Search

Transition metal dichalcogenide (TMD) semiconductor heterostructures are actively explored as a new platform for quantum optoelectronic systems. Most state of the art devices make use of insulating hexagonal boron nitride (hBN) that acts as a wide-bandgap dielectric encapsulating layer that also provides an atomically smooth and clean interface that is paramount for proper device operation. We report the observation of large, through-hBN photocurrents that are generated upon optical excitation of hBN encapsulated MoSe2 and WSe2 monolayer devices. We attribute these effects to Auger recombination in the TMDs, in combination with an asymmetric band offset between the TMD and the hBN. We present experimental investigation of these effects and compare our observations with detailed, ab-initio modeling. Our observations have important implications for the design of optoelectronic devices based on encapsulated TMD devices. In systems where precise charge-state control is desired, the out-of-plane current path presents both a challenge and an opportunity for optical doping control. Since the current directly depends on Auger recombination, it can act as a local, direct probe of both the efficiency of the Auger process as well as its dependence on the local density of states in integrated devices.

A theory of spin injection from a ferromagnetic source into a semiconductor through a paramagnetic ion-doped nanocrystal is developed. Spin-polarized current from the source polarizes the ion; the polarized ion, in turn, controls the spin polarization of the current flowing through the nanocrystal. Depending on voltage, the ion can either enhance the injection coefficient by several times or suppress it. Large ion spins produce stronger enhancement of spin injection., Physics

Semiconductor nanoplatelets are atomically flat nanocrystals which emit light with high spectral purity at wavelengths controlled by their thickness. Despite their technological potential, efforts to further sharpen the emission lines of nanoplatelets have generally failed for unknown reasons. Here, we demonstrate theoretically that the linewidth is controlled by surface chemistry-specifically, inhomogeneities in the ligand layer on the nanoplatelet surface lead to a spatially fluctuating potential that localizes excitons. This localization leads to increased scattering and optical broadening. Importantly, localization also reduces the rate of radiative emission. Our model explains the observed linewidth and predicts that a more uniform ligand layer will sharpen the lines and increase the emission rates. These findings demonstrate that light emission from nanoplatelets can be controlled by optimizing their surface chemistry, an important advantage for their eventual use in optical technologies., (© 2024. This is a U.S. Government work and not under copyright protection in the US; foreign copyright protection may apply.)

The brightness of an emitter is ultimately described by Fermi's golden rule, with a radiative rate proportional to its oscillator strength times the local density of photonic states. As the oscillator strength is an intrinsic material property, the quest for ever brighter emission has relied on the local density of photonic states engineering, using dielectric or plasmonic resonators 1,2 . By contrast, a much less explored avenue is to boost the oscillator strength, and hence the emission rate, using a collective behaviour termed superradiance. Recently, it was proposed 3 that the latter can be realized using the giant oscillator-strength transitions of a weakly confined exciton in a quantum well when its coherent motion extends over many unit cells. Here we demonstrate single-photon superradiance in perovskite quantum dots with a sub-100 picosecond radiative decay time, almost as short as the reported exciton coherence time 4 . The characteristic dependence of radiative rates on the size, composition and temperature of the quantum dot suggests the formation of giant transition dipoles, as confirmed by effective-mass calculations. The results aid in the development of ultrabright, coherent quantum light sources and attest that quantum effects, for example, single-photon emission, persist in nanoparticles ten times larger than the exciton Bohr radius., (© 2024. The Author(s).)

Semiconductor nanoplatelets (NPLs), with their large exciton binding energy, narrow photoluminescence (PL), and absence of dielectric screening for photons emitted normal to the NPL surface, could be expected to become the fastest luminophores amongst all colloidal nanostructures. However, super-fast emission is suppressed by a dark (optically passive) exciton ground state, substantially split from a higher-lying bright (optically active) state. Here, the exciton fine structure in 2-8 monolayer (ML) thick Cs n - 1 Pb n Br 3n + 1 NPLs is revealed by merging temperature-resolved PL spectra and time-resolved PL decay with an effective mass model taking quantum confinement and dielectric confinement anisotropy into account. This approach exposes a thickness-dependent bright-dark exciton splitting reaching 32.3 meV for the 2 ML NPLs. The model also reveals a 5-16 meV splitting of the bright exciton states with transition dipoles polarized parallel and perpendicular to the NPL surfaces, the order of which is reversed for the thinnest NPLs, as confirmed by TR-PL measurements. Accordingly, the individual bright states must be taken into account, while the dark exciton state strongly affects the optical properties of the thinnest NPLs even at room temperature. Significantly, the derived model can be generalized for any isotropically or anisotropically confined nanostructure., (© 2021 The Authors. Advanced Science published by Wiley-VCH GmbH.)

Inorganic lead halide perovskite nanostructures show promise as the active layers in photovoltaics, light emitting diodes, and other optoelectronic devices. They are robust in the presence of oxygen and water, and the electronic structure and dynamics of these nanostructures can be tuned through quantum confinement. Here we create aligned bundles of CsPbBr 3 nanowires with widths resulting in quantum confinement of the electronic wave functions and subject them to ultrafast microscopy. We directly image rapid one-dimensional exciton diffusion along the nanowires, and we measure an exciton trap density of roughly one per nanowire. Using transient absorption microscopy, we observe a polarization-dependent splitting of the band edge exciton line, and from the polarized fluorescence of nanowires in solution, we determine that the exciton transition dipole moments are anisotropic in strength. Our observations are consistent with a model in which splitting is driven by shape anisotropy in conjunction with long-range exchange.

Vibrations are important cues for tactile perception across species. Whisker-based sensation in mice is a powerful model system for investigating mechanisms of tactile perception. However, the role vibration plays in whisker-based sensation remains unsettled, in part due to difficulties in modeling the vibration of whiskers. Here, we develop an analytical approach to calculate the vibrations of whiskers striking objects. We use this approach to quantify vibration forces during active whisker touch at a range of locations along the whisker. The frequency and amplitude of vibrations evoked by contact are strongly dependent on the position of contact along the whisker. The magnitude of vibrational shear force and bending moment is comparable to quasi-static forces. The fundamental vibration frequencies are in a detectable range for mechanoreceptor properties and below the maximum spike rates of primary sensory afferents. These results suggest two dynamic cues exist that rodents can use for object localization: vibration frequency and comparison of vibrational to quasi-static force magnitude. These complement the use of quasi-static force angle as a distance cue, particularly for touches close to the follicle, where whiskers are stiff and force angles hardly change during touch. Our approach also provides a general solution to calculation of whisker vibrations in other sensing tasks.

Nanostructured semiconductors emit light from electronic states known as excitons. For organic materials, Hund's rules state that the lowest-energy exciton is a poorly emitting triplet state. For inorganic semiconductors, similar rules predict an analogue of this triplet state known as the 'dark exciton'. Because dark excitons release photons slowly, hindering emission from inorganic nanostructures, materials that disobey these rules have been sought. However, despite considerable experimental and theoretical efforts, no inorganic semiconductors have been identified in which the lowest exciton is bright. Here we show that the lowest exciton in caesium lead halide perovskites (CsPbX 3 , with X = Cl, Br or I) involves a highly emissive triplet state. We first use an effective-mass model and group theory to demonstrate the possibility of such a state existing, which can occur when the strong spin-orbit coupling in the conduction band of a perovskite is combined with the Rashba effect. We then apply our model to CsPbX 3 nanocrystals, and measure size- and composition-dependent fluorescence at the single-nanocrystal level. The bright triplet character of the lowest exciton explains the anomalous photon-emission rates of these materials, which emit about 20 and 1,000 times faster than any other semiconductor nanocrystal at room and cryogenic temperatures, respectively. The existence of this bright triplet exciton is further confirmed by analysis of the fine structure in low-temperature fluorescence spectra. For semiconductor nanocrystals, which are already used in lighting, lasers and displays, these excitons could lead to materials with brighter emission. More generally, our results provide criteria for identifying other semiconductors that exhibit bright excitons, with potential implications for optoelectronic devices.

Rodents explore the world by palpating objects with their whiskers. Whiskers interact with objects, causing stresses in whisker follicles and spikes in sensory neurons, which are interpreted by the brain to produce tactile perception. The mechanics of the whisker thus couple self-movement and the structure of the world to sensation. Whiskers are elastic thin rods; hence, they tend to vibrate. Whisker vibrations could be a key ingredient of rodent somatosensation. However, the specific conditions under which vibrations contribute appreciably to the stresses in the follicle remain unclear. We present an analytical solution for the deformation of individual whiskers in response to a time-varying force. We tracked the deformation of mouse whiskers during a pole localization task to extract the whisker Young's modulus and damping coefficient. We further extracted the time course and amplitude of steady-state forces during whisker-object contact. We use our model to calculate the relative contribution of steady-state and vibrational forces to stresses in the follicle in a variety of active sensation tasks and during the passive whisker stimuli typically used for sensory physiology. Vibrational stresses are relatively more prominent compared with steady-state forces for short contacts and for contacts close to the whisker tip. Vibrational stresses are large for texture discrimination, and under some conditions, object localization tasks. Vibrational stresses are negligible for typical ramp-and-hold stimuli. Our calculation provides a general framework, applicable to most experimental situations.

The photoluminescence from a variety of individual molecules and nanometre-sized crystallites is defined by large intensity fluctuations, known as 'blinking', whereby their photoluminescence turns 'on' and 'off' intermittently, even under continuous photoexcitation. For semiconductor nanocrystals, it was originally proposed that these 'off' periods corresponded to a nanocrystal with an extra charge. A charged nanocrystal could have its photoluminescence temporarily quenched owing to the high efficiency of non-radiative (for example, Auger) recombination processes between the extra charge and a subsequently excited electron-hole pair; photoluminescence would resume only after the nanocrystal becomes neutralized again. Despite over a decade of research, completely non-blinking nanocrystals have not been synthesized and an understanding of the blinking phenomenon remains elusive. Here we report ternary core/shell CdZnSe/ZnSe semiconductor nanocrystals that individually exhibit continuous, non-blinking photoluminescence. Unexpectedly, these nanocrystals strongly photoluminesce despite being charged, as indicated by a multi-peaked photoluminescence spectral shape and short lifetime. To model the unusual photoluminescence properties of the CdZnSe/ZnSe nanocrystals, we softened the abrupt confinement potential of a typical core/shell nanocrystal, suggesting that the structure is a radially graded alloy of CdZnSe into ZnSe. As photoluminescence blinking severely limits the usefulness of nanocrystals in applications requiring a continuous output of single photons, these non-blinking nanocrystals may enable substantial advances in fields ranging from single-molecule biological labelling to low-threshold lasers.

The critical role that dopants play in semiconductor devices has stimulated research on the properties and the potential applications of semiconductor nanocrystals, or colloidal quantum dots, doped with intentional impurities. We review advances in the chemical synthesis of doped nanocrystals, in the theoretical understanding of the fundamental mechanisms that control doping, and in the creation of highly conducting nanocrystalline films. Because impurities can be used to alter the properties of nanoscale materials in desirable and controllable ways, doped nanocrystals can address key problems in applications from solar cells to bioimaging.

Doping--the intentional introduction of impurities into a material--is fundamental to controlling the properties of bulk semiconductors. This has stimulated similar efforts to dope semiconductor nanocrystals. Despite some successes, many of these efforts have failed, for reasons that remain unclear. For example, Mn can be incorporated into nanocrystals of CdS and ZnSe (refs 7-9), but not into CdSe (ref. 12)--despite comparable bulk solubilities of near 50 per cent. These difficulties, which have hindered development of new nanocrystalline materials, are often attributed to 'self-purification', an allegedly intrinsic mechanism whereby impurities are expelled. Here we show instead that the underlying mechanism that controls doping is the initial adsorption of impurities on the nanocrystal surface during growth. We find that adsorption--and therefore doping efficiency--is determined by three main factors: surface morphology, nanocrystal shape, and surfactants in the growth solution. Calculated Mn adsorption energies and equilibrium shapes for several nanocrystals lead to specific doping predictions. These are confirmed by measuring how the Mn concentration in ZnSe varies with nanocrystal size and shape. Finally, we use our predictions to incorporate Mn into previously undopable CdSe nanocrystals. This success establishes that earlier difficulties with doping are not intrinsic, and suggests that a variety of doped nanocrystals--for applications from solar cells to spintronics--can be anticipated.

A new lens that is a modification of the Veselago lens is proposed. It consists of a slab of the left-handed material embedded into a regular material. The materials for the new lens should have the same refractive index, unlike that of the Veselago lens in which the materials should in addition have the same impedance. Therefore the new lens should be easier to manufacture. As the Veselago lens, the new lens might be useful for the three dimensional imaging. In contrast to the Veselago lens the new lens has multiple foci, and it may image an object that is located at any large distance from the slab.