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Two-dimensional crystals stack together through weak van der Waals (vdW) forces, offering unlimited possibilities to play with layer number, order and twist angle in vdW heterostructures (HSs). The realisation of high-performance optoelectronic devices, however, requires the achievement of specific band alignments, $k$-space matching between conduction band minima and valence band maxima, as well as efficient charge transfer between the constituent layers. Fine tuning mechanisms to design ideal HSs are lacking. Here, we show that layer-selective strain engineering can be exploited as an extra degree of freedom in vdW HSs to tailor their band alignment and optical properties. To that end, strain is selectively applied to MS$_2$ (M=Mo,W) monolayers in InSe/MS$_2$ HSs. This triggers a giant PL enhancement of the highly tuneable but weakly emitting InSe by one to three orders of magnitude. Resonant PL excitation measurements, supported by first-principle calculations, provide evidence of a strain-activated direct charge transfer from the MS$_2$ MLs toward InSe. This significant emission enhancement achieved for InSe widens its range of applications for optoelectronics.

The quantum Hall effect is widely used for the investigation of fundamental phenomena, ranging from topological phases to composite fermions. In particular, the discovery of a room temperature resistance quantum in graphene is significant for compact resistance standards that can operate above cryogenic temperatures. However, this requires large magnetic fields that are accessible only in a few high magnetic field facilities. Here, we report on the quantum Hall effect in graphene encapsulated by the ferroelectric insulator CuInP2S6. Electrostatic gating of the graphene channel enables the Fermi energy to be tuned so that electrons in the localized states of the insulator are in equilibrium with the current-carrying, delocalized states of graphene. Due to the presence of strongly bound states in this hybrid system, a quantum Hall plateau can be achieved at room temperature in relatively modest magnetic fields. This phenomenon offers the prospect for the controlled manipulation of the quantum Hall effect at room temperature., Comment: 24 pages, 6 figures

A promising route for the development of opto-elelctronic technology is to use terahertz radiation to modulate the optical properties of semiconductors. Here we demonstrate the dynamical control of photoluminescence (PL) emission in few-layer InSe using picosecond terahertz pulses. We observe a strong PL quenching (up to 50%) after the arrival of the terahertz pulse followed by a reversible recovery of the emission on the time scale of 50ps at T =10K. Microscopic calculations reveal that the origin of the photoluminescence quenching is the terahertz absorption by photo-excited carriers: this leads to a heating of the carriers and a broadening of their distribution, which reduces the probability of bimolecular electron-hole recombination and, therefore, the luminescence. By numerically evaluating the Boltzmann equation, we are able to clarify the individual roles of optical and acoustic phonons in the subsequent cooling process. The same PL quenchingmechanismis expected in other van derWaals semiconductors and the effectwill be particularly strong for materials with low carrier masses and long carrier relaxation time, which is the case for InSe. This work gives a solid background for the development of opto-electronic applications based on InSe, such as THz detectors and optical modulators., Comment: The following article has been accepted by Applied Physics Letters. After it is published, it will be found at https://publishing.aip.org/resources/librarians/products/journals/

Pristine graphene and graphene-based heterostructures exhibit exceptionally high electron mobility and conductance if their surface contains few electron-scattering impurities. Here, we reveal a universal connection between graphene's carrier mobility and the variation of its electrical conductance with carrier density. Our model of graphene conductivity is based on a convolution of carrier density and its uncertainty, which reproduces the observed universality. Taking a single conductance measurement as input, this model accurately predicts the full shape of the conductance versus carrier density curves for a wide range of reported graphene samples. We verify the convolution model by numerically solving the Boltzmann transport equation to analyse in detail the effects of charged impurity scattering on carrier mobility. In this model, we also include optical phonons, which relax high-energy charge carriers for small impurity densities. Our numerical and analytical results both capture the universality observed in experiment and provide a way to estimate all key transport parameters of graphene devices. Our results demonstrate how the carrier mobility can be predicted and controlled, thereby providing insights for engineering the properties of 2D materials and heterostructures., Comment: 20 pages, 4 figures

The two-dimensional (2D) semiconductor indium selenide (InSe) has attracted significant interest due its unique electronic band structure, high electron mobility and wide tunability of its band gap energy achieved by varying the layer thickness. All these features make 2D InSe a potential candidate for advanced electronic and optoelectronic applications. Here, we report on the discovery of new polymorphs of InSe with enhanced electronic properties. Using a global structure search that combines artificial swarm intelligence with first-principles energetic calculations, we identify polymorphs that consist of a centrosymmetric monolayer belonging to the point group D$_{3d}$, distinct from the well-known polymorphs based on the D$_{3h}$ monolayers that lack inversion symmetry. The new polymorphs are thermodynamically and kinetically stable, and exhibit a wider optical spectral response and larger electron mobilities compared to the known polymorphs. We discuss opportunities to synthesize these newly discovered polymorphs and viable routes to identify them by X-ray diffraction, Raman spectroscopy and second harmonic generation experiments., Comment: 20 pages, 5 figures

We study the optical properties of thin flakes of InSe encapsulated in hBN. More specifically, we investigate the photoluminescence (PL) emission and its dependence on sample thickness and temperature. Through the analysis of the PL lineshape, we discuss the relative weights of the exciton and electron-hole contributions. Thereafter we investigate the PL dynamics. Two contributions are distinguishable at low temperature: direct bandgap electron-hole and defect-assisted recombination. The two recombination processes have lifetime of $\tau_1 \sim 8\;$ns and $\tau_2 \sim 100\;$ns, respectively. The relative weights of the direct bandgap and defect-assisted contributions show a strong layer dependence due to the direct-to-indirect bandgap crossover. Electron-hole PL lifetime is limited by population transfer to lower-energy states and no dependence on the number of layers was observed. The lifetime of the defect-assisted recombination gets longer for thinner samples. Finally, we show that the PL lifetime decreases at high temperatures as a consequence of more efficient non-radiative recombinations., Comment: The manuscript will be published in the journal Physical Review Materials. Copyright 2011 by American Physical Society (https://journals.aps.org/prmaterials/)

Atomically thin layers of van der Waals (vdW) crystals offer an ideal material platform to realize tunnel field effect transistors (TFETs) that exploit the tunneling of charge carriers across the forbidden gap of a vdW heterojunction. This type of device requires a precise energy band alignment of the different layers of the junction to optimize the tunnel current. Amongst two-dimensional (2D) vdW materials, black phosphorus (BP) and indium selenide (InSe) have a Brillouin zone-centered conduction and valence bands, and a type II band offset, both ideally suited for band-to-band tunneling. Here, we demonstrate TFETs based on BP/InSe heterojunctions with diverse electrical transport characteristics: forward rectifying, Zener-tunneling and backward rectifying characteristics are realized in BP/InSe junctions with different thickness of the BP layer or by electrostatic gating of the junction. Electrostatic gating yields a large on/off current ratio of up to 108 and negative differential resistance at low applied voltages (V ~ 0.2V). These findings illustrate versatile functionalities of TFETs based on BP and InSe, offering opportunities for applications of these 2D materials beyond the device architectures reported in the current literature.

Van der Waals (vdW) materials offer new ways to assemble artificial electronic media with properties controlled at the design stage, by combining atomically defined layers into interfaces and heterostructures. Their potential for optoelectronics stems from the possibility to tailor the spectral response over a broad range by exploiting interlayer transitions between different compounds with an appropriate band-edge alignment. For the interlayer transitions to be radiative, however, a serious challenge comes from details of the materials --such as lattice mismatch or even a small misalignment of the constituent layers-- that can drastically suppress the electron-photon coupling. The problem was evidenced in recent studies of heterostructures of monolayer transition metal dichalcogenides, whose band edges are located at the K-point of reciprocal space. Here we demonstrate experimentally that the solution to the interlayer coupling problem is to engineer type-II interfaces by assembling atomically thin crystals that have the bottom of the conduction band and the top of the valence band at the $\Gamma$-point, thus avoiding any momentum mismatch. We find that this type of vdW interfaces exhibits radiative optical transition irrespective of lattice constant, rotational/translational alignment of the two layers, or whether the constituent materials are direct or indirect gap semiconductors. The result, which is robust and of general validity, drastically broadens the scope of future optoelectronics device applications based on 2D materials.

We exploit hyperfine interactions in a single Mn-ion confined in a quantum dot (QD) to create a qudit, i.e. a multi-level quantum-bit system, with well defined, addressable and robust set of spin states for the realization of universal quantum gates. We generate and probe an arbitrary superposition of states between selected hyperfine energy level pairs by using electron double resonance detected nuclear magnetic resonance (EDNMR). This enables the observation of Rabi oscillations and the experimental realization of NOT and SWAP universal quantum gates that are robust against decoherence. Our protocol for cyclical preparation, manipulation and read-out of logic gates offers opportunities for integration of qudits in scalable quantum circuit architectures beyond solid state electron spin qubits.

Most of the studied two-dimensional (2D) materials have been obtained by exfoliation of van der Waals crystals. Recently, there has been growing interest in fabricating synthetic 2D crystals which have no layered bulk analogues. These efforts have been focused mainly on the surface growth of molecules in high vacuum. Here, we report an approach to making 2D crystals of covalent solids by chemical conversion of van der Waals layers. As an example, we use 2D indium selenide (InSe) obtained by exfoliation and converted it by direct fluorination into indium fluoride (InF3), which has a non-layered, rhombohedral structure and therefore cannot be possibly obtained by exfoliation. The conversion of InSe into InF3 is found to be feasible for thicknesses down to three layers of InSe, and the obtained stable InF3 layers are doped with selenium. We study this new 2D material by optical, electron transport and Raman measurements and show that it is a semiconductor with a direct bandgap of 2.2 eV, exhibiting high optical transparency across the visible and infrared spectral ranges. We also demonstrate the scalability of our approach by chemical conversion of large-area, thin InSe laminates obtained by liquid exfoliation into InF3 films. The concept of chemical conversion of cleavable thin van der Waals crystals into covalently-bonded non-cleavable ones opens exciting prospects for synthesizing a wide variety of novel atomically thin covalent crystals.

In the last six years, Indium selenide (InSe) has appeared as a new van der Waals heterostructure platform which has been extensively studied due to its unique electronic and optical properties. Such as transition metal dichalcogenides (TMDCs), the considerable bandgap and high electron mobility can provide a potential optoelectronic application. Here we present low-temperature transport measurements on a few-layer InSe van der Waals heterostructure with graphene-gated contacts. For high magnetic fields, we observe magnetoresistance minima at even filling factors related to two-fold spin degeneracy. By electrostatic gating with negatively biased split gates, a one-dimensional channel is realized. Close to pinch-off, transport through the constriction is dominated by localized states with charging energies ranging from 2 to 5 meV. This work opens new possibility to explore the low-dimensional physics including quantum point contact and quantum dot., Comment: 11 pages, 4 figures

Indium selenide, a post-transition metal chalcogenide, is a novel two-dimensional (2D) semiconductor with interesting electronic properties. Its tunable band gap and high electron mobility have already attracted considerable research interest. Here we demonstrate strong quantum confinement and manipulation of single electrons in devices made from few-layer crystals of InSe using electrostatic gating. We report on gate-controlled quantum dots in the Coulomb blockade regime as well as one-dimensional quantization in point contacts, revealing multiple plateaus. The work represents an important milestone in the development of quality devices based on 2D materials and makes InSe a prime candidate for relevant electronic and optoelectronic applications., Comment: 13 pages, 3 figures

The integration of different two-dimensional materials within a multilayer van der Waals (vdW) heterostructure offers a promising technology for realizing high performance opto-electronic devices such as photodetectors and light sources1-3. Transition metal dichalcogenides, e.g. MoS2 and WSe2, have been employed as the optically-active layer in recently developed heterojunctions. However, MoS2 and WSe2 become direct band gap semiconductors only in mono- or bilayer form4,5. In contrast, the metal monochalcogenides InSe and GaSe retain a direct bandgap over a wide range of layer thicknesses from bulk crystals down to exfoliated flakes only a few atomic monolayers thick6,7. Here we report on vdW heterojunction diodes based on InSe and GaSe: the type II band alignment between the two materials and their distinctive spectral response, combined with the low electrical resistance of transparent graphene electrodes, enable effective separation and extraction of photoexcited carriers from the heterostructure even when no external voltage is applied. Our devices are fast (< 10 {\mu}s), self-driven photodetectors with multicolor photoresponse ranging from the ultraviolet to the near-infrared and have the potential to accelerate the exploitation of two-dimensional vdW crystals by creating new routes to miniaturized optoelectronics beyond present technologies.