Separation-dependent near-field effects in Mie scattering spectra of two optically trapped aerosol droplets.

The backscattering of ultraviolet and visible light by a model organic (squalane) aerosol droplet (1.0 View Article and Find Full Text PDF

Aqueous Radical Initiated Oxidation of an Organic Monolayer at the Air-Water Interface as a Proxy for Thin Films on Atmospheric Aerosol Studied with Neutron Reflectometry.

Neutron reflectometry has been used to study the radical initiated oxidation of a monolayer of the lipid 1,2-distearoyl--glycero-3-phosphocholine (DSPC) at the air-solution interface by aqueous-phase hydroxyl, sulfate, and nitrate radicals. The oxidation of organic films at the surface of atmospheric aqueous aerosols can influence the optical properties of the aerosol and consequently can impact Earth's radiative balance and contribute to modern climate change. The amount of material at the air-solution interface was found to decrease on exposure to aqueous-phase radicals which was consistent with a multistep degradation mechanism, i.

Molecular Self-Organization in Surfactant Atmospheric Aerosol Proxies.

ConspectusAerosols are ubiquitous in the atmosphere. Outdoors, they take part in the climate system via cloud droplet formation, and they contribute to indoor and outdoor air pollution, impacting human health and man-made environmental change. In the indoor environment, aerosols are formed by common activities such as cooking and cleaning.

Applying Optical Tweezers with TIRF Microscopy to Quantify Physical Interactions Between Organelles in the Plant Endomembrane System.

Plant organelles are associated with each other through tethering proteins at membrane contact sites (MCS). Methods such as total internal reflection fluorescence (TIRF) optical tweezers allow us to probe organelle interactions in live plant cells. Optical tweezers (focused infrared laser beams) can trap organelles that have a different refractive index to their surrounding medium (cytosol), whilst TIRF allows us to simultaneously image behaviors of organelles in the thin region of cortical cytoplasm.

In Situ Sol-Gel Synthesis of Unique Silica Structures Using Airborne Assembly: Implications for In-Air Reactive Manufacturing.

Optical trapping enables the real-time manipulation and observation of morphological evolution of individual particles during reaction chemistry. Here, optical trapping was used in combination with Raman spectroscopy to conduct airborne assembly and kinetic experiments. Micro-droplets of alkoxysilane were levitated in air prior to undergoing either acid- or base-catalyzed sol-gel reaction chemistry to form silica particles.

Mie scattering from optically levitated mixed sulfuric acid-silica core-shell aerosols: observation of core-shell morphology for atmospheric science.

Sulfuric acid is shown to form a core-shell particle on a micron-sized, optically-trapped spherical silica bead. The refractive indices of the silica and sulfuric acid, along with the shell thickness and bead radius were determined by reproducing Mie scattered optical white light as a function of wavelength in Mie spectroscopy. Micron-sized silica aerosols (silica beads were used as a proxy for atmospheric silica minerals) were levitated in a mist of sulfuric acid particles; continuous collection of Mie spectra throughout the collision of sulfuric acid aerosols with the optically trapped silica aerosol demonstrated that the resulting aerosol particle had a core-shell morphology.

Chloroplasts alter their morphology and accumulate at the pathogen interface during infection by Phytophthora infestans.

Upon immune activation, chloroplasts switch off photosynthesis, produce antimicrobial compounds and associate with the nucleus through tubular extensions called stromules. Although it is well established that chloroplasts alter their position in response to light, little is known about the dynamics of chloroplast movement in response to pathogen attack. Here, we report that during infection with the Irish potato famine pathogen Phytophthora infestans, chloroplasts accumulate at the pathogen interface, associating with the specialized membrane that engulfs the pathogen haustorium.

Singlet Exciton Fission and Associated Enthalpy Changes with a Covalently Linked Bichromophore Comprising TIPS-Pentacenes Held in an Open Conformation.

A covalently linked bichromophore, embracing 6,13-bis(triisopropylsilylethinyl)pentacene (TIPS-pentacene) terminals bridged by a rigid fluorene spacer, generates a relatively high yield (i.e., 65 ± 6%) of the spin-correlated, triplet biexciton upon illumination in toluene.

The reaction of oleic acid monolayers with gas-phase ozone at the air water interface: the effect of sub-phase viscosity, and inert secondary components.

Organic films that form on atmospheric particulate matter change the optical and cloud condensation nucleation properties of the particulate matter and consequently have implications for modern climate and climate models. The organic films are subject to attack from gas-phase oxidants present in ambient air. Here we revisit in greater detail the oxidation of a monolayer of oleic acid by gas-phase ozone at the air-water interface as this provides a model system for the oxidation reactions that occur at the air-water interface of aqueous atmospheric aerosol.

The persistence of a proxy for cooking emissions in megacities: a kinetic study of the ozonolysis of self-assembled films by simultaneous small and wide angle X-ray scattering (SAXS/WAXS) and Raman microscopy.

Cooking emissions account for a significant proportion of the organic aerosols emitted into the urban environment and high pollution events have been linked to an increased organic content on urban particulate matter surfaces. We present a kinetic study on surface coatings of self-assembled (semi-solid) oleic acid-sodium oleate cooking aerosol proxies undergoing ozonolysis. We found clear film thickness-dependent kinetic behaviour and measured the effect of the organic phase on the kinetics for this system.

Porous Carbon Microparticles as Vehicles for the Intracellular Delivery of Molecules.

In this study the application of porous carbon microparticles for the transport of a sparingly soluble material into cells is demonstrated. Carbon offers an intrinsically sustainable platform material that can meet the multiple and complex requirements imposed by applications in biology and medicine. Porous carbon microparticles are attractive as they are easy to handle and manipulate and combine the chemical versatility and biocompatibility of carbon with a high surface area due to their highly porous structure.

Using Mie Scattering to Determine the Wavelength-Dependent Refractive Index of Polystyrene Beads with Changing Temperature.

Polystyrene beads are often used as test particles in aerosol science. Here, a contact-less technique is reported for determining the refractive index of a solid aerosol particle as a function of wavelength and temperature (20-234 °C) simultaneously. Polystyrene beads with a diameter of 2 μm were optically trapped in air in the central orifice of a ceramic heating element, and Mie spectroscopy was used to determine the radius and refractive index (to precisions of 0.

Miro2 tethers the ER to mitochondria to promote mitochondrial fusion in tobacco leaf epidermal cells.

Mitochondria are highly pleomorphic, undergoing rounds of fission and fusion. Mitochondria are essential for energy conversion, with fusion favouring higher energy demand. Unlike fission, the molecular components involved in mitochondrial fusion in plants are unknown.

Preparation of polymer gold nanoparticle composites with tunable plasmon coupling and their application as SERS substrates.

The controlled surface functionalisation of polystyrene beads (200 nm) with a lipoic acid derivative is used to assemble composites with between 4 to 20% loadings of citrate stabilised gold nanoparticles (13 nm-30 nm), which exhibit variable optical properties arising from interactions of the nanoparticle surface plasmon resonance (SPR). The decrease in average interparticle distance at higher loadings results in a red-shift in the SPR wavelength, which is well described by a universal ruler equation. The composite particles are shown to act as good SERS substrates for the standard analyte 4-mercaptophenol.

Manipulation and Deposition of Complex, Functional Block Copolymer Nanostructures Using Optical Tweezers.

Block copolymer self-assembly has enabled the creation of a range of solution-phase nanostructures with applications from optoelectronics and biomedicine to catalysis. However, to incorporate such materials into devices a method that facilitates their precise manipulation and deposition is desirable. Herein we describe how optical tweezers can be used to trap, manipulate, and pattern individual cylindrical micelles and larger hybrid micellar materials.

Iridium Nanoparticles for Multichannel Luminescence Lifetime Imaging, Mapping Localization in Live Cancer Cells.

The development of long-lived luminescent nanoparticles for lifetime imaging is of wide interest as luminescence lifetime is environmentally sensitive detection independent of probe concentration. We report novel iridium-coated gold nanoparticles as probes for multiphoton lifetime imaging with characteristic long luminescent lifetimes based on iridium luminescence in the range of hundreds of nanoseconds and a short signal on the scale of picoseconds based on gold allowing multichannel detection. The tailor-made IrC complex forms stable, water-soluble gold nanoparticles (AuNPs) of 13, 25, and 100 nm, bearing 1400, 3200, and 22 000 IrC complexes per AuNP, respectively.

1064 nm Dispersive Raman Microspectroscopy and Optical Trapping of Pharmaceutical Aerosols.

Raman spectroscopy is a powerful tool for investigating chemical composition. Coupling Raman spectroscopy with optical microscopy (Raman microspectroscopy) and optical trapping (Raman tweezers) allows microscopic length scales and, hence, femtolitre volumes to be probed. Raman microspectroscopy typically uses UV/visible excitation lasers, but many samples, including organic molecules and complex tissue samples, fluoresce strongly at these wavelengths.

Dynamic viscosity mapping of the oxidation of squalene aerosol particles.

Organic aerosols (OAs) play important roles in multiple atmospheric processes, including climate change, and can impact human health. The physico-chemical properties of OAs are important for all these processes and can evolve through reactions with various atmospheric components, including oxidants. The dynamic nature of these reactions makes it challenging to obtain a true representation of their composition and surface chemistry.

Heteronuclear Ir(III)-Ln(III) Luminescent Complexes: Small-Molecule Probes for Dual Modal Imaging and Oxygen Sensing.

Luminescent, mixed metal d-f complexes have the potential to be used for dual (magnetic resonance imaging (MRI) and luminescence) in vivo imaging. Here, we present dinuclear and trinuclear d-f complexes, comprising a rigid framework linking a luminescent Ir center to one (Ir·Ln) or two (Ir·Ln2) lanthanide metal centers (where Ln = Eu(III) and Gd(III), respectively). A range of physical, spectroscopic, and imaging-based properties including relaxivity arising from the Gd(III) units and the occurrence of Ir(III) → Eu(III) photoinduced energy-transfer are presented.

Mechanical Characterization of Ultralow Interfacial Tension Oil-in-Water Droplets by Thermal Capillary Wave Analysis in a Microfluidic Device.

Measurements of the ultralow interfacial tension and surfactant film bending rigidity for micron-sized heptane droplets in bis(2-ethylhexyl) sodium sulfosuccinate-NaCl aqueous solutions were performed in a microfluidic device through the analysis of thermally driven droplet interface fluctuations. The Fourier spectrum of the stochastic droplet interface displacement was measured through bright-field video microscopy and a contour analysis technique. The droplet interfacial tension, together with the surfactant film bending rigidity, was obtained by fitting the experimental results to the prediction of a capillary wave model.

Directly interrogating single quantum dot labelled UvrA2 molecules on DNA tightropes using an optically trapped nanoprobe.

In this study we describe a new methodology to physically probe individual complexes formed between proteins and DNA. By combining nanoscale, high speed physical force measurement with sensitive fluorescence imaging we investigate the complex formed between the prokaryotic DNA repair protein UvrA2 and DNA. This approach uses a triangular, optically-trapped "nanoprobe" with a nanometer scale tip protruding from one vertex.

Fluorescence spectroscopy and microscopy as tools for monitoring redox transformations of uranium in biological systems.

We report a study of redox reactions of uranium in model conditions using luminescence spectroscopy, which with its ease and wide availability has the potential to offer new insights into a bioremediation strategy of particular interest - the enzymatic reduction of UO by bacteria such as . The inherent luminescent properties of UO have been combined with confocal fluorescence microscopy techniques and lifetime image mapping to report directly on uranium concentration, localisation and oxidation state in cellular systems during uranium bioreduction, suggesting that localisation of uranyl species on the cell membrane surface plays an important role and that extracellular biogenic features form alongside uranyl sorbed cellular species during early stages of the bioreduction. The use of confocal microscopy in tandem with lifetime image mapping offers both improved temporal and spatial resolution (nanoseconds to microseconds and sub-micron respectively) than more conventional X-ray based techniques and offers the potential to image redox reactions occurring .

Heterogeneous oxidation of nitrite anion by gas-phase ozone in an aqueous droplet levitated by laser tweezers (optical trap): is there any evidence for enhanced surface reaction?

The oxidation of nitrite anion within an aqueous atmospheric droplet may be a sink for HONO in the lower atmosphere. An optical trap with Raman spectroscopy is used to demonstrate that the oxidation of aqueous nitrite anion in levitated, micron sized, aqueous droplets by gas-phase ozone is consistent with bulk aqueous-phase kinetics and diffusion. There is no evidence of an enhanced or retarded reaction at the droplet surface at the concentrations used in the experiment or likely to be found in the atmosphere.

Determining the unique refractive index properties of solid polystyrene aerosol using broadband Mie scattering from optically trapped beads.

A method is described to measure the refractive index dispersion with wavelength of optically trapped solid particles in air. Knowledge of the refraction properties of solid particles is critical for the study of aerosol; both in the laboratory and in the atmosphere for climate studies. Single micron-sized polystyrene beads were optically trapped in air using a vertically aligned counter-propagating configuration of focussed laser beams.

Degradation and rearrangement of a lung surfactant lipid at the air-water interface during exposure to the pollutant gas ozone.

The presence of unsaturated lipids in lung surfactant is important for proper respiratory function. In this work, we have used neutron reflection and surface pressure measurements to study the reaction of the ubiquitous pollutant gas-phase ozone, O3, with pure and mixed phospholipid monolayers at the air-water interface. The results reveal that the reaction of the unsaturated lipid 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphocholine, POPC, with ozone leads to the rapid loss of the terminal C9 portion of the oleoyl strand of POPC from the air-water interface.