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We report on the temperature evolution of the polarization-dependent Raman spectrum of exfoliated MoI$_3$, a van der Waals material with a "true one-dimensional" crystal structure that can be exfoliated to individual atomic chains. The temperature evolution of several Raman features reveals anomalous behavior suggesting a phase transition of a magnetic origin. Theoretical considerations indicate that MoI$_3$ is an easy-plane antiferromagnet with alternating spins along the dimerized chains and with inter-chain helical spin ordering. The calculated frequencies of the phonons and magnons are consistent with the interpretation of the experimental Raman data. The obtained results shed light on the specifics of the phononic and magnonic states in MoI$_3$ and provide a strong motivation for future study of this unique material with potential for spintronic device applications., Comment: 28 pages

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

Here we discuss the physics of electro-optic modulators deploying 2D materials. We include a scaling laws analysis showing how energy-efficiency and speed change for three underlying cavity systems as a function of critical device length scaling. A key result is that the energy-per-bit of the modulator is proportional to the volume of the device, thus making the case for submicron-scale modulators possible deploying a plasmonic optical mode. We then show how Graphenes Pauli-blocking modulation mechanism is sensitive to the device operation temperature, whereby a reduction of the temperature enables a 10x reduction in modulator energy efficiency. Furthermore, we show how the high index tunability of Graphene is able to compensate for the small optical overlap factor of 2D-based material modulators, which is unlike classical Silicon-based dispersion devices. Lastly we demonstrate a novel method towards a 2D material printer suitable for cross-contamination free and on-demand printing. The latter paves the way to integrate 2D materials seamlessly into taped-out photonic chips.

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)

Monolayer transition metal dichalcogenides are uniquely-qualified materials for photonics because they combine well defined tunable direct band gaps and selfpassivated surfaces without dangling bonds. However, the atomic thickness of these 2D materials results in low photo absorption limiting the achievable photo luminescence intensity. Such emission can, in principle, be enhanced via nanoscale antennae resulting in; a. an increased absorption cross-section enhancing pump efficiency, b. an acceleration of the internal emission rate via the Purcell factor mainly by reducing the antennas optical mode volume beyond the diffraction limit, and c. improved impedance matching of the emitter dipole to the freespace wavelength. Plasmonic dimer antennae show orders of magnitude hot-spot field enhancements when an emitter is positioned exactly at the midgap. However, a 2D material cannot be grown, or easily transferred, to reside in mid-gap of the metallic dimer cavity. In addition, a spacer layer between the cavity and the emissive material is required to avoid non-radiative recombination channels. Using both computational and experimental methods, in this work we show that the emission enhancement from a 2D emitter- monomer antenna cavity system rivals that of dimers at much reduced lithographic effort. We rationalize this finding by showing that the emission enhancement in dimer antennae does not specifically originate from the gap of the dimer cavity, but is an average effect originating from the effective cavity crosssection taken below each optical cavity where the emitting 2D film is located. In particular, we test an array of different dimer and monomer antenna geometries and observe a representative 3x higher emission for both monomer and dimer cavities as compared to intrinsic emission of Chemical Vapor Deposition synthesized WS2 flakes., Comment: 31 pages, 5 figures

We report on fabrication of large-scale arrays of suspended molybdenum disulfide (MoS2) atomic layers, as two-dimensional (2D) MoS2 nanomechanical resonators. We employ a water-assisted lift-off process to release chemical vapor deposited (CVD) MoS2 atomic layers from a donor substrate, followed by an all-dry transfer onto microtrench arrays. The resultant large arrays of suspended single- and few-layer MoS2 drumhead resonators (0.5 to 2um in diameter) offer fundamental resonances (f_0) in the very high frequency (VHF) band (up to ~120MHz) and excellent figures-of-merit up to f_0*Q ~ 3*10^10Hz. A stretched circular diaphragm model allows us to estimate low pre-tension levels of typically ~15mN/m in these devices. Compared to previous approaches, our transfer process features high yield and uniformity with minimal liquid and chemical exposure (only involving DI water), resulting in high-quality MoS2 crystals and exceptional device performance and homogeneity; and our process is readily applicable to other 2D materials., Comment: 14 pages, 6 figures