Local energy extrema of the bands in momentum space, or valleys, can endow electrons in solids with pseudo-spin in addition to real spin. In transition metal dichalcogenides this valley pseudo-spin, like real spin, is associated with a magnetic momen
t which underlies the valley-dependent circular dichroism that allows optical generation of valley polarization, intervalley quantum coherence, and the valley Hall effect. However, magnetic manipulation of valley pseudospin via this magnetic moment, analogous to what is possible with real spin, has not been shown before. Here we report observation of the valley Zeeman splitting and magnetic tuning of polarization and coherence of the excitonic valley pseudospin, by performing polarization-resolved magneto-photoluminescence on monolayer WSe2. Our measurements reveal both the atomic orbital and lattice contributions to the valley orbital magnetic moment; demonstrate the deviation of the band edges in the valleys from an exact massive Dirac fermion model; and reveal a striking difference between the magnetic responses of neutral and charged valley excitons which is explained by renormalization of the excitonic spectrum due to strong exchange interactions.
Monolayers of transition metal dichalcogenides (TMDCs) are atomically thin direct-gap semiconductors with potential applications in nanoelectronics, optoelectronics, and electrochemical sensing. Recent theoretical and experimental efforts suggest tha
t they are ideal systems for exploiting the valley degrees of freedom of Bloch electrons. For example, Dirac valley polarization has been demonstrated in mechanically exfoliated monolayer MoS2 samples by polarization-resolved photoluminescence, although polarization has rarely been seen at room temperature. Here we report a new method for synthesizing high optical quality monolayer MoS2 single crystals up to 25 microns in size on a variety of standard insulating substrates (SiO2, sapphire and glass) using a catalyst-free vapor-solid growth mechanism. The technique is simple and reliable, and the optical quality of the crystals is extremely high, as demonstrated by the fact that the valley polarization approaches unity at 30 K and persists at 35% even at room temperature, suggesting a virtual absence of defects. This will allow greatly improved optoelectronic TMDC monolayer devices to be fabricated and studied routinely.
Crystal symmetry governs the nature of electronic Bloch states. For example, in the presence of time reversal symmetry, the orbital magnetic moment and Berry curvature of the Bloch states must vanish unless inversion symmetry is broken. In certain 2D
electron systems such as bilayer graphene, the intrinsic inversion symmetry can be broken simply by applying a perpendicular electric field. In principle, this offers the remarkable possibility of switching on/off and continuously tuning the magnetic moment and Berry curvature near the Dirac valleys by reversible electrical control. Here we demonstrate this principle for the first time using bilayer MoS2, which has the same symmetry as bilayer graphene but has a bandgap in the visible that allows direct optical probing of these Berry-phase related properties. We show that the optical circular dichroism, which reflects the orbital magnetic moment in the valleys, can be continuously tuned from -15% to 15% as a function of gate voltage in bilayer MoS2 field-effect transistors. In contrast, the dichroism is gate-independent in monolayer MoS2, which is structurally non-centrosymmetric. Our work demonstrates the ability to continuously vary orbital magnetic moments between positive and negative values via symmetry control. This represents a new approach to manipulating Berry-phase effects for applications in quantum electronics associated with 2D electronic materials.
The unusual electrical and optical properties of graphene make it a promising candidate for optoelectronic applications. An important, but as yet unexplored aspect is the role of photo-excited hot carriers in charge and energy transport at graphene i
nterfaces. Here, we perform time-resolved (~250 fs) scanning photocurrent microscopy on a tunable graphene pn junction. The ultrafast pump-probe measurements yield a photocurrent response time of ~1.5 ps at room temperature increasing to ~4 ps at 20 K. Combined with the negligible dependence of photocurrent amplitude on environmental temperature this implies that hot carriers rather than phonons dominate energy transport at high frequencies. Gate-dependent pump-probe measurements demonstrate that both thermoelectric and built-in electric field effects contribute to the photocurrent excited by laser pulses. The relative weight of each contribution depends on the junction configuration. A single laser beam excitation also displays multiple polarity-reversals as a function of carrier density, a signature of impact ionization. Our results enhance the understanding of non-equilibrium electron dynamics, electron-electron interactions, and electron-phonon interactions in graphene. They also determine fundamental limits on ultrafast device operation speeds (~500 GHz) for potential graphene-based photon detection, sensing, and communication.
