techniques to nondestructively and sensitively probe the fundamental photophysics of a 2D material. Here, we perform a thorough study of the resonant Raman response of the 18 first-order phonons in ReS2 at various layer thicknesses and crystal orientations. Remarkably, we discover that, as opposed to a general increase in intensity of all of the Raman modes at excitonic transitions, each of the 18 modes behave differently relative to each other as a function of laser excitation, layer thickness, and orientation in a manner that highli...

We have performed a novel comparison between electron-beam polarimeters based on Møller and Compton scattering. A sequence of electron-beam polarization measurements were performed at low beam currents (< 5μA) during the Q[subscript weak] experiment in Hall-C at Jefferson Lab. These low current measurements were bracketed by the regular high current (180 μA) operation of the Compton polarimeter. All measurements were found to be consistent within experimental uncertainties of 1% or less, demonstrating that electron polarization does not depend significantly on the beam current. This result lends confidence to the common practice of applying Møller measurements made at low beam currents to physics experiments performed at higher beam currents. The agreement between two polarimetry techniques based on independent physical processes sets an important benchmark for future precision asymmetry measurements that require sub-1% precision in polarimetry. Keywords: Electron polarimetry, Compton polarimeter, Møller polarimeter, Jefferson Lab, United States. Department of Energy (Contract AC05-06OR23177), Natural Sciences and Engineering Research Council of Canada

Polarization-resolved Raman spectroscopy was performed and analyzed from large, high-quality, monodomain single crystal of $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$, a proximate Kitaev quantum spin liquid. Spectra were collected with laser polarizations parallel and perpendicular to the honeycomb plane. Pairs of nearly degenerate phonons were discovered and show either a fourfold or twofold polarization angle dependence in their Raman intensity, thereby providing evidence to definitively assign the bulk crystal point group as ${C}_{2h}$. The low-frequency continuum that is often attributed to scattering from pairs of Majorana fermions was also examined and found to disappear when the laser excitation and scattered photon polarizations were perpendicular to the honeycomb plane. This disappearance, along with the behavior of the phonon spectrum in the same polarization configuration, strongly suggests that the scattering continuum is two-dimensional. We argue that this scattering continuum originates from the Kitaev magnetic interactions that survives up to room temperature, a scale larger than the bare Kitaev exchange energy of approximately 50 K.

Transition metal dichalcogenides such as WS2 show exciting promise in electronic and optoelectronic applications. Significant variations in the transport, Raman, and photoluminescence (PL) can be found in the literature, yet it is rarely addressed why this is. In this report, Raman and PL of monolayered WS2 produced via different methods are studied and distinct features that indicate the degree of crystallinity of the material are observed. While the intensity of the LA(M) Raman mode is found to be a useful indicator to assess the crystallinity, PL is drastically more sensitive to the quality of the material than Raman spectroscopy. We also show that even exfoliated crystals, which are usually regarded as the most pristine material, can contain large amounts of defects that would not be apparent without Raman and PL measurements. These findings can be applied to the understanding of other two-dimensional heterostructured systems.

In recent years, research on two-dimensional (2D) materials including graphene and transition metal dichalcogenides (TMDCs), especially molybdenum and tungsten disulfides (MoS2 and WS2), has rapidly developed. In order to meet the increasing demands of using these 2D materials in fields as diverse as optoelectronics and sensing, heteroatom doping has become an effective method to tune their electronic and physico-chemical properties. This review discusses versatile doping methods applied to graphene and TMDCs, the corresponding changes to their properties, and their potential applications. Future perspectives and new emerging areas are also presented.

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., Scientific Reports 2018

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 $��_i$ ~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., 25 pages, 5 figures

The strong in-plane anisotropy of rhenium disulfide (ReS

Bound exciton is a signature of sulfur vacancies, and thus, it can be used to investigate defects in atomically thin materials., Defects play a significant role in tailoring the optical properties of two-dimensional materials. Optical signatures of defect-bound excitons are important tools to probe defective regions and thus interrogate the optical quality of as-grown semiconducting monolayer materials. We have performed a systematic study of defect-bound excitons using photoluminescence (PL) spectroscopy combined with atomically resolved scanning electron microscopy and first-principles calculations. Spatially resolved PL spectroscopy at low temperatures revealed bound excitons that were present only on the edges of monolayer tungsten disulfide and not in the interior. Optical pumping of the bound excitons was sublinear, confirming their bound nature. Atomic-resolution images reveal that the areal density of monosulfur vacancies is much larger near the edges (0.92 ± 0.45 nm−2) than in the interior (0.33 ± 0.11 nm−2). Temperature-dependent PL measurements found a thermal activation energy of ~36 meV; surprisingly, this is much smaller than the bound-exciton binding energy of ~300 meV. We show that this apparent inconsistency is related to a thermal dissociation of the bound exciton that liberates the neutral excitons from negatively charged point defects. First-principles calculations confirm that sulfur monovacancies introduce midgap states that host optical transitions with finite matrix elements, with emission energies ranging from 200 to 400 meV below the neutral-exciton emission line. These results demonstrate that bound-exciton emission induced by monosulfur vacancies is concentrated near the edges of as-grown monolayer tungsten disulfide.

One of the most fascinating properties of molybdenum disulfide (MoS2) is its ability to be subjected to large amounts of strain without experiencing degradation. The potential of MoS2 mono- and few-layers in electronics, optoelectronics, and flexible devices requires the fundamental understanding of their properties as a function of strain. While previous reports have studied mechanically exfoliated flakes, tensile strain experiments on chemical vapor deposition (CVD)-grown few-layered MoS2 have not been examined hitherto, although CVD is a state of the art synthesis technique with clear potential for scale-up processes. In this report, we used CVD-grown terrace MoS2 layers to study how the number and size of the layers affected the physical properties under uniaxial and biaxial tensile strain. Interestingly, we observed significant shifts in both the Raman in-plane mode (as high as -5.2 cm(-1)) and photoluminescence (PL) energy (as high as -88 meV) for the few-layered MoS2 under ∼1.5% applied uniaxial tensile strain when compared to monolayers and few-layers of MoS2 studied previously. We also observed slippage between the layers which resulted in a hysteresis of the Raman and PL spectra during further applications of strain. Through DFT calculations, we contended that this random layer slippage was due to defects present in CVD-grown materials. This work demonstrates that CVD-grown few-layered MoS2 is a realistic, exciting material for tuning its properties under tensile strain.

In ReS2, a layer-independent direct band gap of 1.5 eV implies a potential for its use in optoelectronic applications. ReS2 crystallizes in the 1T'-structure, which leads to anisotropic physical properties and whose concomitant electronic structure might host a nontrivial topology. Here, we report an overall evaluation of the anisotropic Raman response and the transport properties of few-layered ReS2 field-effect transistors. We find that ReS2 exfoliated on SiO2 behaves as an n-type semiconductor with an intrinsic carrier mobility surpassing μ(i) ∼ 30 cm(2)/(V s) at T = 300 K, which increases up to ∼350 cm(2)/(V s) at 2 K. Semiconducting behavior is observed at low electron densities n, but at high values of n the resistivity decreases by a factor of7 upon cooling to 2 K and displays a metallic T(2)-dependence. This suggests that the band structure of 1T'-ReS2 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 ReS2 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.

Heteroatom doping is an efficient way to modify the chemical and electronic properties of graphene. In particular, boron doping is expected to induce a p-type (boron)-conducting behavior to pristine (nondoped) graphene, which could lead to diverse applications. However, the experimental progress on atomic scale visualization and sensing properties of large-area boron-doped graphene (BG) sheets is still very scarce. This work describes the controlled growth of centimeter size, high-crystallinity BG sheets. Scanning tunneling microscopy and spectroscopy are used to visualize the atomic structure and the local density of states around boron dopants. It is confirmed that BG behaves as a p-type conductor and a unique croissant-like feature is frequently observed within the BG lattice, which is caused by the presence of boron-carbon trimers embedded within the hexagonal lattice. More interestingly, it is demonstrated for the first time that BG exhibits unique sensing capabilities when detecting toxic gases, such as NO2 and NH3, being able to detect extremely low concentrations (e.g., parts per trillion, parts per billion). This work envisions that other attractive applications could now be explored based on as-synthesized BG.

We report on the highest precision yet achieved in the measurement of the polarization of a low-energy, O(1 GeV), continuous-wave (CW) electron beam, accomplished using a new polarimeter based on electron-photon scattering, in Hall C at Jefferson Lab. A number of technical innovations were necessary, including a novel method for precise control of the laser polarization in a cavity and a novel diamond microstrip detector that was able to capture most of the spectrum of scattered electrons. The data analysis technique exploited track finding, the high granularity of the detector, and its large acceptance. The polarization of the 180-μA, 1.16-GeV electron beam was measured with a statistical precision of, United States. Dept. of Energy (Contract AC05-06OR23177), National Science Foundation (U.S.), Natural Sciences and Engineering Research Council of Canada

The Jefferson Lab Q weak experiment determined the weak charge of the proton by measuring the parity-violating elastic scattering asymmetry of longitudinally polarized electrons from an unpolarized liquid hydrogen target at small momentum transfer. A custom apparatus was designed for this experiment to meet the technical challenges presented by the smallest and most precise e → p asymmetry ever measured. Technical milestones were achieved at Jefferson Lab in target power, beam current, beam helicity reversal rate, polarimetry, detected rates, and control of helicity-correlated beam properties. The experiment employed 180 μA of 89% longitudinally polarized electrons whose helicity was reversed 960 times per second. The electrons were accelerated to 1.16 GeV and directed to a beamline with extensive instrumentation to measure helicity-correlated beam properties that can induce false asymmetries. Moller and Compton polarimetry were used to measure the electron beam polarization to better than 1%. The electron beam was incident on a 34.4 cm liquid hydrogen target. After passing through a triple collimator system, scattered electrons between 5.8° and 11.6° were bent in the toroidal magnetic field of a resistive copper-coil magnet. The electrons inside this acceptance were focused onto eight fused silica Cherenkov detectors arrayed symmetrically around the beam axis. A total scattered electron rate of about 7 GHz was incident on the detector array. The detectors were read out in integrating mode by custom-built low-noise pre-amplifiers and 18-bit sampling ADC modules. The momentum transfer Q 2 =0.025 GeV 2 was determined using dedicated low-current ( ~ 100 pA ) measurements with a set of drift chambers before (and a set of drift chambers and trigger scintillation counters after) the toroidal magnet.

Author(s): Lin, Z; McCreary, A; Briggs, N; Subramanian, S; Zhang, K; Sun, Y; Li, X; Borys, NJ; Yuan, H; Fullerton-Shirey, SK; Chernikov, A; Zhao, H; McDonnell, S; Lindenberg, AM; Xiao, K; Le Roy, BJ; Drndic, M; Hwang, JCM; Park, J; Chhowalla, M; Schaak, RE; Javey, A; Hersam, MC; Robinson, J; Terrones, M | Abstract: The rise of two-dimensional (2D) materials research took place following the isolation of graphene in 2004. These new 2D materials include transition metal dichalcogenides, mono-elemental 2D sheets, and several carbide- and nitride-based materials. The number of publications related to these emerging materials has been drastically increasing over the last five years. Thus, through this comprehensive review, we aim to discuss the most recent groundbreaking discoveries as well as emerging opportunities and remaining challenges. This review starts out by delving into the improved methods of producing these new 2D materials via controlled exfoliation, metal organic chemical vapor deposition, and wet chemical means. We look into recent studies of doping as well as the optical properties of 2D materials and their heterostructures. Recent advances towards applications of these materials in 2D electronics are also reviewed, and include the tunnel MOSFET and ways to reduce the contact resistance for fabricating high-quality devices. Finally, several unique and innovative applications recently explored are discussed as well as perspectives of this exciting and fast moving field.

We have measured the beam-normal single-spin asymmetry $A_n$ in the elastic scattering of 1-3 GeV transversely polarized electrons from $^1$H and for the first time from $^4$He, $^{12}$C, and $^{208}$Pb. For $^1$H, $^4$He and $^{12}$C, the measurements are in agreement with calculations that relate $A_n$ to the imaginary part of the two-photon exchange amplitude including inelastic intermediate states. Surprisingly, the $^{208}$Pb result is significantly smaller than the corresponding prediction using the same formalism. These results suggest that a systematic set of new $A_n$ measurements might emerge as a new and sensitive probe of the structure of heavy nuclei., 5 pages, 3 figures, accepted by PRL. v3: fixed one author name and affiliation, otherwise no change

We report the fabrication of a photosensor based on as-grown single crystal monolayers of MoS2 synthesized by chemical vapor deposition (CVD). The measurements were performed using Au/Ti leads in a two terminal configuration on CVD-grown MoS2 on a SiO2/Si substrate. The device was operated in air at room temperature at low bias voltages ranging from −2 V to 2 V and its sensing capabilities were tested for two different excitation wavelengths (514.5 nm and 488 nm). The responsivity reached 1.1 mA W−1 when excited with a 514.5 nm laser at a bias of 1.5 V. This responsivity is one order of magnitude larger than that reported from photo devices fabricated using CVD-grown multilayered WS2. A rectifying-effect was observed for the optically excited current, which was four times larger in the direct polarization bias when compared to the reverse bias photocurrent. Such rectifying behavior can be attributed to the asymmetric electrode placement on the triangular MoS2 monocrystal. It is envisioned that these components could eventually be used as efficient and low cost photosensors based on CVD-grown transition metal dichalcogenide monolayers.