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We identify an optical excitation mechanism that transfers a valley polarization from photo-excited electron-hole pairs to free charge carriers in twisted WSe$_2$/MoSe$_2$ heterobilayers. For small twist angles, the valley lifetimes of the charge carriers are surprisingly short, despite the occurrence of interlayer excitons with their presumably long recombination and polarization lifetimes. For large twist angles, we measure an increase in both the valley polarization and its respective lifetime by more than two orders of magnitude. Interestingly, in such heterobilayers we observe an interlayer transfer of valley polarization from the WSe$_2$ layer into the MoSe$_2$ layer. This mechanism enables the creation of a photo-induced valley polarization of free charge carriers in MoSe$_2$, which amplitude scales with the gate-induced charge carrier density. This is in contrast to monolayer MoSe$_2$, where such a gate-tunable valley polarization cannot be achieved. By combining time-resolved Kerr rotation, photoluminesence and angle-resolved photoemission spectroscopy measurements with first principles calculations, we show that these findings can be explained by twist angle dependent interlayer scattering mechanisms involving the Q- and $\Gamma$-valleys., Comment: 21 pages, 10 figures

While photons in free space barely interact, matter can mediate interactions between them resulting in optical nonlinearities. Such interactions at the single-quantum level result in an on-site photon repulsion, crucial for photon-based quantum information processing and for realizing strongly interacting many-body states of light. Here, we report repulsive dipole-dipole interactions between electric field tuneable, localized interlayer excitons in MoSe$_2$/WSe$_2$ heterobilayer. The presence of a single, localized exciton with an out-of-plane, non-oscillating dipole moment increases the energy of the second excitation by $\sim$ 2 meV -- an order of magnitude larger than the emission linewidth and corresponding to an inter-dipole distance of $\sim$ 5 nm. At higher excitation power, multi-exciton complexes appear at systematically higher energies. The magnetic field dependence of the emission polarization is consistent with spin-valley singlet nature of the dipolar molecular state. Our finding is an important step towards the creation of excitonic few- and many-body states such as dipolar crystals with spin-valley spinor in van der Waals (vdW) heterostructures.

Control and manipulation of single charges and their internal degrees of freedom, such as spins, is a fundamental goal of nanoscience with promising technological applications. Recently, atomically thin semiconductors such as WSe$_2$ have emerged as a platform for valleytronics, offering rich possibilities for optical, magnetic and electrical control of the valley index. While progress has been made in controlling valley index of ensemble of charge carriers, valley control of individual charges, crucial for valleytronics, remains unexplored. Here, we provide unambiguous evidence for localized holes with net spin in optically active WSe$_2$ quantum dots (QDs) and control their spin-valley state with the helicity of the excitation laser under small magnetic field. We estimate a lower bound on the valley lifetime of a single charge in QD from recombination time to be $\sim$ nanoseconds. Remarkably, neutral QDs do not exhibit such a control, demonstrating the role of excess charge in prolonging the valley lifetime. Our work extends the field of 2D valleytronics to the level of single spin-valley, relevant for quantum information and sensing applications

We measure the coherent nonlinear response of excitons in a single-layer of molybdenum disulphide embedded in hexagonal boron nitride, forming a $h$-BN/MoS$_2$/$h$-BN heterostructure. Using four-wave mixing microscopy and imaging, we correlate the exciton homogeneous and inhomogeneous broadenings. We find that the exciton dynamics is governed by microscopic disorder on top of the ideal crystal properties. Analyzing the exciton ultra-fast density dynamics using amplitude and phase of the response, we investigate the relaxation pathways of the resonantly driven exciton population. The surface protection via encapsulation provides stable monolayer samples with low disorder, avoiding surface contaminations and the resulting exciton broadening and modifications of the dynamics. We identify areas localized to a few microns where the optical response is totally dominated by homogeneous broadening. Across the sample of tens of micrometers, weak inhomogeneous broadening and strain effects are observed, attributed to the remaining interaction with the $h$-BN and imperfections in the encapsulation process.

Quantum entanglement is a fundamental phenomenon which, on the one hand, reveals deep connections between quantum mechanics, gravity and the space-time; on the other hand, has practical applications as a key resource in quantum information processing. While it is routinely achieved in photon-atom ensembles, entanglement involving the solid-state or macroscopic objects remains challenging albeit promising for both fundamental physics and technological applications. Here, we report entanglement between collective, chiral vibrations in two-dimensional (2D) WSe$_2$ host --- chiral phonons (CPs) --- and single-photons emitted from quantum dots (QDs) present in it. CPs which carry angular momentum were recently observed in WSe$_2$ and are a distinguishing feature of the underlying honeycomb lattice. The entanglement results from a "which-way" scattering process, involving an optical excitation in a QD and doubly-degenerate CPs, which takes place via two indistinguishable paths. Our unveiling of entanglement involving a macroscopic, collective excitation together with strong interaction between CPs and QDs in 2D materials opens up ways for phonon-driven entanglement of QDs and engineering chiral or non-reciprocal interactions at the single-photon level.

Few- and single-layer MoS2 host substantial densities of defects. They are thought to influence the doping level, the crystal structure, and the binding of electron-hole pairs. We disentangle the concomitant spectroscopic expression of all three effects and identify to what extent they are intrinsic to the material or extrinsic to it, i.e., related to its local environment. We do so by using different sources of MoS2 -- a natural one and one prepared at high pressure and high temperature -- and different substrates bringing varying amounts of charged impurities and by separating the contributions of internal strain and doping in Raman spectra. Photoluminescence unveils various optically active excitonic complexes. We discover a defect-bound state having a low binding energy of 20 meV that does not appear sensitive to strain and doping, unlike charged excitons. Conversely, the defect does not significantly dope or strain MoS2. Scanning tunneling microscopy and density functional theory simulations point to substitutional atoms, presumably individual nitrogen atoms at the sulfur site. Our work shows the way to a systematic understanding of the effect of external and internal fields on the optical properties of two-dimensional materials.

We probe quantum Hall effect in a tunable 1-D lateral superlattice (SL) in graphene created using electrostatic gates. Lack of equilibration is observed along edge states formed by electrostatic gates inside the superlattice. We create strong local electric field at the interface of regions of different charge densities. Crossed electric and magnetic fields modify the wavefunction of the Landau Levels (LLs) - a phenomenon unique to graphene. In the region of copropagating electrons and holes at the interface, the electric field is high enough to modify the Landau levels resulting in increased scattering that tunes equilibration of edge states and this results in large longitudinal resistance., Comment: Analysis modified and errors corrected

We study the photoresponse of graphene field effect transistors using scanning photocurrent microscopy in near and far field configurations, and we find that the response of graphene under a source-drain bias voltage away from the contacts is dominated by the bolometric effect caused by laser induced heating. We find no significant change in the photocurrent with the optical modulation frequency upto 100 kHz. Although the magnitude of the bolometric current scales with bias voltage, it also results in noise. The frequency dependence of this noise indicates that it has a 1/f character, scales with the bias voltage and limits the detectable bolometric photoresponse at low optical powers., Comment: 5 pages, 4 figures

Superlattice in graphene generates extra Dirac points in the band structure and their number depends on the superlattice potential strength. Here, we have created a lateral superlattice in a graphene device with a tunable barrier height using a combination of two gates. In this Letter, we demonstrate the use of lateral superlattice to modify the band structure of graphene leading to the emergence of new Dirac cones. This controlled modification of the band structure persists up to 100 K., Comment: Supplementary Information from the journal web page

We demonstrate a simple technique to transfer CVD-grown graphene from copper and platinum substrates using a soak-and-peel delamination technique utilizing only hot deionized water. The lack of chemical etchants results in cleaner CVD graphene films minimizing unintentional doping, as confirmed by Raman and electrical measurements. The process allows the reuse of substrates and hence can enable the use of oriented substrates for growth of higher quality graphene, and is an inherently inexpensive and scalable process for large-area production.

Using graphene resonator, we perform electromechanical measurements in quantum Hall regime to probe the coupling between a quantum Hall (QH) system and its mechanical motion. Mechanically perturbing the QH state through resonance modifies the DC resistance of the system and results in a Fano-lineshape due to electronic interference. Magnetization of the system modifies the resonator's equilibrium position and effective stiffness leading to changes in resonant frequency. Our experiments show that there is an intimate coupling between the quantum Hall state and mechanics - electron transport is affected by physical motion and in turn the magnetization modifies the electromechanical response., Comment: For supplemental material please go to http://www.tifr.res.in/~nano/publications.htm

In this report, we study electromechanical properties of a suspended InAs nanowire (NW) resonator. At low temperatures, the NW acts as the island of a single electron transistor (SET) and we observe a strong coupling between electrons and mechanical modes at resonance; the rate of electron tunneling is approximately 10 times the resonant frequency. Above and below the mechanical resonance, the magnitude of Coulomb peaks is different and we observe Fano resonance in conductance due to the interference between two contributions to potential of the SET. The quality factor ($Q$) of these devices is observed $\sim10^5$ at 100 mK., Comment: 4 pages. Supplementary material at http://www.tifr.res.in/~nano