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Valley-dependent excitation and emission in transition metal dichalcogenides (TMDCs) have recently emerged as a new avenue for optical data manipulation, quantum optical technologies, and chiral photonics. The valley-polarized electronic states can be optically addressed through photonic spin-orbit interaction of excitonic emission, typically with plasmonic nanostructures, but their performance is limited by the low quantum yield of neutral excitons in TMDC multilayers and the large Ohmic loss of plasmonic systems. Here, we demonstrate a valleytronic system based on the trion emission in high-quantum-yield WS2 monolayers chirally coupled to a low-loss microfiber. The integrated system uses the spin properties of the waveguided modes to achieve long-range directional routing of valley excitations and also provides an approach to selectively address valley-dependent emission from different spatial locations around the microfiber. This valleytronic interface can be integrated with fiber communication devices, allowing for merging valley polarization and chiral photonics as an alternative mechanism for optical information transport and manipulation in classical and quantum regimes.

Benefiting from strong photon–exciton and phonon–exciton interactions in atomic thickness, transition metal dichalcogenides (TMDCs) are viewed as one promising platform for exploring elementary excitonic photoluminescence (PL) and intrinsic spin–valley properties at the monolayer limit. Despite well-studied Stokes downconversion (DC) PL, the anti-Stokes upconversion (UC) PL has been recently reported in TMDC monolayers, which mainly focus on UC mechanisms while detailed valley-related dynamical processes are unwittingly less concerned. Here, we carry out an in-depth investigation on both DC and UC emission features of monolayer WS2 at room temperature, where UC PL persists with energy gain up to 190 meV. The PL excitation and power-dependent experiments clearly distinguish the origins of DC PL and UC PL, which refer to saturated absorption and phonon-assisted transition from charged trions to neutral A-excitons. And contrast valley properties are observed in DC and UC scenarios with polarization-resolved PL and pump–probe measurements. According to the experimental facts, phenomenological dynamical DC and UC scenarios are modeled with intervalley depolarization taken into consideration, in which intermediates from spontaneous intervalley depolarization account for the observed emission and valley properties. This work can help understand the light–matter interactions and valley properties in monolayer TMDCs.

Finding stimuli capable of driving an imbalance of spin polarised electrons within a solid is the central challenge in the development of spintronic devices. However, without the aid of magnetism, routes towards this goal are highly constrained with only a few suitable pairings of compounds and driving mechanisms found to date. Here, through spin and angle resolved photoemission along with density functional theory, we establish how the p derived bulk valence bands of semiconducting 1T HfSe2 possess a local, ground state spin texture spatially confined within each Se sublayer due to strong sublayer localised electric dipoles orientated along the c axis. This hidden spin polarisation manifests in a coupled spin orbital texture with in equivalent contributions from the constituent p orbitals. While the overall spin orbital texture for each Se sublayer is in strict adherence to time reversal symmetry TRS , spin orbital mixing terms with net polarisations at time reversal invariant momenta are locally maintained. These apparent TRS breaking contributions dominate, and can be selectively tuned between with a choice of linear light polarisation, facilitating the observation of pronounced spin polarisations at the Brillouin zone centre for all kz. We discuss the implications for the generation of spin polarised populations from 1T structured transition metal dichalcogenides using a fixed energy, linearly polarised light source

Layered transition metal dichalcogenides (TMDs) provide a favorable research platform for the advancement of spintronics and valleytronics because of their unique spin-valley coupling effect, which is attributed to the absence of inversion symmetry coupled with the presence of time-reversal symmetry. To maneuver the valley pseudospin efficiently is of great importance for the fabrication of conceptual devices in microelectronics. Here, we propose a straightforward way to modulate valley pseudospin with interface engineering. An underlying negative correlation between the quantum yield of photoluminescence and the degree of valley polarization was discovered. Enhanced luminous intensities were observed in the MoS2/hBN heterostructure but with a low value of valley polarization, which was in stark contrast to those observed in the MoS2/SiO2 heterostructure. Based on the steady-state and time-resolved optical measurements, we reveal the correlation between exciton lifetime, luminous efficiency, and valley polarization. Our results emphasize the significance of interface engineering for tailoring valley pseudospin in two-dimensional systems and probably advance the progression of the conceptual devices based on TMDs in spintronics and valleytronics.

We theoretically investigate the valley polarization in silicene with two parallel line defects due to Rashba spin-orbit coupling (RSOC). It is found that as long as RSOC exceeds the intrinsic spin-orbit coupling (SOC), the transmission coefficients of the two valleys oscillate with the same periodicity and intensity, which consists of wide transmission peaks and zero-transmission plateaus. However, in the presence of a perpendicular electric field, the oscillation periodicity of the first valley increases, whereas that of the second valley shortens, generating the corresponding wide peak-zero plateau regions, where perfect valley polarization can be achieved. Moreover, the valley polarizability can be changed from 1 to −1 by controlling the strength of the electric field. Our findings establish a different route for generating valley-polarized current by purely electrical means and open the door for interesting applications of semiconductor valleytronics.

Spatially periodic structures with a long range period, referred to as moir\'e pattern, can be obtained in van der Waals bilayers in the presence of a small stacking angle or of lattice mismatch between the monolayers. Theoretical predictions suggest that the resulting spatially periodic variation of the band structure modifies the optical properties of both intra and interlayer excitons of transition metal dichalcogenides heterostructures. Here, we report on the impact of the moir\'e pattern formed in a MoSe$_2$/MoS$_2$ heterobilayer encapsulated in hexagonal boron nitride. The periodic in-plane potential results in a splitting of the MoSe$_2$ exciton and trion in both emission and absorption spectra. The observed energy difference between the split peaks is fully consistent with theoretical predictions., Comment: just accepted in Nano Letters (10.1021/acs.nanolett.8b03266)

Transition-metal dichalcogenides are unique semiconductors because of their exclusive coupling between the spin and the valley degrees of freedom. The spin flip simultaneously requires a large amount of the crystal momentum variation; hence most of the carrier scattering is expected to be the spin-conserving intravalley scattering. Analysis of the quantum interference effects on the magnetoconductivity in ${\mathrm{WSe}}_{2},{\mathrm{MoSe}}_{2}$, and ${\mathrm{MoS}}_{2}$ reveals that the spin-relaxation time is orders of magnitude longer than the carrier momentum scattering time, indicating that the valley-spin coupling robustly protects the spin polarization from carrier scatterings. In addition, the electron-spin-relaxation time of ${\mathrm{MoSe}}_{2}$ is found to be anomalously short compared to other members, which is likely the origin of the ultrafast valley scattering of excitons in ${\mathrm{MoSe}}_{2}$.

The rise of atomically thin materials has the potential to enable a paradigm shift in modern technologies by introducing multi-functional materials in the semiconductor industry. To date the growth of high quality atomically thin semiconductors (e.g. WS2) is one of the most pressing challenges to unleash the potential of these materials and the growth of mono- or bi-layers with high crystal quality is yet to see its full realization. Here, we show that the novel use of molecular precursors in the controlled synthesis of mono- and bi-layer WS2 leads to superior material quality compared to the widely used topotactic transformation of WO3-based precursors. Record high room temperature charge carrier mobility up to 52 cm2/Vs and ultra-sharp photoluminescence linewidth of just 36 meV over submillimeter areas demonstrate that the quality of this material supersedes also that of naturally occurring materials. By exploiting surface diffusion kinetics of W and S species adsorbed onto a substrate, a deterministic layer thickness control has also been achieved promoting the design of scalable synthesis routes.

We investigate the excitonic transitions in single-and few-layer MoSe2 phototransistors by photocurrent spectroscopy. The measured spectral profiles show a well-defined peak at the optically active (bright) A(0) exciton resonance. More interestingly, when a gate voltage is applied to the MoSe2 to bring its Fermi level near the bottom of the conduction band, another prominent peak emerges at an energy 30 meV above the A(0) exciton. We attribute this second peak to a gate-induced activation of the spin-forbidden dark exciton transition, AD(0). Additionally, we evaluate the thickness-dependent optical bandgap of the fabricated MoSe2 crystals by characterizing their absorption edge.

Stacking atomic monolayers of semiconducting transition metal dichalcogenides (TMDs) has emerged as an effective way to engineer their properties. In principle, the staggered band alignment of TMD heterostructures should result in the formation of inter-layer excitons with long lifetimes and robust valley polarization. However, these features have been observed simultaneously only in MoSe$_2$/WSe$_2$ heterostructures. Here we report on the observation of long lived inter-layer exciton emission in a MoS$_2$/MoSe$_2$/MoS$_2$ trilayer van der Waals heterostructure. The inter-layer nature of the observed transition is confirmed by photoluminescence spectroscopy, as well as by analyzing the temporal, excitation power and temperature dependence of the inter-layer emission peak. The observed complex photoluminescence dynamics suggests the presence of quasi-degenerate momentum-direct and momentum-indirect bandgaps. We show that circularly polarized optical pumping results in long lived valley polarization of inter-layer exciton. Intriguingly, the inter-layer exciton photoluminescence has helicity opposite to the excitation. Our results show that through a careful choice of the TMDs forming the van der Waals heterostructure it is possible to control the circular polarization of the inter-layer exciton emission., Comment: 19 pages, 3 figures. Just accepted for publication in Nano Letters (http://pubs.acs.org/doi/10.1021/acs.nanolett.7b03184)

A rate equation model for the dark and bright excitons kinetics is proposed which explains the wide variation in the observed degree of circular polarization of the PL emission in different TMDs monolayers. Our work suggests that the dark exciton states play an important, and previously unsuspected role in determining the degree of polarization of the PL emission. A dark exciton ground state provides a robust reservoir for valley polarization, which tries to maintain a Boltzmann distribution of the bright exciton states in the same valley via the intra valley bright dark exciton scattering mechanism. The dependence of the degree of circular polarization on the detuning energy of the excitation in MoSe$_2$ suggests that the electron-hole exchange interaction dominates over two LA phonon emission mechanism for inter valley scattering in TMDs., Comment: text without changes, the misspelling of one of the names corrected

Functionalities of two-dimensional (2D) crystals based on semiconducting transition metal dichalcogenides (TMDs) have now stemmed from simple field effect transistors (FETs) to a variety of electronic and opto-valleytronic devices and even to superconductivity. Among them, superconductivity is the least studied property in TMDs due to methodological difficulty accessing it in different TMD species. Here, we report the systematic study of superconductivity in MoSe2, MoTe2 and WS2 by ionic gating in different regimes. Electrostatic gating using ionic liquid was able to induce superconductivity in MoSe2 but not in MoTe2 because of inefficient electron accumulation limited by electronic band alignment. Alternative gating using KClO4/polyethylene glycol enabled a crossover from surface doping to bulk doping, which induced superconductivities in MoTe2 and WS2 electrochemically. These new varieties greatly enriched the TMD superconductor families and unveiled critical methodology to expand the capability of ionic gating to other materials.

Coherent light sources in the visible range are playing important roles in our daily life and modern technology, since about 50% of the capability of the our human brains is devoted to processing visual information. Visible lasers can be achieved by nonlinear optical process of infrared lasers and direct lasing of gain materials and the latter has advantages in the aspects of compactness, efficiency, simplicity, etc. However, due to lack of visible optical modulators, the directly generated visible lasers with only a gain material are constrained in continuous-wave operation. Here, we demonstrated the fabrication of a visible optical modulator and pulsed visible lasers based on atomic-layer molybdenum sulfide (MoS2), a ultrathin two-dimensional material with about 9–10 layers. By employing the nonlinear absorption of the modulator, the pulsed orange, red and deep red lasers were directly generated. Besides, the present atomic-layer MoS2 optical modulator has broadband modulating properties and advantages in the simple preparation process. The present results experimentally verify the theoretical prediction for the low-dimensional optoelectronic modulating devices in the visible wavelength region and may open an attractive avenue for removing a stumbling block for the further development of pulsed visible lasers.

We demonstrate that spin polarization and valley polarization have quantitatively similar effects on the resistivity of a two-dimensional electron gas in a silicon-on-insulator quantum well. In so doing, we also examine the dependence on disorder, leading to a coarse but global phenomenology of how the resistivity depends on its key parameters: spin and valley polarization, density, disorder, and temperature.

Molybdenum disulfide (MoS2) has gained attention because of its high mobility and circular dichroism. As a crucial step to merge these advantages into a single device, we present a method that electronically controls and locates p-n junctions in liquid-gated ambipolar MoS2 transistors. A bias-independent p-n junction was formed, and it displayed rectifying I-V characteristics. This p-n diode could perform a crucial role in the development of optoelectronic valleytronic devices.