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We conducted a tip-enhanced Raman scattering spectroscopy (TERS) and photoluminescence (PL) study of quasi-1D TaSe3 nanoribbons exfoliated onto gold substrates. At a selenium deficiency of ~0.25 (Se/Ta=2.75,), the nanoribbons exhibit a strong, broad PL peak centered around ~920 nm (1.35 eV), suggesting their semiconducting behavior. Such nanoribbons revealed a strong TERS response under 785-nm laser excitation, allowing for their nanoscale spectroscopic imaging. Nanoribbons with a smaller selenium deficiency of ~0.15 (Se/Ta=2.85) did not show any PL or TERS response. The confocal Raman spectra of these samples agree with the previously-reported spectra of metallic TaSe3. The differences in the optical response of the nanoribbons examined in this study suggest that even small variations in Se content can induce changes in electronic structure, causing samples to exhibit either metallic or semiconducting character. The temperature-dependent electrical measurements of devices fabricated with both types of materials corroborate these observations. The density-functional-theory calculations revealed that incorporation of an oxygen atom in a Se vacancy can result in band gap opening and thus enable the transition from a metal to a semiconductor. However, the predicted bandgap is substantially smaller than that derived from PL data. These results indicate that the properties of van der Waals materials can vary significantly depending on stoichiometry, defect types and concentration, and possibly environmental and substrate effects. In view of this finding, local probing of nanoribbon properties with TERS becomes essential to understanding such low-dimensional systems., Comment: 24 pages, 8 figures

One of the main tasks in the investigation of 2-dimensional transition metal dichalcogenides is the determination of valley lifetimes. In this work, we combine time-resolved Kerr rotation with electrical transport measurements to explore the gate-dependent valley lifetimes of free conduction band electrons of monolayer WSe$_2$. When tuning the Fermi energy into the conduction band we observe a strong decrease of the respective valley lifetimes which is consistent with both spin-orbit and electron-phonon scattering. We explain the formation of a valley polarization by the scattering of optically excited valley polarized bright trions into dark states by intervalley scattering. Furthermore, we show that the conventional time-resolved Kerr rotation measurement scheme has to be modified to account for photo-induced gate screening effects. Disregarding this adaptation can lead to erroneous conclusions drawn from gate-dependent optical measurements and can completely mask the true gate-dependent valley dynamics., Comment: 5 pages, 3 figures

We report on nanosecond long, gate-dependent valley lifetimes of free charge carriers in monolayer WSe$_2$, unambiguously identified by the combination of time-resolved Kerr rotation and electrical transport measurements. While the valley polarization increases when tuning the Fermi level into the conduction or valence band, there is a strong decrease of the respective valley lifetime consistent with both electron-phonon and spin-orbit scattering. The longest lifetimes are seen for spin-polarized bound excitons in the band gap region. We explain our findings via two distinct, Fermi level-dependent scattering channels of optically excited, valley polarized bright trions either via dark or bound states. By electrostatic gating we demonstrate that the transition metal dichalcogenide WSe$_2$ can be tuned to be either an ideal host for long-lived localized spin states or allow for nanosecond valley lifetimes of free charge carriers (> 10 ns)., Comment: 22 pages, 13 figures

Micron-scale single-crystal nanowires of metallic TaSe3, a material that forms -Ta-Se3-Ta-Se3- stacks separated from one another by a tubular van der Waals (vdW) gap, have been synthesized using chemical vapor deposition (CVD) on a SiO2/Si substrate, in a process compatible with semiconductor industry requirements. Their electrical resistivity was found unaffected by downscaling from the bulk to as little as 7 nm in width and height, in striking contrast to the resistivity of copper for the same dimensions. While the bulk resistivity of TaSe3 is substantially higher than that of bulk copper, at the nanometer scale the TaSe3 wires become competitive to similar-sized copper ones. Moreover, we find that the vdW TaSe3 nanowires sustain current densities in excess of 108 A/cm2 and feature an electromigration energy barrier twice that of copper. The results highlight the promise of quasi-one-dimensional transition metal trichalcogenides for electronic interconnect applications and the potential of van der Waals materials for downscaled electronics.

Atomically thin two-dimensional (2D) materials provide a wide range of basic building blocks with unique properties, making them ideal for heterogeneous integration with a mature chip platform for advances in optical communication technology. Control and understanding of the precise value of the optical index of these materials, however, is challenging, due to the small lateral flake dimension. Here we demonstrate a semi-empirical method to determine the index of a 2D material (nMoTe2 of 4.36+0.011i) near telecommunication-relevant wavelength by integrating few layers of MoTe2 onto a micro-ring resonator. The placement, control, and optical-property understanding of 2D materials with integrated photonics paves a way for further studies of active 2D material-based optoelectronics and circuits., Comment: arXiv admin note: substantial text overlap with arXiv:1807.03945

Spin-orbit coupling (SOC) in graphene can be greatly enhanced by proximity coupling it to transition metal dichalcogenides (TMDs) such as WSe2. We find that the strength of the acquired SOC in graphene depends on the stacking order of the heterostructures when using hexagonal boron nitride (h-BN) as the capping layer, i.e., SiO2/graphene/WSe2/h-BN exhibiting stronger SOC than SiO2/WSe2/graphene/h-BN. We utilize photoluminescence (PL) as an indicator to characterize the interaction between graphene and monolayer WSe2 grown by chemical vapor deposition. We observe much stronger PL quenching in the SiO2/graphene/WSe2/h-BN stack than in the SiO2/WSe2/graphene/h-BN stack, and correspondingly a much larger weak antilocalization (WAL) effect or stronger induced SOC in the former than in the latter. We attribute these two effects to the interlayer distance between graphene and WSe2, which depends on whether graphene is in immediate contact with h-BN. Our observations and hypothesis are further supported by first-principles calculations which reveal a clear difference in the interlayer distance between graphene and WSe2 in these two stacks.

Precision and chip contamination-free placement of two-dimensional (2D) materials is expected to accelerate both the study of fundamental properties and novel device functionality. Current transfer methods of 2D materials onto an arbitrary substrate deploy wet chemistry and viscoelastic stamping. However, these methods produce a) significant cross contamination of the substrate due to the lack of spatial selectivity b) may not be compatible with chemically sensitive device structures, and c) are challenged with respect to spatial alignment. Here, we demonstrate a novel method of transferring 2D materials resembling the functionality known from printing; utilizing a combination of a sharp micro-stamper and viscoelastic polymer, we show precise placement of individual 2D materials resulting in vanishing cross contamination to the substrate. Our 2D printer-method results show an aerial cross contamination improvement of two to three orders of magnitude relative to state-of-the-art dry and direct transfer methods. Moreover, we find that the 2D material quality is preserved in this transfer method. Testing this 2D material printer on taped-out integrated Silicon photonic chips, we find that the micro-stamper stamping transfer does not physically harm the underneath Silicon nanophotonic structures such as waveguides or micro-ring resonators receiving the 2D material. Such accurate and substrate-benign transfer method for 2D materials could be industrialized for rapid device prototyping due to its high time-reduction, accuracy, and contamination-free process.

Despite its extremely weak intrinsic spin-orbit coupling (SOC), graphene has been shown to acquire considerable SOC by proximity coupling with exfoliated transition metal dichalcogenides (TMDs). Here we demonstrate strong induced Rashba SOC in graphene that is proximity coupled to a monolayer TMD film, MoS2 or WSe2, grown by chemical vapor deposition with drastically different Fermi level positions. Graphene/TMD heterostructures are fabricated with a pickup-transfer technique utilizing hexagonal boron nitride, which serves as a flat template to promote intimate contact and therefore a strong interfacial interaction between TMD and graphene as evidenced by quenching of the TMD photoluminescence. We observe strong induced graphene SOC that manifests itself in a pronounced weak anti-localization (WAL) effect in the graphene magnetoconductance. The spin relaxation rate extracted from the WAL analysis varies linearly with the momentum scattering time and is independent of the carrier type. This indicates a dominantly Dyakonov-Perel spin relaxation mechanism caused by the induced Rashba SOC. Our analysis yields a Rashba SOC energy of ~1.5 meV in graphene/WSe2 and ~0.9 meV in graphene/MoS2, respectively. The nearly electron-hole symmetric nature of the induced Rashba SOC provides a clue to possible underlying SOC mechanisms.

We report the fully-scalable fabrication of a large array of hybrid molybdenum disulfide (MoS$_2$) - silicon dioxide (SiO$_2$) one-dimensional, free-standing photonic-crystal cavities capable of enhancement of the MoS$_2$ photoluminescence at the narrow cavity resonance. We demonstrate continuous tunability of the cavity resonance wavelength across the entire emission band of MoS$_2$ simply by variation of the photonic crystal periodicity. Device fabrication started by substrate-scale growth of MoS$_2$ using chemical vapor deposition (CVD) on non-birefringent thermal oxide on a silicon wafer; it was followed by lithographic fabrication of a photon crystal nanocavity array on the same substrate at more than 50% yield of functional devices. Our cavities exhibit three dominant modes with measured linewidths less than 0.2 nm, corresponding to quality factors exceeding 4000. All experimental findings are found to be in excellent agreement with finite difference time domain simulations., Comment: accepted for Scientific Reports (2017)