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Register a new userPhase Transition in a Memristive Suspended MoS2 Monolayer Probed by Opto- and Electro-Mechanics
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Semiconducting monolayer of 2D material are able to concatenate multiple interesting properties into a single component. Here, by combining opto-mechanical and electronic measurements, we demonstrate the presence of a partial 2H-1T phase transition in a suspended 2D monolayer membrane of MoS2. Electronic transport shows unexpected memristive properties in the MoS2 membrane, in the absence of any external dopants. A strong mechanical softening of the membrane is measured concurrently and may only be related to the phase 2H-1T phase transition which imposes a 3percent directional elongation of the topological 1T phase with respect to the semiconducting 2H. We note that only a few percent 2H- 1T phase switching is sufficient to observe measurable memristive effects. Our experimental results combined with First-principles total energy calculations indicate that sulfur vacancy diffusion plays a key role in the initial nucleation of the phase transition. Our study clearly shows that nanomechanics represents an ultrasensitive technique to probe the crystal phase transition in 2D materials or thin membranes. Finally, a better control of the microscopic mechanisms responsible for the observed memristive effect in MoS2 is important for the implementation of future devices.
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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.
Transitions metal dichalcogenides (TMDs) are direct semiconductors in the atomic monolayer (ML) limit with fascinating optical and spin-valley properties. The strong optical absorption of up to 20 % for a single ML is governed by excitons, electron-hole pairs bound by Coulomb attraction. Excited exciton states in MoSe$_2$ and MoTe$_2$ monolayers have so far been elusive due to their low oscillator strength and strong inhomogeneous broadening. Here we show that encapsulation in hexagonal boron nitride results in emission line width of the A:1$s$ exciton below 1.5 meV and 3 meV in our MoSe$_2$ and MoTe$_2$ monolayer samples, respectively. This allows us to investigate the excited exciton states by photoluminescence upconversion spectroscopy for both monolayer materials. The excitation laser is tuned into resonance with the A:1$s$ transition and we observe emission of excited exciton states up to 200 meV above the laser energy. We demonstrate bias control of the efficiency of this non-linear optical process. At the origin of upconversion our model calculations suggest an exciton-exciton (Auger) scattering mechanism specific to TMD MLs involving an excited conduction band thus generating high energy excitons with small wave-vectors. The optical transitions are further investigated by white light reflectivity, photoluminescence excitation and resonant Raman scattering confirming their origin as excited excitonic states in monolayer thin semiconductors.
Two-dimensional semiconductors such as MoS2 are an emerging material family with wide-ranging potential applications in electronics, optoelectronics and energy harvesting. Large-area growth methods are needed to open the way to the applications. While significant progress to this goal was made, control over lattice orientation during growth still remains a challenge. This is needed in order to minimize or even avoid the formation of grain boundaries which can be detrimental to electrical, optical and mechanical properties of MoS2 and other 2D semiconductors. Here, we report on the uniform growth of high-quality centimeter-scale continuous monolayer MoS2 with control over lattice orientation. Using transmission electron microscopy we show that the monolayer film is composed of coalescing single islands that share a predominant lattice orientation due to an epitaxial growth mechanism. Raman and photoluminescence spectra confirm the high quality of the grown material. Optical absorbance spectra acquired over large areas show new features in the high-energy part of the spectrum, indicating that MoS2 could also be interesting for harvesting this region of the solar spectrum and fabrication of UV-sensitive photodetectors. Even though the interaction between the growth substrate and MoS2 is strong enough to induce lattice alignment, we can easily transfer the grown material and fabricate field-effect transistors on SiO2 substrates showing mobility superior to the exfoliated material.
The (r3xr3)R30{deg} honeycomb of silicene monolayer on Ag(111) was found to undergo a phase transition to two types of mirror-symmetric boundary-separated rhombic phases at temperatures below 40 K by scanning tunneling microscopy. The first-principles calculations reveal that weak interactions between silicene and Ag(111) drive the spontaneous ultra buckling in the monolayer silicene, forming two energy-degenerate and mirror-symmetric (r3xr3)R30{deg} rhombic phases, in which the linear band dispersion near Dirac point (DP) and a significant gap opening (150 meV) at DP were induced. The low transition barrier between these two phases enables them interchangeable through dynamic flip-flop motion, resulting in the (r3xr3)R30{deg} honeycomb structure observed at high temperature.
Interactions between two excitons can result in the formation of bound quasiparticles, known as biexcitons. Their properties are determined by the constituent excitons, with orbital and spin states resembling those of atoms. Monolayer transition metal dichalcogenides (TMDs) present a unique system where excitons acquire a new degree of freedom, the valley pseudospin, from which a novel intervalley biexciton can be created. These biexcitons comprise two excitons from different valleys, which are distinct from biexcitons in conventional semiconductors and have no direct analogue in atomic and molecular systems. However, their valley properties are not accessible to traditional transport and optical measurements. Here, we report the observation of intervalley biexcitons in the monolayer TMD MoS2 using ultrafast pump-probe spectroscopy. By applying broadband probe pulses with different helicities, we identify two species of intervalley biexcitons with large binding energies of 60 meV and 40 meV. In addition, we also reveal effects beyond biexcitonic pairwise interactions in which the exciton energy redshifts at increasing exciton densities, indicating the presence of many-body interactions among them.
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