Emerging quantum technologies for cryptography, computing and metrology exploit quantum mechanical effects for enhanced information processing and nanoscale sensing. Though different platform systems are currently being explored, light-based quantum technologies using single-photon emitters as the basic building block are among the frontrunners 1 . Several strategies have been used to realize deterministic single photon sources in the solid state 2 , including quantum dots 3 , single molecules 4 , and point defects in wide bandgap materials such as diamond and silicon carbide 5-9 . Single photon emitters in novel van der Waals materials have garnered recent attention due to their potential for integration with waveguides, microcavities, and other passive components typical in photonic devices. Example 2D systems hosting quantum emitters include WSe 2 and MoS 2 as well as other transition metal dichalcogenides (TMDs) 10-14 .Here we focus on hexagonal boron nitride (hBN), a wide bandgap semiconductor where defect emission has been shown to be tunable and robust at room temperature 15-22 and above 23 . We use confocal microscopy to investigate the photoluminescence (PL) of point defects within thin hBN flakes deposited on a lithographically patterned SiO 2 substrate. Due to Van der Waals forces the flake conforms to the surface topography thus accumulating significant local strain near protruding features. Using large structured arrays of different sizes and geometries we find nearly perfect correspondence between the strained areas of the flake and defect emission. Our modeling supports the notion of defect activation via charge trapping in deformation potential wells. The physics at play has some similarities with that governing the dynamics of excitons in WSe 2 monolayers subjected to comparable geometries, as reported recently 24,25 . Unlike TMDs, however, the wide bandgap of hBN can accommodate large potential modulations, sufficient to stabilize the defect charge at room temperature. In particular, we calculate deformation potential wells as deep as 500 meV confined to regions of tensile and compressive strain in the hBN flake that correlate well with the spatial localization of the emitters.For the first set of experiments we use an array of 155-nm-high nanopillars with diameters ranging from 200 to 700 nm fabricated via electron beam lithography over a large-area silica substrate (Figure 1a); the sample is a commercial, 20-nmthick flake of hBN grown via chemical vapor deposition (CVD). We follow a wet transfer protocol 26 to drape the flake on the patterned silica substrate (see Methods). This technique takes advantage of the Van der Waals forces to make the flake conform to the surface topography. As an illustration, Figure 1b shows an atomic force microscopy (AFM) image from an hBN fragment where the 20-nm-thick flake folds on itself: We identify single-and double-layer sections near the left and right areas, respectively; bare pillars -visible on the lower, right corner of the image -provide a direct view...
Cooperative phenomena stemming from radiation-field-mediated coupling between individual quantum emitters are presently attracting broad interest for on-chip photonic quantum memories and longrange entanglement. Common to these applications is the generation of electro-magnetic modes over macroscopic distances. Much research, however, is still needed before such systems can be deployed in the form of practical devices, starting with the investigation of alternate physical platforms. Quantum emitters in two-dimensional (2D) systems provide an intriguing route because these materials can be adapted to arbitrarily shaped substrates to form hybrid systems where emitters are near-field-coupled to suitable optical modes. Here, we report a scalable coupling method allowing color center ensembles in a van der Waals material -hexagonal boron nitride -to couple to a delocalized high quality plasmonic surface lattice resonance. This type of architecture is promising for photonic applications, especially given the ability of the hexagonal boron nitride emitters to operate as singlephoton sources at room temperature.
Bilayers of 2D materials offer opportunities for creating devices with tunable electronic, optical, and mechanical properties. In van der Waals heterostructures (vdWHs) where the constituent monolayers have different lattice constants, a moiré superlattice forms with a length scale larger than the lattice constant of either constituent material regardless of twist angle. Here, we report the appearance of moiré Raman modes from nearly aligned WSe2–WS2 vdWHs in the range of 240–260 cm–1, which are absent in both monolayers and homobilayers of WSe2 and WS2 and in largely misaligned WSe2–WS2 vdWHs. Using first-principles calculations and geometric arguments, we show that these moiré Raman modes are a consequence of the large moiré length scale, which results in zone-folded phonon modes that are Raman active. These modes are sensitive to changes in twist angle, but notably, they occur at identical frequencies for a given small twist angle away from either the 0-degree or 60-degree aligned heterostructure. Our measurements also show a strong Raman intensity modulation in the frequency range of interest, with near 0 and near 60-degree vdWHs exhibiting a markedly different dependence on excitation energy. In near 0-degree aligned WSe2–WS2 vdWHs, a nearly complete suppression of both the moiré Raman modes and the WSe2 A1g Raman mode (∼250 cm–1) is observed when exciting with a 532 nm CW laser at room temperature. Temperature-dependent reflectance contrast measurements demonstrate the significant Raman intensity modulation arises from resonant Raman effects.
There is wide interest in understanding and leveraging the nonlinear plasmon-induced potentials of nanostructured materials. We investigate the electrical response produced by spin-polarized light across a large-area bottom-up assembled 2D plasmonic crystal. Numerical approximations of the Lorentz forces provide quantitative agreement with our experimentally-measured DC voltages. We show that the underlying mechanism of the spin-polarized voltages is a gradient force that arises from asymmetric, time-averaged hotspots, whose locations shift with the chirality of light. Finally, we formalize the role of spin-orbit interactions in the shifted intensity patterns and significantly advance our understanding of the physical phenomena, often related to the spin Hall effect of light.
Color centers in hexagonal boron nitride (hBN) are presently attracting broad interest as a novel platform for nanoscale sensing and quantum information processing. Unfortunately, their atomic structures remain largely elusive and only a small percentage of the emitters studied thus far have the properties required to serve as optically addressable spin qubits. Here, we use confocal fluorescence microscopy at variable temperatures to study a new class of point defects produced via cerium ion implantation in thin hBN flakes. We find that, to a significant fraction, emitters show bright room-temperature emission, and good optical stability suggesting the formation of Ce-based point defects. Using density functional theory (DFT) we calculate the emission properties of candidate emitters, and single out the CeVB center—formed by an interlayer Ce atom adjacent to a boron vacancy—as one possible microscopic model. Our results suggest an intriguing route to defect engineering that simultaneously exploits the singular properties of rare-earth ions and the versatility of two-dimensional material hosts.
A broad effort is underway to understand and harness the interaction between superconductors and spin-active color centers with an eye on hybrid quantum devices and novel imaging modalities of superconducting materials. Most work, however, overlooks the interplay between either system and the environment created by the color center host. Here we use a diamond scanning probe to investigate the spin dynamics of a single nitrogen-vacancy (NV) center proximal to a superconducting film. We find that the presence of the superconductor increases the NV spin coherence lifetime, a phenomenon we tentatively rationalize as a change in the electric noise due to a superconductorinduced redistribution of charge carriers near induced redistribution of charge carriers near the NV. We then build on these findings to demonstrate transverse-relaxation-time-weighted imaging of the superconductor film. These results shed light on the dynamics governing the spin coherence of shallow NVs, and promise opportunities for new forms of noise spectroscopy and imaging of superconductors.
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