Physical Review B

Associate DIETRICH BELITZ, University of Oregon Editors: Condensed Matter Physics (Theoretical) J. IGNACIO CIRAC, Max-Planck-Institut für Quantenoptik Quantum Information RAYMOND E. GOLDSTEIN, University of Cambridge Biological Physics ARTHUR F. HEBARD, University of Florida Condensed Matter Physics (Experimental) RANDALL D. KAMIEN, University of Pennsylvania Soft Condensed Matter DANIEL KLEPPNER, Massachusetts Institute of Technology Atomic, Molecular, and Optical Physics (Experimental) PAUL G. LANGACKER, Institute for Advanced Study, Princeton University Particle Physics (Theoretical) VERA LÜTH, Stanford University Particle Physics (Experimental) DAVID D. MEYERHOFER, University of Rochester Physics of Plasmas and Matter at High-Energy Density WITOLD NAZAREWICZ, University of Tennessee, Oak Ridge National Laboratory Nuclear Physics JOHN H. SCHWARZ, California Institute of Technology Mathematical Physics FRIEDRICH-KARL THIELEMANN, Universität Basel Astrophysics Senior Assistant Editor: DEBBIE BRODBAR, APS Editorial Office American Physical Society

Reviews of Modern Physics

Two-dimensional (2D) materials have attracted a great deal of interest in recent years. This family of materials allows for the realization of versatile electronic devices and holds promise for next-generation (opto)electronics. Their electronic properties strongly depend on the number of layers, making them interesting from a fundamental standpoint. For electronic applications, semiconducting 2D materials benefit from sizable mobilities and large on/off ratios, due to the large modulation achievable via the gate field-effect. Moreover, being mechanically strong and flexible, these materials can withstand large strain (>10%) before rupture, making them interesting for strain engineering and flexible devices. Even in their single layer form, semiconducting 2D materials have demonstrated efficient light absorption, enabling large responsivity in photodetectors. Therefore, semiconducting layered 2D materials are strong candidates for optoelectronic applications, especially for photodetection. Here, we review the state-of-the-art in photodetectors based on semiconducting 2D materials, focusing on the transition metal dichalcogenides, novel van der Waals materials, black phosphorus, and heterostructures.

Photocurrent generation with two-dimensional van der Waals semiconductors.

The excellent catalytic activity of metallic MoS2 edges for the hydrogen evolution reaction (HER) has led to substantial efforts towards increasing the edge concentration. The 2H basal plane is less active for the HER because it is less conducting and therefore possesses less efficient charge transfer kinetics. Here we show that the activity of the 2H basal planes of monolayer MoS2 nanosheets can be made comparable to state-of-the-art catalytic properties of metallic edges and the 1T phase by improving the electrical coupling between the substrate and the catalyst so that electron injection from the electrode and transport to the catalyst active site is facilitated. Phase-engineered low-resistance contacts on monolayer 2H-phase MoS2 basal plane lead to higher efficiency of charge injection in the nanosheets so that its intrinsic activity towards the HER can be measured. We demonstrate that onset potentials and Tafel slopes of ∼-0.1 V and ∼50 mV per decade can be achieved from 2H-phase catalysts where only the basal plane is exposed. We show that efficient charge injection and the presence of naturally occurring sulfur vacancies are responsible for the observed increase in catalytic activity of the 2H basal plane. Our results provide new insights into the role of contact resistance and charge transport on the performance of two-dimensional MoS2 nanosheet catalysts for the HER.

The role of electronic coupling between substrate and 2D MoS2 nanosheets in electrocatalytic production of hydrogen.

Electrical metal contacts to two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDCs) are found to be the key bottleneck to the realization of high device performance due to strong Fermi level pinning and high contact resistances (Rc). Until now, Fermi level pinning of monolayer TMDCs has been reported only theoretically, although that of bulk TMDCs has been reported experimentally. Here, we report the experimental study on Fermi level pinning of monolayer MoS2 and MoTe2 by interpreting the thermionic emission results. We also quantitatively compared our results with the theoretical simulation results of the monolayer structure as well as the experimental results of the bulk structure. We measured the pinning factor S to be 0.11 and −0.07 for monolayer MoS2 and MoTe2, respectively, suggesting a much stronger Fermi level pinning effect, a Schottky barrier height (SBH) lower than that by theoretical prediction, and interestingly similar pinning energy levels between monolayer and bulk Mo...

Fermi Level Pinning at Electrical Metal Contacts of Monolayer Molybdenum Dichalcogenides.

The search of a p-type metal contact on MoS2 has remained inconclusive, with high work function metals such as Au, Ni, and Pt showing n-type behavior and mixed reports of n as well as p-type behavior for Pd. In this work, we report quantitative Schottky barrier heights for Au and Pd contacts to MoS2 obtained by analysing low temperature transistor characteristics and contact resistance data obtained using the transfer length method. Both Au and Pd exhibit n-type behavior on multilayer as well as monolayer MoS2 transistors with Schottky barrier heights of 0.126 eV and 0.4 eV, and contact resistances of 42 Ω.mm and 18 × 104 Ω.mm respectively. Scanning photocurrent spectroscopy data is in agreement with the resulting energy band alignment in Au-MoS2-Pd devices further reinforcing the observation that the Fermi-level is pinned in the upper half of MoS2 bandgap.

Schottky barrier heights for Au and Pd contacts to MoS2

Although photons in free space barely interact, matter can mediate interactions between them resulting in optical nonlinearities. Such interactions at the single-quantum level result in an on-site photon repulsion, crucial for photon-based quantum information processing and for realizing strongly interacting many-body states of light. Here, we report repulsive dipole–dipole interactions between electric field-tuneable, localized interlayer excitons in the MoSe2/WSe2 heterobilayer. The presence of a single, localized exciton with an out-of-plane, non-oscillating dipole moment increases the energy of the second excitation by ~2 meV—an order of magnitude larger than the emission linewidth and corresponding to an inter-dipole distance of ~7 nm. At higher excitation power, multi-exciton complexes appear at systematically higher energies. The magnetic field dependence of the emission polarization is consistent with the spin-valley singlet nature of the dipolar molecular state. Our finding represents a step towards the creation of excitonic few- and many-body states such as dipolar crystals with spin-valley spinor in van der Waals heterostructures. Repulsive dipole–dipole interactions between localized interlayer excitons are shown to modify the optical response of van der Waals heterobilayers, forming the basis to obtain strong optical nonlinearity and excitonic many-body states in two-dimensional materials.

Dipolar interactions between localized interlayer excitons in van der Waals heterostructures

We demonstrate a simple technique to transfer chemical vapour deposited (CVD) graphene from copper and platinum substrates using a soak-and-peel delamination technique utilizing only hot deionized water. The lack of chemical etchants results in cleaner CVD graphene films minimizing unintentional doping, as confirmed by Raman and electrical measurements. The process allows the reuse of substrates and hence can enable the use of oriented substrates for growth of higher quality graphene, and is an inherently inexpensive and scalable process for large-area production.

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A facile process for soak-and-peel delamination of CVD graphene from substrates using water.

Quantum entanglement is a fundamental phenomenon that, on the one hand, reveals deep connections between quantum mechanics, gravity and spacetime1,2, and on the other hand, has practical applications as a key resource in quantum information processing3. Although it is routinely achieved in photon–atom ensembles4, entanglement involving solid-state5–7 or macroscopic objects8 remains challenging albeit promising for both fundamental physics and technological applications. Here, we report entanglement between collective, chiral vibrations in a two-dimensional WSe2 host—chiral phonons (CPs)—and single-photons emitted from quantum dots9–13 (QDs) present in it. CPs that carry angular momentum were recently observed in WSe2 and are a distinguishing feature of the underlying honeycomb lattice14,15. The entanglement results from a ‘which-way’ scattering process, involving an optical excitation in a QD and doubly-degenerate CPs, which takes place via two indistinguishable paths. Our unveiling of entanglement involving a macroscopic, collective excitation together with strong interactions between CPs and QDs in two-dimensional materials opens up ways for phonon-driven entanglement of QDs and engineering chiral or non-reciprocal interactions at the single-photon level. A ‘which-way’ scattering process can generate entanglement between single photons and collective chiral vibrations in two-dimensional tungsten diselenide. The result opens up ways for engineering non-reciprocal interactions at the quantum level.

Entanglement of single-photons and chiral phonons in atomically thin WSe 2

Superlattice in graphene generates extra Dirac points in the band structure and their number depends on the superlattice potential strength. Here, we have created a lateral superlattice in a graphene device with a tunable barrier height using a combination of two gates. In this Letter, we demonstrate the use of lateral superlattice to modify the band structure of graphene leading to the emergence of new Dirac cones. This controlled modification of the band structure persists up to 100 K.

Sudipta Dubey

Papers

Schottky barrier heights for Au and Pd contacts to MoS2

Dipolar interactions between localized interlayer excitons in van der Waals heterostructures

A facile process for soak-and-peel delamination of CVD graphene from substrates using water.

Entanglement of single-photons and chiral phonons in atomically thin WSe 2

Tunable Superlattice in Graphene To Control the Number of Dirac Points