Jinsong Xu

Opto-Valleytronic Spin Injection in Monolayer MoS2/Few-Layer Graphene Hybrid Spin Valves

Two-dimensional (2D) materials provide a unique platform for spintronics and valleytronics due to the ability to combine vastly different functionalities into one vertically stacked heterostructure, where the strengths of each of the constituent materials can compensate for the weaknesses of the others. Graphene has been demonstrated to be an exceptional material for spin transport at room temperature; however, it lacks a coupling of the spin and optical degrees of freedom. In contrast, spin/valley polarization can be efficiently generated in monolayer transition metal dichalcogenides (TMD) such as MoS2 via absorption of circularly polarized photons, but lateral spin or valley transport has not been realized at room temperature. In this Letter, we fabricate monolayer MoS2/few-layer graphene hybrid spin valves and demonstrate, for the first time, the opto-valleytronic spin injection across a TMD/graphene interface. We observe that the magnitude and direction of spin polarization is controlled by both helicity and photon energy. In addition, Hanle spin precession measurements confirm optical spin injection, spin transport, and electrical detection up to room temperature. Finally, analysis by a one-dimensional drift-diffusion model quantifies the optically injected spin current and the spin transport parameters. Our results demonstrate a 2D spintronic/valleytronic system that achieves optical spin injection and lateral spin transport at room temperature in a single device, which paves the way for multifunctional 2D spintronic devices for memory and logic applications.

Nanosecond spin relaxation times in single layer graphene spin valves with hexagonal boron nitride tunnel barriers

We present an experimental study of spin transport in single layer graphene using atomic sheets of hexagonal boron nitride (h-BN) as a tunnel barrier for spin injection. While h-BN is expected to be favorable for spin injection, previous experimental studies have been unable to achieve spin relaxation times in the nanosecond regime, suggesting potential problems originating from the contacts. Here, we investigate spin relaxation in graphene spin valves with h-BN barriers and observe room temperature spin lifetimes in excess of a nanosecond, which provides experimental confirmation that h-BN is indeed a good barrier material for spin injection into graphene. By carrying out measurements with different thicknesses of h-BN, we show that few layer h-BN is a better choice than monolayer for achieving high non-local spin signals and longer spin relaxation times in graphene.

NaSn2As2: An Exfoliatable Layered van der Waals Zintl Phase.

The discovery of new families of exfoliatable 2D crystals that have diverse sets of electronic, optical, and spin-orbit coupling properties enables the realization of unique physical phenomena in these few-atom-thick building blocks and in proximity to other materials. Herein, using NaSn2As2 as a model system, we demonstrate that layered Zintl phases having the stoichiometry ATt2Pn2 (A = group 1 or 2 element, Tt = group 14 tetrel element, and Pn = group 15 pnictogen element) and feature networks separated by van der Waals gaps can be readily exfoliated with both mechanical and liquid-phase methods. We identified the symmetries of the Raman-active modes of the bulk crystals via polarized Raman spectroscopy. The bulk and mechanically exfoliated NaSn2As2 samples are resistant toward oxidation, with only the top surface oxidizing in ambient conditions over a couple of days, while the liquid-exfoliated samples oxidize much more quickly in ambient conditions. Employing angle-resolved photoemission spectroscopy, density functional theory, and transport on bulk and exfoliated samples, we show that NaSn2As2 is a highly conducting 2D semimetal, with resistivities on the order of 10-6 Ω·m. Due to peculiarities in the band structure, the dominating p-type carriers at low temperature are nearly compensated by the opening of n-type conduction channels as temperature increases. This work further expands the family of exfoliatable 2D materials to layered van der Waals Zintl phases, opening up opportunities in electronics and spintronics.

Spatially Resolved Electronic Properties of Single-Layer WS2 on Transition Metal Oxides

There is a substantial interest in the heterostructures of semiconducting transition metal dichalcogenides (TMDCs) among each other or with arbitrary materials, through which the control of the chemical, structural, electronic, spintronic, and optical properties can lead to a change in device paradigms. A critical need is to understand the interface between TMDCs and insulating substrates, for example, high-κ dielectrics, which can strongly impact the electronic properties such as the optical gap. Here, we show that the chemical and electronic properties of the single-layer (SL) TMDC, WS2, can be transferred onto high-κ transition metal oxide substrates TiO2 and SrTiO3. The resulting samples are much more suitable for measuring their electronic and chemical structures with angle-resolved photoemission than their native-grown SiO2 substrates. We probe the WS2 on the micron scale across 100 μm flakes and find that the occupied electronic structure is exactly as predicted for free-standing SL WS2 with a strong spin-orbit splitting of 420 meV and a direct band gap at the valence band maximum. Our results suggest that TMDCs can be combined with arbitrary multifunctional oxides, which may introduce alternative means of controlling the optoelectronic properties of such materials.

Giant spin-splitting and gap renormalization driven by trions in single-layer WS2/h-BN heterostructures

In two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs), new electronic phenomena such as tunable bandgaps1–3 and strongly bound excitons and trions emerge from strong many-body effects4–6, beyond the spin and valley degrees of freedom induced by spin–orbit coupling and by lattice symmetry7. Combining single-layer TMDs with other 2D materials in van der Waals heterostructures offers an intriguing means of controlling the electronic properties through these many-body effects, by means of engineered interlayer interactions8–10. Here, we use micro-focused angle-resolved photoemission spectroscopy (microARPES) and in situ surface doping to manipulate the electronic structure of single-layer WS2 on hexagonal boron nitride (WS2/h-BN). Upon electron doping, we observe an unexpected giant renormalization of the spin–orbit splitting of the single-layer WS2 valence band, from 430 meV to 660 meV, together with a bandgap reduction of at least 325 meV, attributed to the formation of trionic quasiparticles. These findings suggest that the electronic, spintronic and excitonic properties are widely tunable in 2D TMD/h-BN heterostructures, as these are intimately linked to the quasiparticle dynamics of the materials11–13.A microfocused angle-resolved photoemission spectroscopy study of single layers of WS2 on hexagonal boron nitride reveals that, upon electron doping, trionic interactions cause a giant increase of the spin splitting in the valence band.

Spin inversion in graphene spin valves by gate-tunable magnetic proximity effect at one-dimensional contacts

Graphene has remarkable opportunities for spintronics due to its high mobility and long spin diffusion length, especially when encapsulated in hexagonal boron nitride (h-BN). Here, we demonstrate gate-tunable spin transport in such encapsulated graphene-based spin valves with one-dimensional (1D) ferromagnetic edge contacts. An electrostatic backgate tunes the Fermi level of graphene to probe different energy levels of the spin-polarized density of states (DOS) of the 1D ferromagnetic contact, which interact through a magnetic proximity effect (MPE) that induces ferromagnetism in graphene. In contrast to conventional spin valves, where switching between high- and low-resistance configuration requires magnetization reversal by an applied magnetic field or a high-density spin-polarized current, we provide an alternative path with the gate-controlled spin inversion in graphene.Owing to its long spin diffusion length, graphene shows promise for spintronics applications, especially when encapsulated within hexagonal boron nitride. Here, the authors demonstrate gate-tunable spin transport in encapsulated graphene-based spin valves with one-dimensional ferromagnetic edge contacts via magnetic proximity effect.

Uniform large-area growth of nanotemplated high-quality monolayer MoS2

Over the past decade, it has become apparent that the extreme sensitivity of 2D crystals to surface interactions presents a unique opportunity to tune material properties through surface functionalization and the mechanical assembly of 2D heterostructures. However, this opportunity carries with it a concurrent challenge: an enhanced sensitivity to surface contamination introduced by standard patterning techniques that is exacerbated by the difficulty in cleaning these atomically thin materials. Here, we report a templated MoS2 growth technique wherein Mo is deposited onto atomically stepped sapphire substrates through a SiN stencil with feature sizes down to 100 nm and subsequently sulfurized at high temperature. These films have a quality comparable to the best MoS2 prepared by other methodologies, and the thickness of the resulting MoS2 patterns can be tuned layer-by-layer by controlling the initial Mo deposition. The quality and thickness of the films are confirmed by scanning electron, scanning tunnel...