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Manipulating Spin-polarized Photocurrent in 2D Transition Metal Dichalcogenides

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 Added by Xiaodong Cui Dr.
 Publication date 2015
  fields Physics
and research's language is English




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Manipulating spin polarization of electrons in nonmagnetic semiconductors by means of electric fields or optical fields is an essential theme of the conceptual nonmagnetic semiconductor-based spintronics. Here we experimentally demonstrate a method of generating spin polarization in monolayer transition metal dichalcogenides (TMD) by the circularly polarized optical pumping. The fully spin-polarized photocurrent is achieved through the valley dependent optical selection rules and the spin-valley locking in monolayer WS2, and electrically detected by a lateral spin-valve structure with ferromagnetic contacts. The demonstrated long spin lifetime, the unique valley contrasted physics and the spin-valley locking make monolayer WS2 an unprecedented candidate for semiconductor based spintronics.



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We study the optical properties of semiconducting transition metal dichalcogenide monolayers under the influence of strong out-of-plane magnetic fields, using the effective massive Dirac model. We pay attention to the role of spin-orbit coupling effects, doping level and electron-electron interactions, treated at the Hartree-Fock level. We find that optically-induced valley and spin imbalance, commonly attained with circularly polarized light, can also be obtained with linearly polarized light in the doped regime. Additionally, we explore an exchange-driven mechanism to enhance the spin-orbit splitting of the conduction band, in n-doped systems, controlling both the carrier density and the intensity of the applied magnetic field.
In this paper we develop the excitonic theory of Kerr rotation angle in a two-dimensional (2D) transition metal dichalcogenide at zero magnetic field. The finite Kerr angle is induced by the interplay between spin-orbit splitting and proximity exchange coupling due to the presence of a ferromagnet. We compare the excitonic effect with the single particle theory approach. We show that the excitonic properties of the 2D material lead to a dramatic change in the frequency dependence of the optical response function. We also find that the excitonic corrections enhance the optical response by a factor of two in the case of MoS2 in proximity to a Cobalt thin film.
Monolayer transition metal dichalcogenides are promising materials for valleytronic operations. They exhibit two inequivalent valleys in the Brillouin zone, and the valley populations can be directly controlled and determined using circularly polarized optical excitation and emission. The photoluminescence polarization reflects the ratio of the two valley populations. A wide range of values for the degree of circularly polarized emission, Pcirc, has been reported for monolayer WS2, although the reasons for the disparity are unclear. Here we optically populate one valley, and measure Pcirc to explore the valley population dynamics at room temperature in a large number of monolayer WS2 samples synthesized via chemical vapor deposition. Under resonant excitation, Pcirc ranges from 2% to 32%, and we observe a pronounced inverse relationship between photoluminescence (PL) intensity and Pcirc. High quality samples exhibiting strong PL and long exciton relaxation time exhibit a low degree of valley polarization, and vice versa. This behavior is also demonstrated in monolayer WSe2 samples and transferred WS2, indicating that this correlation may be more generally observed and account for the wide variations reported for Pcirc. Time resolved PL provides insight into the role of radiative and non-radiative contributions to the observed polarization. Short non-radiative lifetimes result in a higher measured polarization by limiting opportunity for depolarizing scattering events.
We study valley-dependent spin transport theoretically in monolayer transition-metal dichalcogenides in which a variety of spin and valley physics are expected because of spin-valley coupling. The results show that the spins are valley-selectively excited with appropriate carrier doping and valley polarized spin current (VPSC) is generated. The VPSC leads to the spin-current Hall effect, transverse spin accumulation originating from the Berry curvature in momentum space. The results indicate that spin excitations with spin-valley coupling lead to both valley and spin transport, which is promising for future low-consumption nanodevice applications.
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