Structured light, transmission, and scattering

Numerous theoretical and experimental studies have established the principle that beams conveying orbital angular momentum offer a rich scope for information transfer. However, it is not clear how far it is practicable to operate such a concept at the single-photon level - especially when such a beam propagates through a system in which scattering can occur. In cases where scattering leads to photon deflection, it produces losses; however in terms of the retention of information content, there should be more concern over forward scattering. Based on a quantum electrodynamical formulation of theory, this paper aims to frame and resolve the key issues. A quantum amplitude is constructed for the representation of single and multiple scattering events in the propagation an individual photon, from a suitably structured beam. The analysis identifies potential limitations of principle, undermining complete fidelity of quantum information transmission

Limitations and improvements upon the two-level approximation for molecular nonlinear optics

When parametric nonlinear processes are employed in the cause of efficient optical frequency conversion, the media involved are generally subjected to substantially off-resonant input radiation. As such, it is usually only electronic ground states of the conversion material that are significantly populated; higher levels are engaged only in the capacity of virtual states, and it is frequently assumed that just one such state dominates in determining the response. Calculating the nonlinear optical susceptibilities of molecules on this basis, excluding all but the ground and one excited state in a sum-over-states formulation, signifies the adoption of a two-level model, a technique that is widely deployed in the calculation and analysis of nonlinear optical properties. The two-level model offers tractable and physically simple representations of molecular response, including wavelength dependence; it is also the origin of the widely applied 'push-pull' approach to designing optically nonlinear chromophores. By contrast, direct ab initio calculations of optical susceptibility are commonly frustrated by a complete failure to determine such dispersion features. However, caution is required; the two-level model can deliver potentially misleading results if it is applied without regard to the criteria for its validity, especially when molecular excited states are significantly populated. On the basis of a precise, quantum electrodynamical basis for the theory, we explore in detail why there are grounds for questioning the general validity of two-level calculations in nonlinear optics; we assess the criteria for high frequency conversion efficiency and provide a new graphical method to assist in determining the applicability of a two-level model for hyperpolarizability calculations. Lastly, this paper also explores the applicability and detailed conditions for the two-level model for electronically excited molecules, identifying problematic results and providing tractable methods for improving the accuracy of calculations on real molecule-photon interactions

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

Configuring the cancellation of optical near-fields

The characteristic near-field behavior of electromagnetic fields is open to a variety of interpretations. In a classical sense the term 'near-field' can be taken to signify a region, sufficiently close to some primary or secondary source, that the onset of retardation features is insignificant; a quantum theoretic explanation might focus more on the large momentum uncertainty that operates at small distances. Together, both near-field and wave-zone (radiative) features are fully accommodated in a retarded resonance propagation tensor, within which each component individually represents one asymptotic limit - alongside a third term that is distinctly operative at distances comparable to the optical wavelength. The propagation tensor takes different forms according to the level of multipole involved in the signal production and detection. In this presentation the nature and symmetry properties of the retarded propagation tensor are explored with reference to various forms of electric interaction, and it is shown how a suitable arrangement of optical beams can lead to the complete cancellation of near-fields. The conditions for such behavior are fully determined and some important optical trapping applications are discussed

Optically induced multi-particle structures: multi-dimensional energy landscapes

Recent quantum electrodynamical studies on optically induced inter-particle potential energy surfaces have revealed unexpected features of considerable intricacy. The exploitation of these features presents a host of opportunities for the optical fabrication of nanoscale structures, based on the fine control of a variety of attractive and repulsive forces, and the torques that operate on particle pairs. Here we report an extension of these studies, exploring the first detailed potential energy surfaces for a system of three particles irradiated by a polarized laser beam. Such a system is the key prototype for developing generic models of multi-particle complexity. The analysis identifies and characterizes potential points of stability, as well as forces and torques that particles experience as a consequence of the electromagnetic fields, generated by optical perturbations. Promising results are exhibited for the optical fabrication of assemblies of molecules, nanoparticles, microparticles, and colloidal multi-particle arrays. The comprehension of mechanism that is emerging should help determine the fine principles of multi-particle optical assembly