118 research outputs found
Cathodoluminescence-based nanoscopic thermometry in a lanthanide-doped phosphor
Crucial to analyze phenomena as varied as plasmonic hot spots and the spread
of cancer in living tissue, nanoscale thermometry is challenging: probes are
usually larger than the sample under study, and contact techniques may alter
the sample temperature itself. Many photostable nanomaterials whose
luminescence is temperature-dependent, such as lanthanide-doped phosphors, have
been shown to be good non-contact thermometric sensors when optically excited.
Using such nanomaterials, in this work we accomplished the key milestone of
enabling far-field thermometry with a spatial resolution that is not
diffraction-limited at readout.
We explore thermal effects on the cathodoluminescence of lanthanide-doped
NaYF nanoparticles. Whereas cathodoluminescence from such lanthanide-doped
nanomaterials has been previously observed, here we use quantitative features
of such emission for the first time towards an application beyond localization.
We demonstrate a thermometry scheme that is based on cathodoluminescence
lifetime changes as a function of temperature that achieves 30 mK
sensitivity in sub-m nanoparticle patches. The scheme is robust against
spurious effects related to electron beam radiation damage and optical
alignment fluctuations.
We foresee the potential of single nanoparticles, of sheets of nanoparticles,
and also of thin films of lanthanide-doped NaYF to yield temperature
information via cathodoluminescence changes when in the vicinity of a sample of
interest; the phosphor may even protect the sample from direct contact to
damaging electron beam radiation. Cathodoluminescence-based thermometry is thus
a valuable novel tool towards temperature monitoring at the nanoscale, with
broad applications including heat dissipation in miniaturized electronics and
biological diagnostics.Comment: Main text: 30 pages + 4 figures; supplementary information: 22 pages
+ 8 figure
Blue-Light-Emitting Color Centers in High-Quality Hexagonal Boron Nitride
Light emitters in wide band gap semiconductors are of great fundamental
interest and have potential as optically addressable qubits. Here we describe
the discovery of a new color center in high-quality hexagonal boron nitride
(h-BN) with a sharp emission line at 435 nm. The emitters are activated and
deactivated by electron beam irradiation and have spectral and temporal
characteristics consistent with atomic color centers weakly coupled to lattice
vibrations. The emitters are conspicuously absent from commercially available
h-BN and are only present in ultra-high-quality h-BN grown using a
high-pressure, high-temperature Ba-B-N flux/solvent, suggesting that these
emitters originate from impurities or related defects specific to this unique
synthetic route. Our results imply that the light emission is activated and
deactivated by electron beam manipulation of the charge state of an
impurity-defect complex
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Chemical reactions of water molecules on Ru(0001) induced by selective excitation of vibrational modes
Tunneling electrons in a scanning tunneling microscope were used to excite specific vibrational quantum states of adsorbed water and hydroxyl molecules on a Ru(0 0 0 1) surface. The excited molecules relaxed by transfer of energy to lower energy modes, resulting in diffusion, dissociation, desorption, and surface-tip transfer processes. Diffusion of H{sub 2}O molecules could be induced by excitation of the O-H stretch vibration mode at 445 meV. Isolated molecules required excitation of one single quantum while molecules bonded to a C atom required at least two quanta. Dissociation of single H{sub 2}O molecules into H and OH required electron energies of 1 eV or higher while dissociation of OH required at least 2 eV electrons. In contrast, water molecules forming part of a cluster could be dissociated with electron energies of 0.5 eV
Electrically driven photon emission from individual atomic defects in monolayer WS2.
Quantum dot-like single-photon sources in transition metal dichalcogenides (TMDs) exhibit appealing quantum optical properties but lack a well-defined atomic structure and are subject to large spectral variability. Here, we demonstrate electrically stimulated photon emission from individual atomic defects in monolayer WS2 and directly correlate the emission with the local atomic and electronic structure. Radiative transitions are locally excited by sequential inelastic electron tunneling from a metallic tip into selected discrete defect states in the WS2 bandgap. Coupling to the optical far field is mediated by tip plasmons, which transduce the excess energy into a single photon. The applied tip-sample voltage determines the transition energy. Atomically resolved emission maps of individual point defects closely resemble electronic defect orbitals, the final states of the optical transitions. Inelastic charge carrier injection into localized defect states of two-dimensional materials provides a powerful platform for electrically driven, broadly tunable, atomic-scale single-photon sources
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Electronic interactions between gold nanoclusters in constrainedgeometries
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Reactivity of Ozone with Solid Potassium Iodide Investigated by Atomic Force Microscopy
The reaction of ozone with the (100) plane of solid potassium iodide (KI) was investigated using atomic force microscopy (AFM). The reaction forming potassium iodate (KIO{sub 3}) initiates at step edges prior to reacting on the flat terraces. Small domains of KIO{sub 3}, initially 3.8 {angstrom} in height are formed on the top of step edges. Following reaction at the step edge, domains of KIO{sub 3} are formed across the terraces. With prolonged exposure to ozone, KIO{sub 3} domains nucleate further growth until the surface is evenly covered with KIO{sub 3} particles that are 4-6 nm in height, at which point the surface is passivated and the reaction terminates
Near-monochromatic tuneable cryogenic niobium electron field emitter
Creating, manipulating, and detecting coherent electrons is at the heart of
future quantum microscopy and spectroscopy technologies. Leveraging and
specifically altering the quantum features of an electron beam source at low
temperatures can enhance its emission properties. Here, we describe electron
field emission from a monocrystalline, superconducting niobium nanotip at a
temperature of 5.9 K. The emitted electron energy spectrum reveals an
ultra-narrow distribution down to 16 meV due to tunable resonant tunneling
field emission via localized band states at a nano-protrusion's apex and a
cut-off at the sharp low-temperature Fermi-edge. This is an order of magnitude
lower than for conventional field emission electron sources. The self-focusing
geometry of the tip leads to emission in an angle of 3.7 deg, a reduced
brightness of 3.8 x 10exp8 A/(m2 sr V), and a stability of hours at 4.1 nA beam
current and 69 meV energy width. This source will decrease the impact of lens
aberration and enable new modes in low-energy electron microscopy, electron
energy loss spectroscopy, and high-resolution vibrational spectroscopy.Comment: to be published in Phys. Rev. Lett. (2022
Identifying substitutional oxygen as a prolific point defect in monolayer transition metal dichalcogenides with experiment and theory
Chalcogen vacancies are considered to be the most abundant point defects in
two-dimensional (2D) transition-metal dichalcogenide (TMD) semiconductors, and
predicted to result in deep in-gap states (IGS). As a result, important
features in the optical response of 2D-TMDs have typically been attributed to
chalcogen vacancies, with indirect support from Transmission Electron
Microscopy (TEM) and Scanning Tunneling Microscopy (STM) images. However, TEM
imaging measurements do not provide direct access to the electronic structure
of individual defects; and while Scanning Tunneling Spectroscopy (STS) is a
direct probe of local electronic structure, the interpretation of the chemical
nature of atomically-resolved STM images of point defects in 2D-TMDs can be
ambiguous. As a result, the assignment of point defects as vacancies or
substitutional atoms of different kinds in 2D-TMDs, and their influence on
their electronic properties, has been inconsistent and lacks consensus. Here,
we combine low-temperature non-contact atomic force microscopy (nc-AFM), STS,
and state-of-the-art ab initio density functional theory (DFT) and GW
calculations to determine both the structure and electronic properties of the
most abundant individual chalcogen-site defects common to 2D-TMDs.
Surprisingly, we observe no IGS for any of the chalcogen defects probed. Our
results and analysis strongly suggest that the common chalcogen defects in our
2D-TMDs, prepared and measured in standard environments, are substitutional
oxygen rather than vacancies
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