A two-dimensional honeycomb lattice harbours a pair of inequivalent valleys in the k-space electronic structure, in the vicinities of the vertices of a hexagonal Brillouin zone, K±. It is particularly appealing to exploit this emergent degree of freedom of charge carriers, in what is termed 'valleytronics'. The physics of valleys mimics that of spin, and will make possible devices, analogous to spintronics, such as valley filter and valve, and optoelectronic Hall devices, all very promising for next-generation electronics. The key challenge lies with achieving valley polarization, of which a convincing demonstration in a two-dimensional honeycomb structure remains evasive. Here we show, using first principles calculations, that monolayer molybdenum disulphide is an ideal material for valleytronics, for which valley polarization is achievable via valley-selective circular dichroism arising from its unique symmetry. We also provide experimental evidence by measuring the circularly polarized photoluminescence on monolayer molybdenum disulphide, which shows up to 50% polarization.
Molybdenum disulfide (MoS2) is back in the spotlight because of the indirect-to-direct bandgap tunability and valley related physics emerging in the monolayer regime. However, rigorous control of the monolayer thickness is still a huge challenge for commonly utilized physical exfoliation and chemical synthesis methods. Herein, we have successfully grown predominantly monolayer MoS2 on an inert and nearly lattice-matching mica substrate by using a low-pressure chemical vapor deposition method. The growth is proposed to be mediated by an epitaxial mechanism, and the epitaxial monolayer MoS2 is intrinsically strained on mica due to a small adlayer-substrate lattice mismatch (~2.7%). Photoluminescence (PL) measurements indicate strong single-exciton emission in as-grown MoS2 and room-temperature PL helicity (circular polarization ~0.35) on transferred samples, providing straightforward proof of the high quality of the prepared monolayer crystals. The homogeneously strained high-quality monolayer MoS2 prepared in this study could competitively be exploited for a variety of future applications.
Diamond-anvil-cell and shock-wave technologies now permit the study of matter under multimegabar pressure (that is, of several hundred GPa). The properties of matter in this pressure regime differ drastically from those known at 1 atm (about 10(5) Pa). Just how different chemistry is at high pressure and what role chemical intuition for bonding and structure can have in understanding matter at high pressure will be explored in this account. We will discuss in detail an overlapping hierarchy of responses to increased density: a) squeezing out van der Waals space (for molecular crystals); b) increasing coordination; c) decreasing the length of covalent bonds and the size of anions; and d) in an extreme regime, moving electrons off atoms and generating new modes of correlation. Examples of the startling chemistry and physics that emerge under such extreme conditions will alternate in this account with qualitative chemical ideas about the bonding involved.
Conventional electronics are based invariably on the intrinsic degrees of freedom of an electron, namely its charge and spin. The exploration of novel electronic degrees of freedom has important implications in both basic quantum physics and advanced information technology. Valley, as a new electronic degree of freedom, has received considerable attention in recent years. In this paper, we develop the theory of spin and valley physics of an antiferromagnetic honeycomb lattice. We show that by coupling the valley degree of freedom to antiferromagnetic order, there is an emergent electronic degree of freedom characterized by the product of spin and valley indices, which leads to spinvalley-dependent optical selection rule and Berry curvatureinduced topological quantum transport. These properties will enable optical polarization in the spin-valley space, and electrical detection/manipulation through the induced spin, valley, and charge fluxes. The domain walls of an antiferromagnetic honeycomb lattice harbors valley-protected edge states that support spin-dependent transport. Finally, we use first-principles calculations to show that the proposed optoelectronic properties may be realized in antiferromagnetic manganese chalcogenophosphates (MnPX 3 , X = S, Se) in monolayer form.antiferromagnetism | valleytronics
We investigate the valley-related carrier dynamics in monolayer molybdenum disulfide using helicity-resolved nondegenerate ultrafast pump-probe spectroscopy at the vicinity of the high-symmetry K point under the temperature down to 78 K. Monolayer molybdenum disulfide shows remarkable transient reflection signals, in stark contrast to bilayer and bulk molybdenum disulfide due to the enhancement of many-body effect at reduced dimensionality. The helicity-resolved ultrafast time-resolved result shows that the valley polarization is preserved for only several picoseconds before the scattering process makes it undistinguishable. We suggest that the dynamical degradation of valley polarization is attributable primarily to the exciton trapping by defect states in the exfoliated molybdenum disulfide samples. Our experiment and a tight-binding model analysis also show that the perfect valley circular dichroism selectivity is fairly robust against disorder at the K point but quickly decays from the high-symmetry point in the momentum space in the presence of disorder.
Valleys in monolayer transition-metal dichalcogenides seamlessly connect two basic carriers of quantum information, the electron spin and photon helicity. Lifting the valley degeneracy is an attractive route to achieve further optelectronic manipulations. However, magnetic field only creates a very small valley splitting. We propose a strategy to create giant valley splitting by proximityinduced Zeeman effect. Our first principles calculations of monolayer MoTe2 on a EuO substrate show that valley splitting over 300 meV can be generated. Interband transition energies become valley dependent, leading to selective spin-photon coupling by optical frequency tuning. The valley splitting is also continuously tunable by rotating the substrate magnetization. The giant and tunable valley splitting adds a new dimension to the exploration of novel optoelectronic devices based on magneto-optical coupling and magnetoelectric coupling. Introduction.-In many kinds of transition-metal dichalcogenide monolayers, a pair of degenerate valleys in the band structure give rise to novel valley-contrasting physics and potential applications. Electrons with a definite spin can be selectively excited by photons with a given helicity through the valleys, thereby furnishing a unique interface between the two elementary carriers of quantum information.1-4 . Valley Hall effect has also been observed recently, enabling electrical detection and manipulation of the photocurrent 5 . Furthermore, electronic states also possess valley-dependent orbital magnetic moments, which, together with the spin magnetic moment, provide the opportunities for magnetic control of the valleys and multiple electronic/optoelectronic functionalities based on magnetic effects.
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