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Coherent coupling between excitons is at the heart of many-body interactions with transition metal dichalcogenide (TMD) heterostructures as an emergent platform for the investigation of these interactions. We employ multi-dimensional coherent spectroscopy on monolayer MoSe\textsubscript{2}/WSe\textsubscript{2} heterostructures and observe coherent coupling between excitons spatially localized in monolayer MoSe$_2$ and WSe$_2$. Through many-body spectroscopy, we further observe the absorption state arising from free interlayer electron-hole pairs. This observation yields a spectroscopic measurement of the interlayer exciton binding energy of about 250 meV.

New techniques for probing hyperbolic phonon polaritons (HPP) in 2D materials will support the development of the emerging technologies in this field. Previous reports have shown that it is possible for WSe2 monolayers in contact with the hexagonal boron nitride (hBN) to generate HPP in the hBN via Raman scattering. In this paper, we set out new results on HPP Raman scattering induced in hBN by WSe2 and MoSe2 monolayers including new resonances at which the Raman scattering is enhanced. Analysis of the observed Raman lineshapes demonstrates that Raman scattering allows HPP with wavevectors with magnitudes significantly in excess of 15000 cm-1 to be probed. We present evidence that the Raman scattering can probe HPP with frequencies less than the expected lower bound on the Reststrahlen band suggesting new HPP physics still waits to be discovered., 14 + 10 pages, 5 + 6 figures, in paper + supplementary info

The functional form of Coulomb interactions in the transition metal dichalcogenides and other van der Waals solids is critical to many of their unique properties, e.g. strongly-correlated electron states, superconductivity and emergent ferromagnetism. This paper presents measurements of key excitonic energy levels in MoSe2/WSe2 heterostructures. These measurements are obtained from resonance Raman experiments on specific Raman peaks only observed at excited states of the excitons. This data is used to validate a model of the Coulomb potential in these structures which predicts the exciton energies to within ~5 meV / 2.5%. This model is used to determine the effect of heterostructure formation on the single-particle band gaps of the layers and will have a wide applicability in designing the next generation of more complex transition metal dichalcogenide structures., Comment: 19 pages, 3 figures and an additional 14 pages, 7 figures of supplimentary info. Submitted to IOP 2D Materials

Moir�� structures in van der Waals heterostructures lead to emergent phenomena including superconductivity in twisted bilayer graphene and optically accessible strongly-correlated electron states in transition metal dichalcogenide heterobilayers. Dual periodicity moir�� structures (DPMS) formed in layered structures with more than two layers have been shown to lead to ferromagnetism and multiple secondary Dirac points in TBG. Whilst in principle it is possible to obtain DPMS in bilayers there has not been clear experimental evidence of this yet. In this paper we present signatures of DPMS in a twisted MoSe$_2$/WSe$_2$ bilayer revealed by resonance Raman spectroscopy. We observed zone-folded acoustic and optical phonon modes with a wavevector twice of the moir�� wavevector, evidence of a dual periodicity moir�� heterostructure. These results simultaneously open up opportunities for new emergent phenomena and an optical method for characterising DPMS in a wide range of van der Waals heterostructures., 16 pages, 3 Figures, 1 Table

The formation of interfacial moir�� patterns from angular and/or lattice mismatch has become a powerful approach to engineer a range of quantum phenomena in van der Waals heterostructures. For long-lived and valley-polarized interlayer excitons in transition-metal dichalcogenide (TMDC) heterobilayers, signatures of quantum confinement by the moir�� landscape have been reported in recent experimental studies. Such moir�� confinement has offered the exciting possibility to tailor new excitonic systems, such as ordered arrays of zero-dimensional (0D) quantum emitters and their coupling into topological superlattices. A remarkable nature of the moir�� potential is its dramatic response to strain, where a small uniaxial strain can tune the array of quantum-dot-like 0D traps into parallel stripes of one-dimensional (1D) quantum wires. Here, we present direct evidence for the 1D moir�� potentials from real space imaging and the corresponding 1D moir�� excitons from photoluminescence (PL) emission in MoSe2/WSe2 heterobilayers. Whereas the 0D moir�� excitons display quantum emitter-like sharp PL peaks with circular polarization, the PL emission from 1D moir�� excitons has linear polarization and two orders of magnitude higher intensity. The results presented here establish strain engineering as a powerful new method to tailor moir�� potentials as well as their optical and electronic responses on demand.

The creation of moir�� patterns in crystalline solids is a powerful approach to manipulate their electronic properties, which are fundamentally influenced by periodic potential landscapes. In 2D materials, a moir�� pattern with a superlattice potential can form by vertically stacking two layered materials with a twist and/or finite lattice constant difference. This unique approach has led to emergent electronic phenomena, including the fractal quantum Hall effect, tunable Mott insulators, and unconventional superconductivity. Furthermore, theory predicts intriguing effects on optical excitations by a moir�� potential in 2D valley semiconductors, but these signatures have yet to be experimentally detected. Here, we report experimental evidence of interlayer valley excitons trapped in a moir�� potential in MoSe$_2$/WSe$_2$ heterobilayers. At low temperatures, we observe photoluminescence near the free interlayer exciton energy but with over 100 times narrower linewidths. The emitter g-factors are homogeneous across the same sample and only take two values, -15.9 and 6.7, in samples with twisting angles near 60�� and 0��, respectively. The g-factors match those of the free interlayer exciton, which is determined by one of two possible valley pairing configurations. At a twist angle near 20��, the emitters become two orders of magnitude dimmer, but remarkably, they possess the same g-factor as the heterobilayer near 60��. This is consistent with the Umklapp recombination of interlayer excitons near the commensurate 21.8�� twist angle. The emitters exhibit strong circular polarization, which implies the preservation of three-fold rotation symmetry by the trapping potential. Together with the power and excitation energy dependence, all evidence points to their origin as interlayer excitons trapped in a smooth moir�� potential with inherited valley-contrasting physics.

Combining monolayers of different two-dimensional (2D) semiconductors into heterostructures opens up a wealth of possibilities for novel electronic and optical functionalities. Exploiting them hinges on accurate measurements of the band parameters and orbital hybridization in separate and stacked monolayers, many of which are only available as small samples. The recently introduced technique of angle-resolved photoemission spectroscopy with submicron spatial resolution ({\mu}-ARPES) offers the capability to measure small samples, but the energy resolution obtained for such exfoliated samples to date (~0.5 eV) has been inadequate. Here, we show that by suitable heterostructure sample design the full potential of {\mu}-ARPES can be realized. We focus on MoSe2/WSe2 van der Waals heterostructures, which are 2D analogs of 3D semiconductor heterostructures. We find that in a MoSe2/WSe2 heterobilayer the bands in the K valleys are weakly hybridized, with the conduction and valence band edges originating in the MoSe2 and WSe2 respectively. There is stronger hybridization at the {\Gamma} point, but the valence band edge remains at the K points. This is consistent with the recent observation of interlayer excitons where the electron and hole are valley polarized but in opposite layers. We determine the valence band offset to be 300 meV, which combined with photoluminescence measurements implies that the binding energy of interlayer excitons is at least 200 meV, comparable with that of intralayer excitons., Comment: 10 pages, 4 figures; + 14 pages, 8 figures in supplementary

Heterostructures comprising different monolayer semiconductors provide a new system for fundamental science and device technologies, such as in the emerging field of valleytronics. Here, we realize valley-specific interlayer excitons in monolayer WSe2-MoSe2 vertical heterostructures. We create interlayer exciton spin-valley polarization by circularly polarized optical pumping and determine a valley lifetime of 40 nanoseconds. This long-lived polarization enables the visualization of the expansion of a valley-polarized exciton cloud over several microns. The spatial pattern of the polarization evolves into a ring with increasing exciton density, a manifestation of valley exciton exchange interactions. Our work lays a foundation for quantum optoelectronics and valleytronics based on interlayer excitons in van der Waals heterostructures., Comment: This is the original submitted version. The final version is to appear in Science

Monolayer transition metal dichalcogenides, a new class of atomically thin semiconductors, possess optically coupled 2D valley excitons. The nature of exciton relaxation in these systems is currently poorly understood. Here, we investigate exciton relaxation in monolayer MoSe2 using polarization-resolved coherent nonlinear optical spectroscopy with high spectral resolution. We report strikingly narrow population pulsation resonances with two different characteristic linewidths of 1 ��eV and, (PRL, in press)

Heterojunctions between three-dimensional (3D) semiconductors with different bandgaps are the basis of modern light-emitting diodes, diode lasers, and high-speed transistors. Creating analogous heterojunctions between different two-dimensional (2D) semiconductors would enable band engineering within the 2D plane and open up new realms in materials science, device physics and engineering. Here we demonstrate that seamless high-quality in-plane heterojunctions can be grown between the 2D monolayer semiconductors MoSe2 and WSe2. The junctions, grown by lateral hetero-epitaxy using physical vapor transport, are visible in an optical microscope and show enhanced photoluminescence. Atomically resolved transmission electron microscopy reveals that their structure is an undistorted honeycomb lattice in which substitution of one transition metal by another occurs across the interface. The growth of such lateral junctions will allow new device functionalities, such as in-plane transistors and diodes, to be integrated within a single atomically thin layer., Comment: 14 pages manuscript + 12 pages supplementary information