Laser-controlled fluorescence in two-level systems

The ability to modify the character of fluorescent emission by a laser-controlled, optically nonlinear process has recently been shown theoretically feasible, and several possible applications have already been identified. In operation, a pulse of off-resonant probe laser beam, of sufficient intensity, is applied to a system exhibiting fluorescence, during the interval of excited- state decay following the initial excitation. The result is a rate of decay that can be controllably modified, the associated changes in fluorescence behavior affording new, chemically specific information. In this paper, a two-level emission model is employed in the further analysis of this all-optical process; the results should prove especially relevant to the analysis and imaging of physical systems employing fluorescent markers, these ranging from quantum dots to green fluorescence protein. Expressions are presented for the laser-controlled fluorescence anisotropy exhibited by samples in which the fluorophores are randomly oriented. It is also shown that, in systems with suitably configured electronic levels and symmetry properties, fluorescence emission can be produced from energy levels that would normally decay nonradiatively. © 2010 American Chemical Society

Influence of biomass combustion emissions on the distribution of acidic trace gases over the southern Pacific basin during austral springtime

This paper describes the large-scale distributions of HNO3, HCOOH, and CH3COOH over the central and South Pacific basins during the Pacific Exploratory Mission-Tropics (PEM-Tropics) in austral springtime. Because of the remoteness of this region from continental areas, low part per trillion by volume (pptv) mixing ratios of acidic gases were anticipated to be pervasive over the South Pacific basin. However, at altitudes of 2–12 km over the South Pacific, air parcels were encountered frequently with significantly enhanced mixing ratios (up to 1200 pptv) of acidic gases. Most of these air parcels were centered in the 3–7 km altitude range and occurred within the 15°−65°S latitudinal band. The acidic gases exhibited an overall general correlation with CH3Cl, PAN, and O3, suggestive of photochemical and biomass burning sources. There was no correlation or trend of acidic gases with common industrial tracer compounds (e.g., C2Cl4 or CH3CCl3). The combustion emissions sampled over the South Pacific basin were relatively aged exhibiting C2H2/CO ratios in the range of 0.2–2.2 pptv/ppbv. The relationships between acidic gases and this ratio were similar to what was observed in aged air parcels (i.e., \u3e3–5 days since they were over a continental area) over the western North Pacific during the Pacific Exploratory Mission-West Phases A and B (PEM-West A and B). In the South Pacific marine boundary layer a median C2H2/CO ratio of 0.6 suggested that this region was generally not influenced by direct inputs of biomass combustion emissions. Here we observed the lowest mixing ratios of acidic gases, with median values of 14 pptv for HNO3, 19 pptv for HCOOH, and 18 pptv for CH3COOH. These values were coincident with low mixing ratios of NOx(\u3c10 pptv), CO (≈50 parts per billion by volume (ppbv)), O3 (\u3c 20 ppbv), and long-lived hydrocarbons (e.g., C2H6 \u3c300 pptv). Overall, the PEM-Tropics data suggest an important influence of aged biomass combustion emissions on the distributions of acidic gases over the South Pacific basin in austral springtime

A photonic basis for deriving nonlinear optical response

Nonlinear optics is generally first presented as an extension of conventional optics. Typically the subject is introduced with reference to a classical oscillatory electric polarization, accommodating correction terms that become significant at high intensities. The material parameters that quantify the extent of the nonlinear response are cast as coefficients in a power series - nonlinear optical susceptibilities signifying a propensity to generate optical harmonics, for example. Taking the subject to a deeper level requires a more detailed knowledge of the structure and properties of each nonlinear susceptibility tensor, the latter differing in form according to the process under investigation. Typically, the derivations involve intricate development based on time-dependent perturbation theory, assisted by recourse to a set of Feynman diagrams. This paper presents a more direct route to the required results, based on photonic rather than semiclassical principles, and offers a significantly clearer perspective on the photophysics underlying nonlinear optical response. The method, here illustrated by specific application to harmonic generation and down-conversion processes, is simple, intuitive and readily amenable for processes of arbitrary photonic order. © 2009 IOP Publishing Ltd

Chiral discrimination in optical trapping and manipulation

When circularly polarized light interacts with chiral molecules or nanoscale particles powerful symmetry principles determine the possibility of achieving chiral discrimination, and the detailed form of electrodynamic mechanisms dictate the types of interaction that can be involved. The optical trapping of molecules and nanoscale particles can be described in terms of a forward-Rayleigh scattering mechanism, with trapping forces being dependent on the positioning within the commonly non-uniform intensity beam profile. In such a scheme, nanoparticles are commonly attracted to local potential energy minima, ordinarily towards the centre of the beam. For achiral particles the pertinent material response property usually entails an electronic polarizability involving transition electric dipole moments. However, in the case of chiral molecules, additional effects arise through the engagement of magnetic counterpart transition dipoles. It emerges that, when circularly polarized light is used for the trapping, a discriminatory response can be identified between left- and right-handed polarizations. Developing a quantum framework to accurately describe this phenomenon, with a tensor formulation to correctly represent the relevant molecular properties, the theory leads to exact analytical expressions for the associated energy landscape contributions. Specific results are identified for liquids and solutions, both for isotropic media and also where partial alignment arises due to a static electric field. The paper concludes with a pragmatic analysis of the scope for achieving enantiomer separation by such methods

Optically induced forces and torques:Interactions between nanoparticles in a laser beam

Distinctive optical forces and torques arise between nanoparticles irradiated by intense laser radiation. These forces, associated with a pairwise process of stimulated scattering, prove to enable the possibility of producing significant modifications to both the form and magnitude of interparticle forces, with additional contributions arising in the case of dipolar materials. Moreover, such forces have the capacity to generate unusual patterns of nanoscale response, entirely controlled by the input beam characteristics- principally the optical frequency, intensity, and polarization. Based on quantum electrodynamical theory, a general result is secured for the laser-induced force under arbitrary conditions, incorporating both static and dynamic coupling mechanisms. Specific features of the results are identified for pairs of particles with prolate cylindrical symmetry, e.g., carbon nanotubes, where it is shown that the laser-induced forces and torques are sensitive functions of the pair spacing and orientation, and the laser beam geometry; significantly, they can be either repulsive or attractive according to conditions. For nanoparticles trapped in a Laguerre-Gaussian laser beam the results also reveal additional and highly distinctive torques that suggest further possibilities for nanomanipulation with light. The paper concludes with a discussion on several potential applications of such forces. © 2005 The American Physical Society

Synthesis of folic acid functionalized gold nanoclusters for targeting folate receptor-positive cells

We report on the synthesis of water-soluble gold nanoclusters capped with polyethylene glycol (PEG)-based ligands and further functionalized with folic acid for specific cellular uptake. The dihydrolipoic acid-PEG-based ligands terminated with -OMe, -NH2 and -COOH functional groups are produced and used for surface passivation of Au nanoclusters (NCs) with diameters <2 nm. The produced sub 2 nm Au NCs possess long-shelf life and are stable in physiologically relevant environments (temperature and pH), are paramagnetic and biocompatible. The paramagnetism of Au NCs in solution is also reported. The functional groups on the capping ligands are used for direct conjugation of targeting molecules onto Au NCs without the need for post synthesis modification. Folic acid (FA) is attached via an amide group and effectively target cells expressing the folate receptor. The combination of targeting ability, biocompatibility and paramagnetism in FA-functionalized Au NCs is of relevance for their exploitation in nanomedicine for targeted imaging

Phase Transitions and Oscillations in a Lattice Prey-Predator Model

A coarse grained description of a two-dimensional prey-predator system is given in terms of a 3-state lattice model containing two control parameters: the spreading rates of preys and predators. The properties of the model are investigated by dynamical mean-field approximations and extensive numerical simulations. It is shown that the stationary state phase diagram is divided into two phases: a pure prey phase and a coexistence phase of preys and predators in which temporal and spatial oscillations can be present. The different type of phase transitions occuring at the boundary of the prey absorbing phase, as well as the crossover phenomena occuring between the oscillatory and non-oscillatory domains of the coexistence phase are studied. The importance of finite size effects are discussed and scaling relations between different quantities are established. Finally, physical arguments, based on the spatial structure of the model, are given to explain the underlying mechanism leading to oscillations.Comment: 11 pages, 13 figure

Space Qualification of the Optical Filter Assemblies for the ICESat-2/ATLAS Instrument

The Advanced Topographic Laser Altimeter System (ATLAS) will be the only instrument on the Ice, Cloud, and Land Elevation Satellite -2 (ICESat-2). ICESat-2 is the 2nd-generation of the orbiting laser altimeter ICESat, which will continue polar ice topography measurements with improved precision laser-ranging techniques. In contrast to the original ICESat design, ICESat-2 will use a micro-pulse, multi-beam approach that provides dense cross-track sampling to help scientists determine a surface's slope with each pass of the satellite. The ATLAS laser will emit visible, green laser pulses at a wavelength of 532 nm and a rate of 10 kHz and will be split into 6 beams. A set of six identical, thermally tuned optical filter assemblies (OFA) will be used to remove background solar radiation from the collected signal while transmitting the laser light to the detectors. A seventh assembly will be used to monitor the laser center wavelength during the mission. In this paper, we present the design and optical performance measurements of the ATLAS OFA in air and in vacuum prior to their integration on the ATLAS instrument