Two-dimensional perovskites, in which inorganic layers are stabilized by organic spacer molecules, are attracting increasing attention as a more robust analogue to the conventional three-dimensional metal-halide perovskites. However, reducing the perovskite dimensionality alters their optoelectronic properties dramatically, yielding excited states that are dominated by bound electron-hole pairs known as excitons, rather than by free charge carriers common to their bulk counterparts. Despite the growing interest in two-dimensional perovskites for both light harvesting and light emitting applications, the full impact of the excitonic nature on their optoelectronic properties remains unclear, particularly regarding the spatial dynamics of the excitons within the two-dimensional (2D) plane.Here, we present direct measurements of in-plane exciton transport in single-crystalline layered perovskites. Using time-resolved fluorescence microscopy, we show that excitons undergo an initial fast, intrinsic normal diffusion through the crystalline plane, followed by a transition to a slower subdiffusive regime as excitons get trapped. Interestingly, the early intrinsic exciton diffusivity depends sensitively on the choice of organic spacer. We find a clear correlation between the stiffness of the lattice and the diffusivity, suggesting exciton-phonon interactions to be dominant in determining the spatial dynamics of the excitons in these materials. Our findings provide a clear design strategy to optimize exciton transport in these systems. lead, tin), X is a halide anion (chloride, bromide, iodide), L is a long organic spacer molecule, and n is the number of octahedra that make up the thickness of the inorganic layer. The separation into fewatom thick inorganic layers yields strong quantum and dielectric confinement effects. 38 As a result, the exciton binding energies in 2D perovskites can be as high as several hundreds of meVs, which is around an order of magnitude larger than those found in bulk perovskites. [39][40][41] The excitonic character of the excited state is accompanied by an effective widening of the bandgap, an increase in the oscillator strength, and a narrowing of the emission spectrum. [40][41][42] The strongest confinement effects are observed for n = 1, where the excited state is confined to a single B-X-octahedral layer (see Figure 1a).Light harvesting using 2D perovskites relies on the efficient transport of excitons and their subsequent separation into free charges. 43 This stands in contrast to bulk perovskites in which free charges are generated instantaneously thanks to the small exciton binding energy. 39 Particularly, with excitons being neutral quasi-particles, the charge extraction becomes significantly more challenging as they cannot be guided to the electrodes through an external electric field. 44 Excitons need to diffuse to an interface before the electron and hole can be efficiently separated into free charges. 45 On the other hand, for light emitting applications the spatial displacement is ...
The quartz-crystal microbalance (QCM) has become an important technique for the detection of biomolecules and their interactions. Acoustic sensing of DNA requires hybridizing the oligonucleotide chain with a nanoparticle that acts as an acoustic amplifier. In this device, the amplifier remains suspended in the liquid, nanometers away from the surface. The hydrodynamics of nonadsorbed nanoparticles in QCM sensing devices has, however, been overlooked in the literature. Here, we show that the acoustic response (shifts in frequency, f , and dissipation, D) of the amplifier-target complex is determined by the hydrodynamic wall stress. Our study focuses on an alternative type of DNA sensor based on liposome-DNA complexes and provides a theoretical analysis backed up by experiments with 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphocholine liposomes. The target DNA strands are attached on one side to surface-adsorbed neutravidin through a biotin linker, while the other side is anchored to a liposome acting as an amplifier. A range of liposome radii and double-stranded-DNA contour lengths are studied, covering sizes up to the wave penetration depth (δ ∼ 100 nm). Simulations, based on the immersed boundary method and an elastic-network model, are in excellent agreement with the experiments. We derive an analytical expression for the acoustic impedance, which reflects strong signal amplification as the liposome gets closer to the wall. This enhancement is due to hydrodynamic reflection: the ambient flow induces a stress on the liposome surface, which propagates back to the resonator. For this reason, acoustic signals are extremely sensitive to the distribution of the liposome-wall distance (which we determine from the mechanical properties of double-stranded-DNA chains). Our approach helps in deciphering the role of hydrodynamics in acoustic sensing and reveals the role of parameters hitherto largely unexplored. A practical consequence may be improvements in the design of biosensors and detection schemes.
Two-dimensional layered perovskites are attracting increasing attention as more robust analogues to the conventional three-dimensional metal-halide perovskites for both light harvesting and light emitting applications. However, the impact of the reduced dimensionality on the optoelectronic properties remains unclear, particularly regarding the spatial dynamics of the excitonic excited state within the two-dimensional plane. Here, we present direct measurements of exciton transport in single-crystalline layered perovskites. Using transient photoluminescence microscopy, we show that excitons undergo an initial fast diffusion through the crystalline plane, followed by a slower subdiffusive regime as excitons get trapped. Interestingly, the early intrinsic diffusivity depends sensitively on the choice of organic spacer. A clear correlation between lattice stiffness and diffusivity is found, suggesting exciton-phonon interactions to be dominant in the spatial dynamics of the excitons in perovskites, consistent with the formation of exciton-polarons. Our findings provide a clear design strategy to optimize exciton transport in these systems.
Background Transmission of COVID-19 via salivary aerosol particles generated when using handpieces or ultrasonic scalers is a major concern during the COVID-19 pandemic. The aim of this study was to assess the spread of dental aerosols on patients and dental providers during aerosol-generating dental procedures. Methods This pilot study was conducted with one volunteer. A dental unit used at the dental school for general dental care was the site of the experiment. Before the study, three measurement meters (DustTrak 8534, PTrak 8525 and AeroTrak 9306) were used to measure the ambient distribution of particles in the ambient air surrounding the dental chair. The volunteer wore a bouffant, goggles, and shoe covers and was seated in the dental chair in supine position, and covered with a surgical drape. The dentist and dental assistant donned bouffant, goggles, face shields, N95 masks, surgical gowns and shoe covers. The simulation was conducted by using a high-speed handpiece with a diamond bur operating in the oral cavity for 6 min without touching the teeth. A new set of measurement was obtained while using an ultrasonic scaler to clean all teeth of the volunteer. For both aerosol generating procedures, the aerosol particles were measured with the use of saliva ejector (SE) and high-speed suction (HSS) followed a separate set of measurement with the additional use of an extra oral high-volume suction (HVS) unit that was placed close to the mouth to capture the aerosol in addition to SE and HSS. The distribution of the air particles, including the size and concentration of aerosols, was measured around the patient, dentist, dental assistant, 3 feet above the patient, and the floor. Results Four locations were identified with elevated aerosol levels compared to the baseline, including the chest of the dentist, the chest of patient, the chest of assistant and 3 feet above the patient. The use of additional extra oral high volume suction reduced aerosol to or below the baseline level. Conclusions The increase of the level of aerosol with size less than 10 µm was minimal during dental procedures when using SE and HSS. Use of HVS further reduced aerosol levels below the ambient levels.
We discuss the properties of pure multipole beams with well-defined handedness or helicity, with the beam field a simultaneous eigenvector of the squared total angular momentum and its projection along the propagation axis. Under the condition of hemispherical illumination, we show that the only possible propagating multipole beams are "sectoral" multipoles. The sectoral dipole beam is shown to be equivalent to the non-singular time-reversed field of an electric and a magnetic point dipole Huygens' source located at the beam focus. Higher order multipolar beams are vortex beams vanishing on the propagation axis. The simple analytical expressions of the electric field of sectoral multipole beams, exact solutions of Maxwell's equations, and the peculiar behaviour of the Poynting vector and spin and orbital angular momenta in the focal volume could help to understand and model light-matter interactions under strongly focused beams. * juanjo.saenz@dipc.org 1 arXiv:1903.04753v1 [physics.optics]
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