Chemical vapor sensing with monolayer MoS2.

Two-dimensional materials such as graphene show great potential for future nanoscale electronic devices. The high surface-to-volume ratio is a natural asset for applications such as chemical sensing, where perturbations to the surface resulting in charge redistribution are readily manifested in the transport characteristics. Here we show that single monolayer MoS(2) functions effectively as a chemical sensor, exhibiting highly selective reactivity to a range of analytes and providing sensitive transduction of transient surface physisorption events to the conductance of the monolayer channel. We find strong response upon exposure to triethylamine, a decomposition product of the V-series nerve gas agents. We discuss these results in the context of analyte/sensor interaction in which the analyte serves as either an electron donor or acceptor, producing a temporary charge perturbation of the sensor material. We find highly selective response to electron donors and little response to electron acceptors, consistent with the weak n-type character of our MoS(2). The MoS(2) sensor exhibits a much higher selectivity than carbon nanotube-based sensors.

Electrical detection of current generated spin in topological insulator surface states: Role of interface resistance.

Current generated spin polarization in topological insulator (TI) surface states due to spin-momentum locking has been detected recently using ferromagnet/tunnel barrier contacts, where the projection of the TI spin onto the magnetization of the ferromagnet is measured as a voltage. However, opposing signs of the spin voltage have been reported, which had been tentatively attributed to the coexistence of trivial two-dimensional electron gas states on the TI surface which may exhibit opposite current-induced polarization than that of the TI Dirac surface states. Models based on electrochemical potential have been presented to determine the sign of the spin voltage expected for the TI surface states. However, these models neglect critical experimental parameters which also affect the sign measured. Here we present a Mott two-spin current resistor model which takes into account these parameters such as spin-dependent interface resistances, and show that such inclusion can lead to a crossing of the voltage potential profiles for the spin-up and spin-down electrons within the channel, which can lead to measured spin voltages of either sign. These findings offer a resolution of the ongoing controversy regarding opposite signs of spin signal reported in the literature, and highlight the importance of including realistic experimental parameters in the model.

Electrical Detection of Charge-to-spin and Spin-to-Charge Conversion in a Topological Insulator Bi2Te3 Using BN/Al2O3 Hybrid Tunnel Barrier.

One of the most striking properties of three-dimensional topological insulators (TIs) is spin-momentum locking, where the spin is locked at right angles to momentum and hence an unpolarized charge current creates a net spin polarization. Alternatively, if a net spin is injected into the TI surface state system, it is distinctively associated with a unique carrier momentum and hence should generate a charge accumulation, as in the so-called inverse Edelstein effect. Here using a Fe/Al2O3/BN tunnel barrier, we demonstrate both effects in a single device in Bi2Te3: the electrical detection of the spin accumulation generated by an unpolarized current flowing through the surface states, and that of the charge accumulation generated by spins injected into the surface state system. This work is the first to utilize BN as part of a hybrid tunnel barrier on TI, where we observed a high spin polarization of 93% for the TI surfaces states. The reverse spin-to-charge measurement is an independent confirmation that spin and momentum are locked in the surface states of TI, and offers additional avenues for spin manipulation. It further demonstrates the robustness and versatility of electrical access to the spin system within TI surface states, an important step towards its utilization in TI-based spintronics devices.

Optical polarization of excitons and trions under continuous and pulsed excitation in single layers of WSe2.

The potential for valleytronic operation has stimulated much interest in studying polarized emission from transition metal dichalcogenides. In most studies, however, little regard is given to the character of laser excitation. We measure the circularly polarized photoluminescence of WSe2 monolayers as a function of excitation energy for both continuous-wave (cw) and pulsed laser excitation sources. Using cw excitation, the temperature dependence of the depolarization of the trion follows the same trend as that of the neutral exciton and involves collisional broadening. However, the polarization of the trion is nearly twice the polarization of the neutral exciton at low temperatures. When a pulsed laser with the same average fluence is used as the excitation source, the degrees of polarization become very similar, in stark contrast to the cw results. The difference in polarization behaviors is linked to the different amounts of energy deposited in the system during these measurements for similar average fluences. At a moderate fluence, pulsed excitation also has the potential to fundamentally alter the emission characteristics of WSe2.

Electrical Detection of the Helical Spin Texture in a p-type Topological Insulator Sb2Te3.

The surface states of 3D topological insulators (TIs) exhibit a helical spin texture with spin locked at right angles with momentum. The chirality of this spin texture is expected to invert crossing the Dirac point, a property that has been experimentally observed by optical probes. Here, we directly determine the chirality below the Dirac point by electrically detecting spin-momentum locking in surface states of a p-type TI, Sb2Te3. A current flowing in the Sb2Te3 surface states generates a net spin polarization due to spin-momentum locking, which is electrically detected as a voltage on an Fe/Al2O3 tunnel barrier detector. Measurements of this voltage as a function of current direction and detector magnetization indicate that hole spin-momentum locking follows the right-hand rule, opposite that of electron, providing direct confirmation that the chirality is indeed inverted below Dirac point. The spin signal is linear with current, and exhibits a temperature dependence consistent with the semiconducting nature of the TI film and freeze-out of bulk conduction below 100 K. Our results demonstrate that the chirality of the helical spin texture of TI surface states can be determined electrically, an enabling step in the electrical manipulation of spins in next generation TI-based quantum devices.

Direct comparison of current-induced spin polarization in topological insulator Bi2Se3 and InAs Rashba states.

Three-dimensional topological insulators (TIs) exhibit time-reversal symmetry protected, linearly dispersing Dirac surface states with spin-momentum locking. Band bending at the TI surface may also lead to coexisting trivial two-dimensional electron gas (2DEG) states with parabolic energy dispersion. A bias current is expected to generate spin polarization in both systems, although with different magnitude and sign. Here we compare spin potentiometric measurements of bias current-generated spin polarization in Bi2Se3(111) where Dirac surface states coexist with trivial 2DEG states, and in InAs(001) where only trivial 2DEG states are present. We observe spin polarization arising from spin-momentum locking in both cases, with opposite signs of the measured spin voltage. We present a model based on spin dependent electrochemical potentials to directly derive the sign expected for the Dirac surface states, and show that the dominant contribution to the current-generated spin polarization in the TI is from the Dirac surface states.

Optical polarization and intervalley scattering in single layers of MoS2 and MoSe2.

Single layers of MoS2 and MoSe2 were optically pumped with circularly polarized light and an appreciable polarization was initialized as the pump energy was varied. The circular polarization of the emitted photoluminescence was monitored as a function of the difference between the excitation energy and the A-exciton emission at the K-point of the Brillouin zone. Our results show a threshold of twice the LA phonon energy, specific to the material, above which phonon-assisted intervalley scattering causes depolarization. In both materials this leads to almost complete depolarization within ~100 meV above the threshold energy. We identify the extra kinetic energy of the exciton (independent of whether it is neutral or charged) as the key parameter for presenting a unifying picture of the depolarization process.

Anomalous temperature-dependent spin-valley polarization in monolayer WS2.

Single layers of transition metal dichalcogenides (TMDs) are direct gap semiconductors with nondegenerate valley indices. An intriguing possibility for these materials is the use of their valley index as an alternate state variable. Several limitations to such a utility include strong intervalley scattering, as well as multiparticle interactions leading to multiple emission channels. We prepare single-layer WS2 films such that the photoluminescence is from either the neutral or charged exciton (trion). After excitation with circularly polarized light, the neutral exciton emission has zero polarization. However, the trion emission has a large polarization (28%) at room temperature. The trion emission also has a unique, non-monotonic temperature dependence that is a consequence of the multiparticle nature of the trion. This temperature dependence enables us to determine that intervalley scattering, electron-hole radiative recombination, and Auger processes are the dominant mechanisms at work in this system. Because this dependence involves trion systems, one can use gate voltages to modulate the polarization (or intensity) emitted from TMD structures.

Spin transport and Hanle effect in silicon nanowires using graphene tunnel barriers.

Spin-based devices offer non-volatile, scalable, low power and reprogrammable functionality for emerging device technologies. Here we fabricate nanoscale spintronic devices with ferromagnetic metal/single-layer graphene tunnel barriers used to generate spin accumulation and spin currents in a silicon nanowire transport channel. We report the first observation of spin precession via the Hanle effect in both local three-terminal and non-local spin-valve geometries, providing a direct measure of spin lifetimes and confirmation of spin accumulation and pure spin transport. The use of graphene as the tunnel barrier provides a low-resistance area product contact and clean magnetic switching characteristics, because it smoothly bridges the nanowire and minimizes complicated magnetic domains that otherwise compromise the magnetic behaviour. Utilizing intrinsic two-dimensional layers such as graphene or hexagonal boron nitride as tunnel contacts on nanowires offers many advantages over conventional materials deposited by vapour deposition, enabling a path to highly scaled electronic and spintronic devices.

Electrical detection of charge-current-induced spin polarization due to spin-momentum locking in Bi2Se3.

Topological insulators exhibit metallic surface states populated by massless Dirac fermions with spin-momentum locking, where the carrier spin lies in-plane, locked at right angles to the carrier momentum. Here, we show that a charge current produces a net spin polarization via spin-momentum locking in Bi2Se3 films, and this polarization is directly manifested as a voltage on a ferromagnetic contact. This voltage is proportional to the projection of the spin polarization onto the contact magnetization, is determined by the direction and magnitude of the charge current, scales inversely with Bi2Se3 film thickness, and its sign is that expected from spin-momentum locking rather than Rashba effects. Similar data are obtained for two different ferromagnetic contacts, demonstrating that these behaviours are independent of the details of the ferromagnetic contact. These results demonstrate direct electrical access to the topological insulators' surface-state spin system and enable utilization of its remarkable properties for future technological applications.

Exchange bias of the interface spin system at the Fe/MgO interface.

The ferromagnet/oxide interface is key to developing emerging multiferroic and spintronic technologies with new functionality. Here we probe the Fe/MgO interface magnetization, and identify a new exchange bias phenomenon manifested only in the interface spin system, and not in the bulk. The interface magnetization exhibits a pronounced exchange bias, and the hysteresis loop is shifted entirely to one side of the zero field axis. However, the bulk magnetization does not, in marked contrast to typical systems where exchange bias is manifested in the net magnetization. This reveals the existence of an antiferromagnetic exchange pinning layer at the interface, identified here as FeO patches that exist even for a nominally 'clean' interface. These results demonstrate that atomic moments at the interface are non-collinear with the bulk magnetization, and therefore may affect the net anisotropy or serve as spin scattering sites. We control the exchange bias magnitude by varying the interface oxygen concentration and Fe-O bonding.

Low-resistance spin injection into silicon using graphene tunnel barriers.

Spin manipulation in a semiconductor offers a new paradigm for device operation beyond Moore's law. Ferromagnetic metals are ideal contacts for spin injection and detection, but the intervening tunnel barrier required to accommodate the large difference in conductivity introduces defects, trapped charge and material interdiffusion, which severely compromise performance. Here, we show that single-layer graphene successfully circumvents the classic issue of conductivity mismatch between a metal and a semiconductor for electrical spin injection and detection, providing a highly uniform, chemically inert and thermally robust tunnel barrier. We demonstrate electrical generation and detection of spin accumulation in silicon above room temperature, and show that the contact resistance-area products are two to three orders of magnitude lower than those achieved with oxide tunnel barriers on silicon substrates with identical doping levels. Our results identify a new route to low resistance-area product spin-polarized contacts, a key requirement for semiconductor spintronic devices that rely on two-terminal magnetoresistance, including spin-based transistors, logic and memory.

Electrical injection and detection of spin accumulation in silicon at 500 K with magnetic metal/silicon dioxide contacts.

The International Technology Roadmap for Semiconductors has identified the electron's spin angular momentum as a new state variable that should be explored as an alternative to the electron's charge for use beyond the size scaling of Moore's Law. A major obstacle has been achieving control of the spin variable at temperatures required for practical applications. Here we demonstrate electrical injection, detection and precession of spin accumulation in silicon, the cornerstone material of device technology, at temperatures that easily exceed these requirements. We observe Hanle precession of electron spin accumulation in silicon for a wide range of bias, show that the magnitude of the Hanle signal agrees well with theory, and that the spin lifetime varies with silicon carrier density. These results confirm spin accumulation in the silicon transport channel to 500 K rather than trapping in localized interface states, and enable utilization of the spin variable in practical device applications.

Intershell exchange and sequential electrically injected spin populations of InAs quantum-dot shell states.

We report sequential spin population of individual shell states of self-assembled InAs quantum dots controlled by a spin-polarized current from an Fe contact, and determine the s-p and p-d intershell exchange energies. We resolve excitonic features in the electroluminescence (EL) spectra associated with individual quantum levels. In contrast with simple models of shell occupation, the EL circular polarization exhibits maxima shifted with respect to the intensity peaks. Calculations show that this is due to intershell exchange. Exchange energies for the s-p and p-d shells are 7+/-2 and 13.5+/-1 meV, respectively.

Interface magnetization reversal and anisotropy in Fe/AlGaAs(001).

The reversal process of the Fe interface layer magnetization in Fe/AlGaAs heterostructures is measured directly using magnetization-induced second-harmonic generation, and is compared with the reversal of the bulk magnetization as obtained from magneto-optic Kerr effect. The switching characteristics are distinctly different due to interface-derived anisotropy--single step switching occurs at the interface layer, while two-jump switching occurs in the bulk Fe for the magnetic field orientations employed. The angle between the interface and bulk magnetization may be as large as 40-85 degrees. Such interface switching will dominate the behavior of nanoscale structures.

Reduction of spin injection efficiency by interface defect spin scattering in ZnMnSe/AlGaAs-GaAs spin-polarized light-emitting diodes.

We report the first experimental demonstration that interface microstructure limits diffusive electrical spin-injection efficiency across heteroepitaxial interfaces. An inverse correlation be-tween spin-polarized electron injection efficiency and interface defect density is demonstrated for ZnMnSe/AlGaAs-GaAs spin-polarized light-emitting diodes that exhibit quantum well spin polarizations up to 85%. A theoretical treatment shows that the suppression of spin injection due to interface defects results from the contribution of the defect potential to the spin-orbit interaction, which increases the spin-flip scattering.

A group-IV ferromagnetic semiconductor: MnxGe1-x.

We report on the epitaxial growth of a group-IV ferromagnetic semiconductor, Mn(x)Ge(1-x), in which the Curie temperature is found to increase linearly with manganese (Mn) concentration from 25 to 116 kelvin. The p-type semiconducting character and hole-mediated exchange permit control of ferromagnetic order through application of a +/-0.5-volt gate voltage, a value compatible with present microelectronic technology. Total-energy calculations within density-functional theory show that the magnetically ordered phase arises from a long-range ferromagnetic interaction that dominates a short-range antiferromagnetic interaction. Calculated spin interactions and percolation theory predict transition temperatures larger than measured, consistent with the observed suppression of magnetically active Mn atoms and hole concentration.