Microsphere-Enabled Micropillar Array for Whispering Gallery Mode Virus Detection.

Rapid detection of pathogens and analytes at the point of care offers an opportunity for prompt patient management and public health control. This paper reports an open microfluidic platform coupled with active whispering gallery mode (WGM) microsphere resonators for the rapid detection of influenza viruses. The WGM microsphere resonators, precoated with influenza A polyclonal antibodies, are mechanically trapped in the open micropillar array, where the evaporation-driven flow continuously transports a small volume (∼µL) of sample to the resonators without auxiliaries. Selective chemical modification of the pillar array changes surface wettability and flow pattern, which enhances the detection sensitivity of the WGM resonator-based virus sensor. The optofluidic sensing platform is able to specifically detect influenza A viruses within 15 min using a few microliters of sample and displays a linear response to different virus concentrations.

Ultra-high-resolution greyscale fluorescence images via UV-exposure of thin flexible phosphor films.

Thin films of BaFCl:Sm nanocrystals prepared using a polymer binder were used to create fluorescence images. The phosphor films were exposed to a UV-C mercury lamp light source via chromium-coated quartz greyscale masks to create 4 µm resolution greyscale fluorescence images. The mechanism relies on the highly efficient conversion of Sm3+ to Sm2+ ions upon exposure to UV-C light which displays a large linear dynamic range. The red fluorescence around 688 nm of the Sm2+ is then read-out using blue-violet illumination under a laser scanning confocal microscope. The greyscale images with 16 greyscale levels had a resolution equivalent to ∼125 line pairs per mm or ∼6400 dpi. Improvements in the resolution would be possible using collimated UV-C laser exposure of the film or the use of higher resolution photomasks. Ultra-high resolution binary fluorescence images were also created with resolutions down to 2 µm (∼250 line pairs per mm, ∼12 700 dpi). Downstream applications of the technology could include tailored covert or overt anti-counterfeiting labelling.

Caged-Sphere Optofluidic Sensors: Whispering Gallery Resonators in Wicking Microfluidics.

The rapid development of optofluidic technologies in recent years has seen the need for sensing platforms with ease-of-use, simple sample manipulation, and high performance and sensitivity. Herein, an integrated optofluidic sensor consisting of a pillar array-based open microfluidic chip and caged dye-doped whispering gallery mode microspheres is demonstrated and shown to have potential for simple real-time monitoring of liquids. The open microfluidic chip allows for the wicking of a thin film of liquid across an open surface with subsequent evaporation-driven flow enabling continuous passive flow for sampling. The active dye-doped whispering gallery mode microspheres placed between pillars, avoid the use of cumbersome fibre tapers to couple light to the resonators as is required for passive microspheres. The performance of this integrated sensor is demonstrated using glucose solutions (0.05-0.3 g/mL) and the sensor response is shown to be dynamic and reversible. The sensor achieves a refractive index sensitivity of ~40 nm/RIU, with Q-factors of ~5 × 103 indicating a detection limit of ~3 × 10-3 RIU (~20 mg/mL glucose). Further enhancement of the detection limit is expected by increasing the microsphere Q-factor using high-index materials for the resonators, or alternatively, inducing lasing. The integrated sensors are expected to have significant potential for a host of downstream applications, particularly relating to point-of-care diagnostics.

Efficient coupling between single mode fibers and glass chip waveguides via graded refractive index fiber tips.

Coupling characteristics between a single mode fiber (SMF) and a waveguide embedded in a glass chip via a graded index fiber (GIF) tip are investigated at a wavelength of 976 nm. The GIF tips comprise a coreless fiber section and a GIF section. A depressed cladding waveguide in a ZBLAN glass chip with a core diameter of 35 µm is coupled with GIF tips that have a range of coreless fiber and GIF lengths. An experimental coupling efficiency as high as 88% is obtained while a numerical simulation predicts 92.9% for the same GIF tip configuration. Since it is measured in the presence of Fresnel reflection, it can be further improved by anti-reflection coating. Additionally, it is demonstrated that a gap can be introduced between the chip waveguide and the GIF tip while maintaining the high coupling efficiency, thus allowing a thin planar optical component to be inserted. The results presented here will enable miniaturization and simplification of photonic chips with integrated waveguides by replacing bulk coupling lenses with integrated optical fibers.

Reversible Mn valence state switching in submicron α-Al2O3:Mn by soft X-rays and blue light - a potential pathway towards multilevel optical data storage.

The generation of Mn4+ in α-Al2O3:Mn3+ by soft X-ray exposure is demonstrated with a large dynamic range of the X-ray generated Mn4+ luminescence signal, indicating the potential use of α-Al2O3:Mn3+ for multilevel optical data storage. Samples with a range of Mn concentrations (0.05, 0.1, 0.2, 0.4, 0.6 and 1.2 atom%) were prepared via a facile combustion method and the sample with 0.4 atom% was found to display the highest luminescence intensity. The stored information can be read out via the R-lines (2E → 4A2) under ∼470 nm (4A2 → 4T2), or ∼630 nm (4A2 → 2T1) excitation with the latter being preferred since photobleaching is minimized. Interestingly, the Mn4+ valence state can be fully switched back to Mn3+ by blue light exposure (e.g., 462 nm laser diode). The stored information could be repeatedly written and erased, showing no significant deterioration over five consecutive cycles, with less than 5% uncertainty.

Spin-forbidden near-infrared luminescence from a F3+ colour centre generated upon annealing in mechanochemically prepared nanocrystalline BaLiF3.

We report the properties of a unique colour centre in mechanochemically synthesized inverse perovskite BaLiF3 submicron crystals that are luminescent at ∼765 nm. The spin-forbidden luminescence with a lifetime of 5 ms is attributed to a F3+ (F-centre aggregate) in the fluoride octahedra, with three fluoride anion vacancies (3F+) filled with two electrons (2e-). The Zeeman splitting of the electronic origin and its temperature dependence indicate that the transition is from a singlet excited state to a triplet ground state. The F3+ emission occurred after annealing (≥500 °C) the mechanochemically prepared pure BaLiF3 nanocrystals and is characterized by a structured emission with a relatively narrow zero-phonon line. A reduction of photoluminescence intensity of the F3+ band upon increasing X-ray dose was observed. Importantly, it is observed that the F3+ luminescence is stable in the dark but bleaches upon exposure to natural sunlight. Our results point to the potential for a new colour centre-based nano-laser in the near-infrared region. Additionally, our experiments also indicate that BaLiF3 : F3+ has some potential for data storage, and X-ray imaging and dosimetry.

Luminescence and photoionization of X-ray generated Sm2+ in coprecipitated CaF2 nanocrystals.

We report photoluminescence and photoionization properties of Sm2+ ions generated by X-irradiation of nanocrystalline CaF2:Sm3+ prepared by coprecipitation. The nanocrystals were of 46 nm average crystallite size with a distribution of ±20 nm and they were characterised by XRD, TEM and SEM-EDS. At room temperature, the X-irradiated sample displayed broad electric dipole allowed Sm2+ 4f55d (A1u) → 4f6 7F1 (T1g) luminescence at 725 nm that narrowed to an intense peak at 708 nm on cooling to ∼30 K. The narrow f-f transitions of Sm3+ were also observed. The X-irradiation-induced reduction of Sm3+ + e- → Sm2+ as a function of X-ray dose was investigated over a very wide dynamic range from 0.01 mGy to 850 Gy by monitoring the photoluminescence intensities of both Sm2+ and Sm3+ ions. The reverse Sm2+ → Sm3+ + e- photoionization can be modelled by employing dispersive first-order kinetics and using a standard gamma distribution function, yielding an average separation of 13 Å between the Sm2+ ions and the hole traps (e.g. oxide ion impurities). The present results point towards potential applications of Sm doped CaF2 nanocrystals in the fields of dosimetry and X-ray imaging.

Whispering gallery mode excitation using exposed-core fiber.

Whispering gallery modes (WGMs) in micro-resonators are of interest due to their high Q-factors. Ultra-thin fiber tapers are widely deployed to couple light into micro-resonators but achieving stable and practical coupling for out-of-lab use remains challenging. Here, a new WGM coupling scheme using an exposed-core silica fiber (ECF) is proposed, which overcomes the challenge of using fragile fiber tapers. Microspheres are deposited onto the exposed channel for excitation via the evanescent field of the fiber's guided modes. The outer jacket of the ECF partially encapsulates the microspheres, protecting them from external physical disturbance. By varying the mode launching conditions in this few-mode ECF, in combination with a Fano resonance effect, we demonstrate a high degree of tunability in the reflection spectrum. Furthermore, we show multi-particle WGM excitation, which could be controlled to occur either simultaneously or separately through controlling the ECF mode launching conditions. This work can bring value towards applications such as optical switches and modulators, multiplexed/distributed biosensing, and multi-point lasing, integrated in a single optical fiber device that avoids fiber post-processing.

Design guidelines for collimating or focusing graded-index fiber tips.

Graded-index optical fiber probes suitable for focusing or collimating the output of an optical fiber at a wavelength of 1.3 µm have become an enabling technology in optical coherence tomography imaging applications for in vivo bioimaging. Such fiber tips however remain uncommon in other photonics applications. This paper provides the first numerical study of graded-index fiber tips covering a broad range of wavelengths spanning from the UV to short-infrared. The wavelength dependency and the influence of probe geometry on performance characteristics such as far-field divergence angle, spot size and working distance are analyzed. The paper yields easily accessible design guidelines for the fabrication of collimating or focusing fiber tips. Fiber collimators have considerable potential for use in free-space systems and could benefit a range of devices such as variable attenuators, dynamic wavelength equalisers and large 3D optical cross-connect switches, whereas focusing fiber tips have applications in high-resolution imaging.

On-chip absorption spectroscopy enabled by graded index fiber tips.

This paper describes the design and characterization of miniaturized optofluidic devices for sensing based on integrating collimating optical fibers with custom microfluidic chips. The use of collimating graded-index fiber (GIF) tips allows for effective fiber-channel-fiber interfaces to be realized when compared with using highly-divergent standard single-mode fiber (SMF). The reduction in both beam divergence and insertion losses for the GIF configuration compared with SMF was characterized for a 10.0 mm channel. Absorption spectroscopy was demonstrated on chip for the measurement of red color dye (Ponceau 4R), and the detection of thiocyanate in water and artificial human saliva. The proposed optofluidic setup allows for absorption spectroscopy measurements to be performed with only 200 µL of solution which is an order of magnitude smaller than for standard cuvettes but provides a comparable sensitivity. The approach could be integrated into a lab-on-a-chip system that is compact and does not require free-space optics to perform absorption spectroscopy.

On the origins of the green luminescence in the "zero-dimensional perovskite" Cs4PbBr6: conclusive results from cathodoluminescence imaging.

There is great interest in the use of highly-efficient all-inorganic halide perovskites CsnPbBr2+n for optoelectronic applications. There however remains considerable debate as to the origins of the green luminescence in the zero-dimensional phase of the perovskite Cs4PbBr6, with theories suggesting it originates either from defects in the Cs4PbBr6 lattice or CsPbBr3 impurities/inclusions. The confusion has arisen due to the two phases being miscible and typically co-existing. Moreover, low impurity levels of CsPbBr3 in Cs4PbBr6 are difficult to detect by XRD measurements, yet have much stronger photoluminescence than bulk CsPbBr3 that exhibits quenching, further contributing to the confusion as to the origins of the green photoluminescence. With the rise of significant debate and misconceptions, we provide conclusive evidence that the green emission from Cs4PbBr6 is indeed due to nanocrystalline CsPbBr3 impurities. This is demonstrated by undertaking cathodoluminescence and EDX measurements on samples prepared mechanochemically by ball-milling. Cathodoluminescence imaging clearly shows the presence of small crystals embedded in/or between larger crystallites of Cs4PbBr6 and they emit around 520 nm. EDX shows that the smaller crystal inclusions have a Pb : Br ratio that is approximately 2 times higher, confirming the CsPbBr3 phase, which has the expected size-dependent shift to shorter wavelengths (about 528 to 515 nm). These studies make significant inroads into understanding these lead halide perovskites for their use in a variety of optoelectronic and photovoltaic applications.

Mode-Splitting for Refractive Index Sensing in Fluorescent Whispering Gallery Mode Microspheres with Broken Symmetry.

Whispering gallery mode (WGM) resonators have become increasingly diverse in terms of both architecture and applications, especially as refractometric sensors, allowing for unprecedented levels of sensitivity. However, like every refractometric sensor, a single WGM resonator cannot distinguish temperature variations from changes in the refractive index of the surrounding environment. Here, we investigate how breaking the symmetry of an otherwise perfect fluorescent microsphere, by covering half of the resonator with a high-refractive-index (RI) glue, might enable discrimination of changes in temperature from variations in the surrounding refractive index. This novel approach takes advantage of the difference of optical pathway experienced by WGMs circulating in different equatorial planes of a single microsphere resonator, which induces mode-splitting. We investigated the influence of the surrounding RI of the microsphere on mode-splitting through an evaluation of the sphere's WGM spectrum and quality factor (Q-factor). Our results reveal that the magnitude of the mode-splitting increases as the refractive index contrast between the high-refractive-index (RI) glue and the surrounding environment increases, and that when they are equal no mode-splitting can be seen. Investigating the refractive index sensitivity of the individual sub modes resulting from the mode-splitting unveils a new methodology for RI sensing, and enables discrimination between surrounding refractive index changes and temperature changes, although it comes at the cost of an overall reduced refractive index sensitivity.

Towards rewritable multilevel optical data storage in single nanocrystals.

Novel approaches for digital data storage are imperative, as storage capacities are drastically being outpaced by the exponential growth in data generation. Optical data storage represents the most promising alternative to traditional magnetic and solid-state data storage. In this paper, a novel and energy efficient approach to optical data storage using rare-earth ion doped inorganic insulators is demonstrated. In particular, the nanocrystalline alkaline earth halide BaFCl:Sm is shown to provide great potential for multilevel optical data storage. Proof-of-concept demonstrations reveal for the first time that these phosphors could be used for rewritable, multilevel optical data storage on the physical dimensions of a single nanocrystal. Multilevel information storage is based on the very efficient and reversible conversion of Sm3+ to Sm2+ ions upon exposure to UV-C light. The stored information is then read-out using confocal optics by employing the photoluminescence of the Sm2+ ions in the nanocrystals, with the signal strength depending on the UV-C fluence used during the write step. The latter serves as the mechanism for multilevel data storage in the individual nanocrystals, as demonstrated in this paper. This data storage platform has the potential to be extended to 2D and 3D memory for storage densities that could potentially approach petabyte/cm3 levels.

Mechanochemically prepared SrFCl nanophosphor co-doped with Yb3+ and Er3+ for detecting ionizing radiation by upconversion luminescence.

We report a novel method for detecting ionizing radiation by employing the phenomenon of upconversion luminescence. Nanocrystalline SrFCl:Yb3+/Er3+ was prepared by ball-milling and characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). The photoluminescence properties of nanocrystalline SrFCl:Yb3+, SrFCl:Er3+ and SrFCl:Yb3+/Er3+ before and after X-irradiation were investigated. The results demonstrate that both Yb3+ and Er3+ ions in the SrFCl host are reduced to their divalent state upon X-ray exposure. Under 980 nm infrared excitation, SrFCl:Yb3+/Er3+ nanocrystals displayed efficient upconversion luminescence. The upconversion luminescence intensity gradually decreased with increasing X-irradiation in a double exponential fashion with rate constants of k1 = 0.08 Gy-1 and k2 = 0.01 Gy-1. In comparison with other X-ray storage phosphors, the present system shows a much higher stability of stored information since it is not subject to photobleaching in the read-out process. This is the first report on detecting ionizing radiation by upconversion luminescence, with the potential for improved read-out performance over traditional storage phosphors. Possible applications of the present phosphor include bioimaging and in vivo cell-level X-ray dose monitoring.

Monolithic mode-selective few-mode multicore fiber multiplexers.

With the capacity limits of standard single-mode optical fiber fast approaching, new technologies such as space-division multiplexing are required to avoid an Internet capacity crunch. Few-mode multicore fiber (FM-MCF) could allow for a two orders of magnitude increase in capacity by using the individual spatial modes in the different cores as unique data channels. We report the realization of a monolithic mode-selective few-mode multicore fiber multiplexer capable of addressing the individual modes of such a fiber. These compact multiplexers operate across the S + C + L telecommunications bands and were inscribed into a photonic chip using ultrafast laser inscription. They allow for the simultaneous multiplexing of the LP01, LP11a and LP11b modes of all cores in a 3-mode, 4-core fiber with excellent mode extinction ratios and low insertion losses. The devices are scalable to more modes and cores and therefore could represent an enabling technology for practical ultra-high capacity dense space-division multiplexing.

Unified theory of whispering gallery multilayer microspheres with single dipole or active layer sources.

The development of a fast and reliable whispering gallery mode (WGM) simulator capable of generating spectra that are comparable with experiment is an important step forward for designing microresonators. We present a new model for generating WGM spectra for multilayer microspheres, which allows for an arbitrary number of concentric dielectric layers, and any number of embedded dipole sources or uniform distributions of dipole sources to be modeled. The mode excitation methods model embedded nanoparticles, or fluorescent dye coatings, from which normalized power spectra with accurate representation of the mode coupling efficiencies can be derived. In each case, the emitted power is expressed conveniently as a function of wavelength, with minimal computational load. The model makes use of the transfer-matrix approach, incorporating improvements to its stability, resulting in a reliable, general set of formulae for calculating whispering gallery mode spectra. In the specific cases of the dielectric microsphere and the single-layer coated microsphere, our model simplifies to confirmed formulae in the literature.

Lasing of whispering gallery modes in optofluidic microcapillaries.

This paper demonstrates lasing of the whispering gallery modes in polymer coated optofluidic capillaries and their application to refractive index sensing. The laser gain medium used here is fluorescent Nile Red dye, which is embedded inside the high refractive index polymer coating. We investigate the refractometric sensing properties of these devices for different coating thicknesses, revealing that the high Q factors required to achieve low lasing thresholds can only be realized for relatively thick polymer coatings (in this case ≥ 800 nm). Lasing capillaries therefore tend to have a lower refractive index sensitivity, compared to non-lasing capillaries which can have a thinner polymer coating, due to the stronger WGM confinement within the polymer layer. However we find that the large improvement in signal-to-noise ratio realized for lasing capillaries more than compensates for the decreased sensitivity and results in an order-of-magnitude improvement in the detection limit for refractive index sensing.

Dispersion analysis of whispering gallery mode microbubble resonators.

This paper examines the opportunities existing for engineering dispersion in non-silica whispering gallery mode microbubble resonators, for applications such as optical frequency comb generation. More specifically, the zero dispersion wavelength is analyzed as a function of microbubble diameter and wall thickness for several different material groups such as highly-nonlinear soft glasses, polymers and crystalline materials. The zero dispersion wavelength is shown to be highly-tunable by changing the thickness of the shell. Using certain materials it is shown that dispersion equalization can be realized at interesting wavelengths such as deep within the visible or mid-infrared, opening up new possibilities for optical frequency comb generation. This study represents the first extensive analysis of the prospects of using non-silica microbubbles for nonlinear optics.

Dynamic Self-Referencing Approach to Whispering Gallery Mode Biosensing and Its Application to Measurement within Undiluted Serum.

Biosensing within complex biological samples requires a sensor that can compensate for fluctuations in the signal due to changing environmental conditions and nonspecific binding events. To achieve this, we developed a novel self-referenced biosensor consisting of two almost identically sized dye-doped polystyrene microspheres placed on adjacent holes at the tip of a microstructured optical fiber (MOF). Here self-referenced biosensing is demonstrated with the detection of Neutravidin in undiluted, immunoglobulin-deprived human serum samples. The MOF allows remote excitation and collection of the whispering gallery modes (WGMs) of the microspheres while also providing a robust and easy to manipulate dip-sensing platform. By taking advantage of surface functionalization techniques, one microsphere acts as a dynamic reference, compensating for nonspecific binding events and changes in the environment (such as refractive index and temperature), while the other microsphere is functionalized to detect a specific interaction. The almost identical size allows the two spheres to have virtually identical refractive index sensitivity and surface area, while still having discernible WGM spectra. This ensures their responses to nonspecific binding and environmental changes are almost identical, whereby any specific changes, such as binding events, can be monitored via the relative movement between the two sets of WGM peaks.

Dispersion in silica microbubble resonators.

We explore the scope for engineering dispersion in whispering gallery mode silica microbubbles for nonlinear applications, such as optical frequency comb generation. In particular, the zero dispersion wavelength is shown to be highly tunable by changing the thickness of the shell. Using a small diameter and small wall thickness, dispersion equalization within the visible is predicted. This opens up the possibility of realizing visible frequency combs for a range of different applications.