The strong light-matter interaction in monolayer transition metal dichalcogenides (TMDs) is promising for nanoscale optoelectronics with their direct band gap nature and the ultrafast radiative decay of the strongly bound excitons these materials host. However, the impeded amount of light absorption imposed by the ultra-thin nature of the monolayers impairs their viability in photonic applications. Using a layered heterostructure of a monolayer TMD stacked on top of strongly absorbing, non-luminescent, multi-layer SnSe2, we show that both single-photon and two-photon luminescence from the TMD monolayer can be enhanced by a factor of 14 and 7.5, respectively. This is enabled through inter-layer dipole-dipole coupling induced non-radiative Förster resonance energy transfer (FRET) from SnSe2 underneath which acts as a scavenger of the light unabsorbed by the monolayer TMD. The design strategy exploits the near-resonance between the direct energy gap of SnSe2 and the excitonic gap of monolayer TMD, the smallest possible separation between donor and acceptor facilitated by van der Waals heterojunction, and the inplane orientation of dipoles in these layered materials. The FRET driven uniform single-and twophoton luminescence enhancement over the entire junction area is advantageous over the local enhancement in quantum dot or plasmonic structure integrated 2D layers, and is promising for improving quantum efficiency in imaging, optoelectronic, and photonic applications. KEYWORDS: MoS2, WS2, SnSe2, van der Waals heterostructure, photoluminescence enhancement, two-photon luminescence, Förster Resonance Energy Transfer (FRET), charge transfer.transfer across WS2/MoSe2 hetero-bilayer stack through FRET across higher order exciton transitions. Nonetheless, the donor's absorption is still constrained by its physical thickness at the monolayer limit despite the high efficiency of FRET at the closest possible physical separation.Here, we demonstrate enhanced PL of monolayer MoS2 (and WS2) across its vdW heterojunction with multi-layer SnSe2 via FRET with single and two-photon excitation. Counteracting the charge transfer across highly staggered conduction bands of MoS2 and SnSe2, MoS2 single-photon luminescence (1P-PL) shows ~14-fold enhancement at room temperature with resonant excitation and ~5-fold enhancement with non-resonant excitation, while two-photon luminescence (2P-PL) of MoS2 shows up to ~7.5-fold enhancement with non-resonant excitation. Even with the insertion of few-layer hBN between MoS2 and SnSe2, the 1P-PL enhancement persists up to 5 times with resonant excitation. We demonstrate modulation of the degree of the PL enhancement by systematic parameter variation, including donor material, acceptor material, their thickness, physical separation between donor and acceptor, sample temperature, and excitation wavelength which corroborate FRET aided PL enhancement. We emphasize the intrinsic advantage of realizing FRET with SnSe2 as a donor and elucidate the impact of multiple parameters on the luminescence enhance...

Twisted van der Waals heterostructures unravel a new platform to study strongly correlated quantum phases. The interlayer coupling in these heterostructures is sensitive to twist angles (θ) and key to controllably tune several exotic properties. Here, we demonstrate a systematic evolution of the interlayer coupling strength with twist angle in bilayer MoS 2 using a combination of Raman spectroscopy and classical simulations. At zero doping, we show a monotonic increment of the separation between the A 1g and E 1 2g mode frequencies as θ decreases from 10 • → 1 • , which saturates to that for a bilayer at small twist angles. Furthermore, using doping-dependent Raman spectroscopy we reveal θ dependent softening and broadening of the A 1g mode, whereas the E 1 2g mode remains unaffected. Using first principles based simulations we demonstrate large (weak) electron-phonon coupling for the A 1g (E 1 2g ) mode explaining the experimentally observed trends. Our study provides a non-destructive way to characterize the twist angle, the interlayer coupling and establishes the manipulation of phonons in twisted bilayer MoS 2 (twistnonics).

Nonlinear optics is an important area of photonics research for realizing active optical functionalities such as light emission, frequency conversion, and ultrafast optical switching for applications in optical communication, material processing, precision measurements, spectroscopic sensing and label-free biological imaging. An emerging topic in nonlinear optics research is to realize high efficiency optical functionalities in ultra-small, sub-wavelength length scale structures by leveraging interesting optical resonances in surface relief metasurfaces. Such artificial surfaces can be engineered to support high quality factor resonances for enhanced nonlinear optical interaction by leveraging interesting physical mechanisms. The aim of this review article is to give an overview of the emerging field of nonlinear optics in dielectric based sub-wavelength periodic structures to realize efficient harmonic generators, wavelength mixers, optical switches etc. Dielectric metasurfaces support the realization of high quality-factor resonances with electric field concentrated either inside or in the vicinity of the dielectric media, while at the same time operate at high optical intensities without damage. The periodic dielectric structures considered here are broadly classified into guided-mode resonant structures and resonant metasurfaces. The basic physical mechanisms behind guided-mode resonances, electromagnetically-induced transparency like resonances and bound-states in continuum resonances in periodic photonic structures are discussed. Various nonlinear optical processes studied in such structures with example implementations are also reviewed. Finally, some future directions of interest in terms of realizing large-area metasurfaces, techniques for enhancing the efficiency of the nonlinear processes, heterogenous integration, and extension to non-conventional wavelength ranges in the ultra-violet and infrared region are discussed.

We report strong second-harmonic generation (SHG) from 2H polytype of multilayer Tin diselenide (SnSe2) for fundamental excitation close to the indirect band-edge in the absence of excitonic resonances. Comparison of SHG and Raman spectra from exfoliated SnSe2 flakes of different polytypes shows strong (negligible) SHG and Raman Eg mode at 109 cm−1 (119 cm−1), consistent with 2H (1T) polytypes. The difference between the A1g–Eg Raman peak positions is found to exhibit significant thickness dependent for the 1T form, which is found to be absent for the 2H form. The observed thickness dependence of SHG with rapid oscillations in signal strength for small changes in flake thickness are in good agreement with a nonlinear wave propagation model considering nonlinear polarization with alternating sign from each monolayer. The nonlinear optical susceptibility extracted from SHG signal comparison with standard quartz samples for 1040 nm excitation is found to be more than 4-times higher than that at 1550 nm. This enhanced nonlinear response at 1040 nm is attributed to the enhanced nonlinear optical response for fundamental excitation close to the indirect band-edge. We also study SHG from heterostructures of monolayer MoS2/multilayer SnSe2 which allows us to unambiguously compare the nonlinear optical response of SnSe2 with MoS2. We find the SHG signal and any interference effect in the overlap region to be dominated by the SnSe2 layer for the excitation wavelengths considered. The comparison of SHG from SnSe2 and MoS2 underscores that the choice of the 2D material for a particular nonlinear optical application is contextual on the wavelength range of interest and its optical properties at those wavelengths. The present works further highlights the usefulness of near band-edge enhancement of nonlinear processes in emerging 2D materials towards realizing useful nanophotonic devices.

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The integration of BaTiO3 with Si(100) is essential to exploit its ferroelectric capabilities in the well-established Si-complementary metal–oxide–semiconductor (CMOS) technological platform. To enable this goal, epitaxial BaTiO3 films with both in-plane and out-of-plane polarization are demonstrated on Si(100) with just a single TiN layer that is also CMOS-compatible. This change in polarization direction is brought about very simply by changing the growth temperature. Piezo force microscopy and optical second-harmonic generation measurements confirm the presence of out-of-plane and in-plane polarization. Films deposited at relatively higher temperatures of 800 °C have polarization lying in-plane at room temperature. The nonlinear dielectric susceptibilities were found to be comparable to the state-of-the-art films integrated with more complex transition schemes. Films deposited at a relatively lower temperature of 600 °C are defective and revert to 800 °C like films on annealing. The defects however confer on them an out-of-plane polarization with a large tetragonality of 1.6% at 500 °C. The changes in anomalous lattice expansion in out-of-plane coupled with coefficient of thermal expansion (CTE) strain result in orientation selection in our films.

Piezoelectric response in two-dimensional (2D) materials has evoked immense interest in using them for various applications involving electromechanical coupling. In most of the 2D materials, piezoelectricity is coupled along the in-plane direction. Here, we propose a technique to probe the in-plane piezoelectric coupling strength in layered nanomaterials quantitively. The method involves a novel approach for in-plane field excitation in lateral Piezoresponse force microscopy (PFM) for 2D materials. Operating near contact resonance has enabled the measurement of the piezoelectric coupling coefficients in the sub pm/V range. Detailed methodology for the signal calibration and the background subtraction when PFM is operated near the contact resonance of the cantilever is also provided. The technique is verified by estimating the in-plane piezoelectric coupling coefficients (d11) for freely suspended MoS2 of one to five atomic layers. For 2D-MoS2 with the odd number of atomic layers, which are non-centrosymmetric, finite d11 is measured. The measurements also indicate that the coupling strength decreases with an increase in the number of layers. The techniques presented would be an effective tool to study the in-plane piezoelectricity quantitatively in various materials along with emerging 2D-materials.

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