Although semiconductor defects can often be detrimental to device performance, they are also responsible for the breadth of functionality exhibited by modern optoelectronic devices. Artificially engineered defects (so-called quantum dots) or naturally occurring defects in solids are currently being investigated for applications ranging from quantum information science and optoelectronics to high-resolution metrology. In parallel, the quantum confinement exhibited by atomically thin materials (semi-metals, semiconductors and insulators) has ushered in an era of flatland optoelectronics whose full potential is still being articulated. In this Letter we demonstrate the possibility of leveraging the atomically thin semiconductor tungsten diselenide (WSe2) as a host for quantum dot-like defects. We report that this previously unexplored solid-state quantum emitter in WSe2 generates single photons with emission properties that can be controlled via the application of external d.c. electric and magnetic fields. These new optically active quantum dots exhibit excited-state lifetimes on the order of 1 ns and remarkably large excitonic g-factors of 10. It is anticipated that WSe2 quantum dots will provide a novel platform for integrated solid-state quantum photonics and quantum information processing, as well as a rich condensed-matter physics playground with which to explore the coupling of quantum dots and atomically thin semiconductors.
The optical properties of atomically thin semiconductor materials have been widely studied because of the isolation of monolayer transition metal dichalcogenides (TMDCs). They have rich optoelectronic properties owing to their large direct bandgap, the interplay between the spin and the valley degree of freedom of charge carriers, and the recently discovered localized excitonic states giving rise to single photon emission. In this Letter, we study the quantum-confined Stark effect of these localized emitters present near the edges of monolayer tungsten diselenide (WSe). By carefully designing sequences of metallic (graphene), insulating (hexagonal boron nitride), and semiconducting (WSe) two-dimensional materials, we fabricate a van der Waals heterostructure field effect device with WSe hosting quantum emitters that is responsive to external static electric field applied to the device. A very efficient spectral tunability up to 21 meV is demonstrated. Further, evaluation of the spectral shift in the photoluminescence signal as a function of the applied voltage enables us to extract the polarizability volume (up to 2000 Å) as well as information on the dipole moment of an individual emitter. The Stark shift can be further modulated on application of an external magnetic field, where we observe a flip in the sign of dipole moment possibly due to rearrangement of the position of electron and hole wave functions within the emitter.
Molybdenum disulfide (MoS2) flakes can grow beyond the edge of an underlying substrate into a planar freestanding crystal. When the substrate edge is in the form of an aperture, reagent-limited nucleation followed by edge growth facilitate direct and selective growth of freestanding MoS2 membranes. We have found conditions under which MoS2 grows preferentially across micrometer-scale prefabricated solid-state apertures in silicon nitride membranes, resulting in sealed membranes that are one to a few atomic layers thick. We have investigated the structure and purity of our membranes by a combination of atomic-resolution transmission electron microscopy, elemental analysis, Raman spectroscopy, photoluminescence spectroscopy, and low-noise ion-current recordings through nanopores fabricated in such membranes. Finally, we demonstrate the utility of fabricated ultrathin nanopores in such membranes for single-stranded DNA translocation detection.
The continually increasing demands for higher-speed and lower-operating-power devices have resulted in the continued impetus to shrink photonic components. We demonstrate a primitive nanophotonic integrated circuit element composed of a single silver nanowire and single-layer molybdenum disulfide (MoS 2 ) flake. Using scanning confocal fluorescence microscopy and spectroscopy, we find that nanowire plasmons can excite MoS 2 photoluminescence and that MoS 2 excitons can decay into nanowire plasmons. Finally, we show that the nanowire may serve the dual purpose of both exciting MoS 2 photoluminescence via plasmons and recollecting the decaying exciton as nanowire plasmons. The potential for subwavelength light guiding and strong nanoscale light-matter interaction afforded by our device may facilitate compact and efficient on-chip optical processing.
Atomically thin semiconductors, such as the transition metal dichalcogenides, show great potential for nanoscale photodetection, energy harvesting, and nanophotonics. Here, we investigate the efficiency of energy transfer between colloidal quantum dots with a cadmium selenide core and cadmium sulfide shell and monolayer molybdenum diselenide (MoSe 2). We show that MoSe 2 effectively quenches the fluorescence of quantum dots when the two materials are in contact. We then separate the MoSe 2 and quantum dots by inserting variable thickness hexagonal boron nitride (h-BN) spacers and show that the efficiency at which the MoSe 2 quenches fluorescence decreases as the h-BN thickness is increased. For distances d, this trend can be modeled by a 1/d 4 decay, in agreement with theory and recent studies involving graphene. V
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