Advanced electrodynamic mechanisms for the nanoscale control of light by light

The laser-induced intermolecular force that exists between two or more particles subjected to a moderately intense laser beam is termed ‘optical binding’. Completely distinct from the single-particle forces that give rise to optical trapping, the phenomenon of optical binding is a manifestation of the coupling between optically induced dipole moments in neutral particles. In conjunction with optical trapping, the optomechanical forces in optical binding afford means for the manipulation and fabrication of optically bound matter. The Casimir-Polder potential that is intrinsic to all matter can be overridden by the optical binding force in cases where the laser beam is of sufficient intensity. Chiral discrimination can arise when the laser input has a circular polarization, if the particles are themselves chiral. Then, it emerges that the interaction between particles with a particular handedness is responsive to the left- or right-handedness of the light. The present analysis, which expands upon previous studies of chiral discrimination in optical binding, identifies a novel mechanism that others have previously overlooked, signifying that the discriminatory effect is much more prominent than originally thought. The new theory leads to results for freely-tumbling chiral particles subjected to circularly polarized light. Rigorous conditions are established for the energy shifts to be non-zero and display discriminatory effects with respect to the handedness of the incident beam. Detailed calculations indicate that the energy shift is larger than those previously reported by three orders of magnitude

Nonlinear optical techniques for improved data capture in fluorescence microscopy and imaging

Multiphoton fluorescence microscopy is now a well-established technique, currently attracting much interest across all fields of biophysics - especially with regard to enhanced focal resolution. The fundamental mechanism behind the technique, identified and understood through the application of quantum theory, reveals new optical polarization features that can be exploited to increase the information content of images from biological samples. In another development, based on a newly discovered, fundamentally related mechanism, it emerges the passage of off-resonant probe laser pulses may characteristically modify the intensity of single-photon fluorescence, and its associated optical polarization behavior. Here, the probe essentially confers optical nonlinearity on the decay transition, affording a means of optical control over the fluorescent emission. Compared to a catalogue of other laser-based techniques widely used in the life sciences, most suffer limitations reflecting the exploitation of specifically lifetime-associated features; the new optical control mechanism promises to be more generally applicable for the determination of kinetic data. Again, there is a prospect of improving spatial resolution, non-intrusively. It is anticipated that tight directionality can be imposed on single-photon fluorescence emission, expediting the development of new imaging applications. In addition, varying the optical frequency of the probe beam can add another dimension to the experimental parameter space. This affords a means of differentiating between molecular species with strongly overlapping fluorescence spectra, on the basis of their differential nonlinear optical properties. Such techniques significantly extend the scope and the precision of spatial and temporal information accessible from fluorescence studies

Surface functionalized spherical nanoparticles: an optical assessment of local chirality

Electromagnetic radiation propagating through any molecular system typically experiences a characteristic change in its polarization state as a result of light-matter interaction. Circularly polarized light is commonly absorbed or scattered to an extent that is sensitive to the incident circularity, when it traverses a medium whose constituents are chiral. This research assesses specific modifications to the properties of circularly polarized light that arise on passage through a system of surface-functionalized spherical nanoparticles, through the influence of chiral molecules on their surfaces. Non-functionalized nanospheres of atomic constitution are usually inherently achiral, but can exhibit local chirality associated with such surface-bound chromophores. The principal result of this investigation is the quantification of functionally conferred nanoparticle chirality, manifest through optical measurements such as circularly polarized emission. The relative position of chiral chromophores fixed to a nanoparticle sphere are first determined by means of spherical coverage co-ordinate analysis. The total electromagnetic field received by a spatially fixed, remote detector is then determined. It is shown that bound chromophores will accommodate both electric and magnetic dipole transition moments, whose scalar product represents the physical and mathematical origin of chiral properties identified in the detected signal. The analysis concludes with discussion of the magnitude of circular differential optical effects, and their potential significance for the characterization of surface-functionalized nanoparticles

London force and energy transportation between interfacial surfaces

With appropriately selected optical frequencies, pulses of radiation propagating through a system of chemically distinct and organized components can produce areas of spatially selective excitation. This paper focuses on a system in which there are two absorptive components, each one represented by surface adsorbates arrayed on a pair of juxtaposed interfaces. The adsorbates are chosen to be chemically distinct from the material of the underlying surface. On promotion of any adsorbate molecule to an electronic excited state, its local electronic environment is duly modified, and its London interaction with nearest neighbor molecules becomes accommodated to the new potential energy landscape. If the absorbed energy then transfers to a neighboring adsorbate of another species, so that the latter acquires the excitation, the local electronic environment changes and compensating motion can be expected to occur. Physically, this is achieved through a mechanism of photon absorption and emission by molecular pairs, and by the engagement of resonance transfer of energy between them. This paper presents a detailed analysis of the possibility of optically effecting such modifications to the London force between neutral adsorbates, based on quantum electrodynamics (QED). Thus, a precise link is established between the transfer of excitation and ensuing mechanical effects

Static and dynamic modifications to photon absorption:The effects of surrounding chromophores

This Letter investigates the influence, on the molecular absorption of light, of surrounding chromophores. Two novel rate contributions are identified - one vanishing for a medium with no static dipole moment. The other, dynamic term is used to model a system of primary absorbers and secondary chromophores distributed in a host medium. Further modification provides a basis for modelling a case where the medium is, itself, marginally absorptive, thus accounting for optical losses as the input propagates through the surrounding host. The results facilitate tailoring of secondary chromophore and host effects in the pursuit of materials with specific absorption features

On the interactions between molecules in an off-resonant laser beam:Evaluating the response to energy migration and optically induced pair forces

Electronically excited molecules interact with their neighbors differently from their ground-state counterparts. Any migration of the excitation between molecules can modify intermolecular forces, reflecting changes to a local potential energy landscape. It emerges that throughput off-resonant radiation can also produce significant additional effects. The context for the present analysis of the mechanisms is a range of chemical and physical processes that fundamentally depend on intermolecular interactions resulting from second and fourth-order electric-dipole couplings. The most familiar are static dipole-dipole interactions, resonance energy transfer (both second-order interactions), and dispersion forces (fourth order). For neighboring molecules subjected to off-resonant light, additional forms of intermolecular interaction arise in the fourth order, including radiation-induced energy transfer and optical binding. Here, in a quantum electrodynamical formulation, these phenomena are cast in a unified description that establishes their inter-relationship and connectivity at a fundamental level. Theory is then developed for systems in which the interplay of these forms of interaction can be readily identified and analyzed in terms of dynamical behavior. The results are potentially significant in Förster measurements of conformational change and in the operation of microelectromechanical and nanoelectromechanical devices. © 2009 American Institute of Physics

Dynamics of the dispersion interaction in an energy transfer system

On the propagation of resonant radiation through an optically dense system, photon capture is commonly followed by one or more near-field transfers of the resulting optical excitation. The process invokes secondary changes to the local electronic environment, shifting the electromagnetic interactions between participant chromophores and producing modified intermolecular forces. From the theory it emerges that energy transfer, when it occurs between chromophores with electronically dissimilar properties, can itself generate significant changes in the intermolecular potentials. This report highlights specific effects that can be anticipated when laser light propagates across an interface between differentially absorbing components in a model energy transfer system

Signatures of material and optical chirality:Origins and measures

Chirality in materials and light is of abiding interest across a broad range of scientific disciplines. This article discusses present and emerging issues in relation to molecular and optical chirality, also including some important developments in chiral metamaterials. Quantifying the chirality of matter or light leads to issues concerning the most appropriate measures, such as a helicity parameter for specific chiral chromophores and technical measures of light chirality. An optical helicity and chirality density depend on a difference between the numbers of left- and right-handed photons in a beam. In connection with circularly polarized luminescence, adoption of the Stokes parameter to spontaneous emission from chiral molecules invites critical attention. Modern spectroscopic techniques are often based on the different response arising from left-handed circularly polarized light compared to right-handed light. This dissimilarity can be exploited as a foundation for the separation of chiral molecules, promising new avenues of application

Point source generation of chiral fields:measures of near- and far-field optical helicity

To consider the relationship between different measures of chirality in an optical field, the simplest case is considered: direct spontaneous emission of circularly polarized light by a point source. In the electromagnetic fields radiated from a suitably chiral source, such as a low-symmetry chiral molecule undergoing radiative decay, optical helicity is exhibited in the extent of a difference in left- and right-handed circular polarization components. There are several practical measures for quantifying the emergence of ensuing optical helicity, exhibiting different forms of dependence on the properties of the emitter and the positioning of a detector. By casting each measure in terms of an irreducible helicity density, connections and distinctions can be drawn between results expressible in either classical or quantum form

Computing and Diagnosing Changes in Unit Test Energy Consumption

Many developers have reason to be concerned with with power consumption. For example, mobile app developers want to minimize how much power their applications draw, while still providing useful functionality. However, developers have few tools to get feedback about changes to their application\u27s power consumption behavior as they implement an application and make changes to it over time. We present a tool that, using a team\u27s existing test cases, performs repeated measurements of energy consumption based on instructions executed, objects generated, and blocking latency, generating a distribution of energy use estimates for each test run, recording these distributions in a time series of distributions over time. Then, when these distributions change substantially, we inform the developer of this change, and offer them diagnostic information about the elements of their code potentially responsible for the change and the inputs responsible. Through this information, we believe that developers will be better enabled to relate recent changes in their code to changes in energy consumption, enabling them to better incorporate changes in software energy consumption into their software evolution decisions