Tommaso Venanzi, Malte Selig, Alexej Pashkin, Stephan Winnerl, Manuel Katzer, Himani Arora, Artur Erbe, Amalia Patanè, Zakhar R. Kudrynskyi, Zakhar D. Kovalyuk, Leonetta Baldassarre, Andreas Knorr, Manfred Helm, Harald Schneider 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.
We demonstrate that spin-orbit coupling (SOC) strength for electrons near the conduction band edge in few-layer $\gamma$-InSe films can be tuned over a wide range. This tunability is the result of a competition between film-thickness-dependent intrinsic and electric-field-induced SOC, potentially, allowing for electrically switchable spintronic devices. Using a hybrid $\mathbf{k\cdot p}$ tight-binding model, fully parameterized with the help of density functional theory computations, we quantify SOC strength for various geometries of InSe-based field-effect transistors. The theoretically computed SOC strengths are compared with the results of weak antilocalization measurements on dual-gated multilayer InSe films, interpreted in terms of Dyakonov-Perel spin relaxation due to SOC, showing a good agreement between theory and experiment.
M. Osiekowicz, D. Staszczuk, K. Olkowska-Pucko, Ł. Kipczak, M. Grzeszczyk, M. Zinkiewicz, K. Nogajewski, Z. R. Kudrynskyi, Z. D. Kovalyuk, A. Patané, A. Babiński, M. R. Molas The temperature effect on the Raman scattering efficiency is investigated in $\varepsilon$-GaSe and $\gamma$-InSe crystals. We found that varying the temperature over a broad range from 5 K to 350 K permits to achieve both the resonant conditions and the antiresonance behaviour in Raman scattering of the studied materials. The resonant conditions of Raman scattering are observed at about 270 K under the 1.96 eV excitation for GaSe due to the energy proximity of the optical band gap. In the case of InSe, the resonant Raman spectra are apparent at about 50 K and 270 K under correspondingly the 2.41 eV and 2.54 eV excitations as a result of the energy proximity of the \mboxso-called B transition. Interestingly, the observed resonances for both materials are followed by an antiresonance behaviour noticeable at higher temperatures than the detected resonances. The significant variations of phonon-modes intensities can be explained in terms of electron-phonon coupling and quantum interference of contributions from different points of the Brillouin zone
Tommaso Venanzi, Himani Arora, Stephan Winnerl, Alexej Pashkin, Phanish Chava, Amalia Patanè, Zakhar D. Kovalyuk, Zalhar R. Kudrynskyi, Kenji Watanabe, Takashi Taniguchi, Artur Erbe, Manfred Helm, Harald Schneider 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.
Nicolas Ubrig, Evgeniy Ponomarev, Johanna Zultak, Daniil Domaretskiy, Viktor Zólyomi, Daniel Terry, James Howarth, Ignacio Gutiérrez-Lezama, Alexander Zhukov, Zakhar R. Kudrynskyi, Zakhar D. Kovalyuk, Amalia Patanè, Takashi Taniguchi, Kenji Watanabe, Roman V. Gorbachev, Vladimir I. Fal'ko, Alberto F. Morpurgo 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.
Vishnu Sreepal, Mehmet Yagmurcukardes, Kalangi S. Vasu, Daniel J. Kelly, Sarah F. R. Taylor, Vasyl G. Kravets, Zakhar Kudrynskyi, Zakhar D. Kovalyuk, Amalia Patanè, Alexander N. Grigorenko, Sarah J. Haigh, Christopher Hardacre, Laurence Eaves, Hasan Sahin, Andre K. Geim, Francois M. Peeters, Rahul R. Nair 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.
Yongjin Lee, Riccardo Pisoni, Hiske Overweg, Marius Eich, Peter Rickhaus, Amalia Patanè, Zakhar R. Kudrynskyi, Zakhar. D. Kovalyuk, Roman Gorbachev, Kenji Watanabe, Takashi Taniguchi, Thomas Ihn, Klaus Ensslin 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.
Matthew Hamer, Endre Tóvári, Mengjian Zhu, Michael D. Thompson, Alexander Mayorov, Jonathon Prance, Yongjin Lee, Richard P. Haley, Zakhar R. Kudrynskyi, Amalia Patanè, Daniel Terry, Zakhar D. Kovalyuk, Klaus Ensslin, Andrey V. Kretinin, Andre Geim, Roman Gorbachev 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.
Complex electron-microscopic, energy-dispersed and wide-temperature optical absorption and photoluminescence (PL) investigations are carried out into Bridgeman-grown layered In2Se3 crystals. It is shown that In2Se3 crystals as a whole have a homogeneous concentration of In and Se atoms, corresponding with In2Se3 stoichiometry. Nevertheless, In2Se3 crystals contain a significant amount of dislocations, on which nano-sized interspersions of crystal phases of pure InSe, In6Se7 and monoclinic red Se settle down. Optical wide-temperature investigations of In2Se3 allow us to do the following: establish the width of the band-gap, the exciton binding energy; determine the frequency of a half-layer A-phonon, which takes part in electron (exciton)-phonon interaction; and to evaluate the effective masses of carriers and the dielectric permeability. Finally, blue shift of the band-gap and character of the electron (exciton)-phonon interaction of nano-sized 3D InSe crystals confined in an In2Se3 crystal matrix; influence of an InSe nanocrystal radius and of an ensemble of 3D InSe nanocrystals with different radii for an increase of the exciton emission/absorption half-width line with temperature and radii of InSe nanocrystals are discussed.
D. A. Bandurin, A. V. Tyurnina, G. L. Yu, A. Mishchenko, V. Zolyomi, S. V. Morozov, R. Krishna Kumar, R. V. Gorbachev, Z. R. Kudrynskyi, S. Pezzini, Z. D. Kovalyuk, U. Zeitler, K. S. Novoselov, A. Patane, L. Eaves, I. V. Grigorieva, V. I. Fal'ko, A. K. Geim, Y. Cao A decade of intense research on two-dimensional (2D) atomic crystals has revealed that their properties can differ greatly from those of the parent compound. These differences are governed by changes in the band structure due to quantum confinement and are most profound if the underlying lattice symmetry changes. Here we report a high-quality 2D electron gas in few-layer InSe encapsulated in hexagonal boron nitride under an inert atmosphere. Carrier mobilities are found to exceed 1,000 and 10,000 cm2/Vs at room and liquid-helium temperatures, respectively, allowing the observation of the fully-developed quantum Hall effect. The conduction electrons occupy a single 2D subband and have a small effective mass. Photoluminescence spectroscopy reveals that the bandgap increases by more than 0.5 eV with decreasing the thickness from bulk to bilayer InSe. The band-edge optical response vanishes in monolayer InSe, which is attributed to monolayer's mirror-plane symmetry. Encapsulated 2D InSe expands the family of graphene-like semiconductors and, in terms of quality, is competitive with atomically-thin dichalcogenides and black phosphorus.