Electrostatic Control of Nonlinear Photonic-Crystal Polaritons in a Monolayer Semiconductor.

Integration of 2D semiconductors with photonic crystal slabs provides an attractive approach to achieving strong light-matter coupling and exciton-polariton formation in a chip-compatible geometry. However, for the development of practical devices, it is crucial that polariton excitations are easily tunable and exhibit a strong nonlinear response. Here we study neutral and charged exciton-polaritons in an electrostatically gated photonic crystal slab with an embedded monolayer semiconductor MoSe2 and experimentally demonstrate a novel approach to optical control based on polariton nonlinearity. We show that spatial modulation of the dielectric environment within the photonic crystal unit cell results in the formation of two distinct excitonic species with significantly different nonlinear responses of the corresponding charged exciton-polaritons under optical pumping. This behavior enables optical switching with ultrashort laser pulses and can be sensitively controlled via an electrostatic gate voltage. Our results open new avenues toward the development of active polaritonic devices in a compact chip-compatible implementation.

Enhanced Superconductivity in Few-Layer TaS2 due to Healing by Oxygenation.

When approaching the atomically thin limit, defects and disorder play an increasingly important role in the properties of two-dimensional (2D) materials. While defects are generally thought to negatively affect superconductivity in 2D materials, here we demonstrate the contrary in the case of oxygenation of ultrathin tantalum disulfide (TaS2). Our first-principles calculations show that incorporation of oxygen into the TaS2 crystal lattice is energetically favorable and effectively heals sulfur vacancies typically present in these crystals, thus restoring the electronic band structure and the carrier density to the intrinsic characteristics of TaS2. Strikingly, this leads to a strong enhancement of the electron-phonon coupling, by up to 80% in the highly oxygenated limit. Using transport measurements on fresh and aged (oxygenated) few-layer TaS2, we found a marked increase of the superconducting critical temperature (Tc) upon aging, in agreement with our theory, while concurrent electron microscopy and electron-energy loss spectroscopy confirmed the presence of sulfur vacancies in freshly prepared TaS2 and incorporation of oxygen into the crystal lattice with time. Our work thus reveals the mechanism by which certain atomic-scale defects can be beneficial to superconductivity and opens a new route to engineer Tc in ultrathin materials.

Superconductivity in Potassium-Doped Metallic Polymorphs of MoS2.

Superconducting layered transition metal dichalcogenides (TMDs) stand out among other superconductors due to the tunable nature of the superconducting transition, coexistence with other collective electronic excitations (charge density waves), and strong intrinsic spin-orbit coupling. Molybdenum disulfide (MoS2) is the most studied representative of this family of materials, especially since the recent demonstration of the possibility to tune its critical temperature, Tc, by electric-field doping. However, just one of its polymorphs, band-insulator 2H-MoS2, has so far been explored for its potential to host superconductivity. We have investigated the possibility to induce superconductivity in metallic polytypes, 1T- and 1T'-MoS2, by potassium (K) intercalation. We demonstrate that at doping levels significantly higher than that required to induce superconductivity in 2H-MoS2, both 1T and 1T' phases become superconducting with Tc = 2.8 and 4.6 K, respectively. Unusually, K intercalation in this case is responsible both for the structural and superconducting phase transitions. By adding new members to the family of superconducting TMDs, our findings open the way to further manipulate and enhance the electronic properties of these technologically important materials.

Tunable interlayer excitons and switchable interlayer trions via dynamic near-field cavity.

Emerging photo-induced excitonic processes in transition metal dichalcogenide (TMD) heterobilayers, e.g., interplay of intra- and inter-layer excitons and conversion of excitons to trions, allow new opportunities for ultrathin hybrid photonic devices. However, with the associated large degree of spatial heterogeneity, understanding and controlling their complex competing interactions in TMD heterobilayers at the nanoscale remains a challenge. Here, we present an all-round dynamic control of interlayer-excitons and -trions in a WSe2/Mo0.5 W0.5 Se2 heterobilayer using multifunctional tip-enhanced photoluminescence (TEPL) spectroscopy with <20 nm spatial resolution. Specifically, we demonstrate the bandgap tunable interlayer excitons and the dynamic interconversion between interlayer-trions and -excitons, through the combinational tip-induced engineering of GPa-scale pressure and plasmonic hot electron injection, with simultaneous spectroscopic TEPL measurements. This unique nano-opto-electro-mechanical control approach provides new strategies for developing versatile nano-excitonic/trionic devices using TMD heterobilayers.

Freestanding complex-oxide membranes.

Complex oxides show a vast range of functional responses, unparalleled within the inorganic solids realm, making them promising materials for applications as varied as next-generation field-effect transistors, spintronic devices, electro-optic modulators, pyroelectric detectors, or oxygen reduction catalysts. Their stability in ambient conditions, chemical versatility, and large susceptibility to minute structural and electronic modifications make them ideal subjects of study to discover emergent phenomena and to generate novel functionalities for next-generation devices. Recent advances in the synthesis of single-crystal, freestanding complex oxide membranes provide an unprecedented opportunity to study these materials in a nearly-ideal system (e.g. free of mechanical/thermal interaction with substrates) as well as expanding the range of tools for tweaking their order parameters (i.e. (anti-)ferromagnetic, (anti-)ferroelectric, ferroelastic), and increasing the possibility of achieving novel heterointegration approaches (including interfacing dissimilar materials) by avoiding the chemical, structural, or thermal constraints in synthesis processes. Here, we review the recent developments in the fabrication and characterization of complex-oxide membranes and discuss their potential for unraveling novel physicochemical phenomena at the nanoscale and for further exploiting their functionalities in technologically relevant devices.

Experimental observation of topological Z2 exciton-polaritons in transition metal dichalcogenide monolayers.

The rise of quantum science and technologies motivates photonics research to seek new platforms with strong light-matter interactions to facilitate quantum behaviors at moderate light intensities. Topological polaritons (TPs) offer an ideal platform in this context, with unique properties stemming from resilient topological states of light strongly coupled with matter. Here we explore polaritonic metasurfaces based on 2D transition metal dichalcogenides (TMDs) as a promising platform for topological polaritonics. We show that the strong coupling between topological photonic modes of the metasurface and excitons in TMDs yields a topological polaritonic Z2 phase. We experimentally confirm the emergence of one-way spin-polarized edge TPs in metasurfaces integrating MoSe2 and WSe2. Combined with the valley polarization in TMD monolayers, the proposed system enables an approach to engage the photonic angular momentum and valley and spin of excitons, offering a promising platform for photonic/solid-state interfaces for valleytronics and spintronics.

Nonlinear polaritons in a monolayer semiconductor coupled to optical bound states in the continuum.

Optical bound states in the continuum (BICs) provide a way to engineer very narrow resonances in photonic crystals. The extended interaction time in these systems is particularly promising for the enhancement of nonlinear optical processes and the development of the next generation of active optical devices. However, the achievable interaction strength is limited by the purely photonic character of optical BICs. Here, we mix the optical BIC in a photonic crystal slab with excitons in the atomically thin semiconductor MoSe2 to form nonlinear exciton-polaritons with a Rabi splitting of 27 meV, exhibiting large interaction-induced spectral blueshifts. The asymptotic BIC-like suppression of polariton radiation into the far field toward the BIC wavevector, in combination with effective reduction of the excitonic disorder through motional narrowing, results in small polariton linewidths below 3 meV. Together with a strongly wavevector-dependent Q-factor, this provides for the enhancement and control of polariton-polariton interactions and the resulting nonlinear optical effects, paving the way toward tuneable BIC-based polaritonic devices for sensing, lasing, and nonlinear optics.

Atomic Defects and Doping of Monolayer NbSe2.

We have investigated the structure of atomic defects within monolayer NbSe2 encapsulated in graphene by combining atomic resolution transmission electron microscope imaging, density functional theory (DFT) calculations, and strain mapping using geometric phase analysis. We demonstrate the presence of stable Nb and Se monovacancies in monolayer material and reveal that Se monovacancies are the most frequently observed defects, consistent with DFT calculations of their formation energy. We reveal that adventitious impurities of C, N, and O can substitute into the NbSe2 lattice stabilizing Se divacancies. We further observe evidence of Pt substitution into both Se and Nb vacancy sites. This knowledge of the character and relative frequency of different atomic defects provides the potential to better understand and control the unusual electronic and magnetic properties of this exciting two-dimensional material.