Quantum issues with structured light

Descriptions of optical beams with structured wavefronts or vector polarizations are widely cast in terms of classical field theory. The corresponding fully quantum counterparts often present new insights into what is physically observed, and they are especially of interest when tackling issues such as entanglement. Similarly, when determining angular momentum densities, it appears that the separate roles of photon spin and beam topological charge can only be satisfactorily addressed within a quantum framework. In some such respects, the quantum versions of theory might be considered to introduce an additional layer of complexity; in others, they can clearly and very substantially simplify the theoretical representation. At the photon level, the fully quantized descriptions of topologically structured and singular beams nonetheless raise important fundamental questions and puzzles, whose resolution continue to invite attention. Many of the mechanistic interpretations and predictions (those that appear to be supported by a true congruence between classic and quantum optical descriptions, essentially conflating electromagnetic field and state wavefunction concepts) can lead to theoretical pitfalls. This paper highlights some physical implications that emerge from a fully quantum treatment of theory

Can seasonal and interannual variation in landscape CO2 fluxes be detected by atmospheric observations of CO2 concentrations made at a tall tower?

The coupled numerical weather model WRF-SPA (Weather Research and Forecasting model and Soil-Plant-Atmosphere model) has been used to investigate a 3 yr time series of observed atmospheric CO₂ concentrations from a tall tower in Scotland, UK. Ecosystem-specific tracers of net CO₂ uptake and net CO₂ release were used to investigate the contributions to the tower signal of key land covers within its footprint, and how contributions varied at seasonal and interannual timescales. In addition, WRF-SPA simulated atmospheric CO₂ concentrations were compared with two coarse global inversion models, CarbonTrackerEurope and the National Oceanic and Atmospheric Administration's CarbonTracker (CTE-CT). WRF-SPA realistically modelled both seasonal (except post harvest) and daily cycles seen in observed atmospheric CO₂ at the tall tower (<i>R</i>² = 0.67, rmse = 3.5 ppm, bias = 0.58 ppm). Atmospheric CO₂ concentrations from the tall tower were well simulated by CTE-CT, but the inverse model showed a poorer representation of diurnal variation and simulated a larger bias from observations (up to 1.9 ppm) at seasonal timescales, compared to the forward modelling of WRF-SPA. However, we have highlighted a consistent post-harvest increase in the seasonal bias between WRF-SPA and observations. Ecosystem-specific tracers of CO₂ exchange indicate that the increased bias is potentially due to the representation of agricultural processes within SPA and/or biases in land cover maps. The ecosystem-specific tracers also indicate that the majority of seasonal variation in CO₂ uptake for Scotland's dominant ecosystems (forests, cropland and managed grassland) is detectable in observations within the footprint of the tall tower; however, the amount of variation explained varies between years. The between years variation in detectability of Scotland's ecosystems is potentially due to seasonal and interannual variation in the simulated prevailing wind direction. This result highlights the importance of accurately representing atmospheric transport used within atmospheric inversion models used to estimate terrestrial source/sink distribution and magnitude

Can Intrusion Detection Implementation be Adapted to End-User Capabilities?

In an environment where technical solutions for securing networked systems are commonplace, there still exist problems in implementation of such solutions f or home and small business users. One component of this protection is the use of intrusion detection systems. Intrusion detection monitors network traffic for suspicious activity, performs access blocking and alerts the system administrator or user of potential attacks. This paper reviews the basic function of intrusion detection systems and maps them to an existing end-llser capability framework. Using this framework, implementation guidance and systematic improvement in implementation of this security measure are defined

Optical vortex mode generation by nanoarrays with a tailored geometry

Light generated with orbital angular momentum, commonly known as an optical vortex, is widely achieved by modifying the phase structure of a conventional laser beam through the utilization of a suitable optical element. In recent research, a process has been introduced that can produce electromagnetic radiation with a helical wave-front directly from a source. The chirally driven optical emission originates from a hierarchy of tailored nanoscale chromophore arrays arranged with a specific propeller-like geometry and symmetry. In particular, a nanoarray composed of n particles requires each component to be held in a configuration with a rotation and associated phase shift of 2 π/n radians with respect to its neighbor. Following initial electronic excitation, each such array is capable of supporting delocalized doubly degenerate excitons, whose azimuthal phase progression is responsible for the helical wave-front. Under identified conditions, the relaxation of the electronically-excited nanoarray produces structured light in a spontaneous manner. Nanoarrays of escalating order, i.e. those containing an increasing number of components, enable access to a set of topological charges of higher order. Practical considerations for the development of this technique are discussed, and potential new applications are identified. © (2014) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE)

Chiral nanoemitter array: A launchpad for optical vortices

A chiral arrangement of molecular nanoemitters is shown to support delocalised exciton states whose spontaneous decay can generate optical vortex radiation. In contrast to techniques in which phase modification is imposed upon conventional optical beams, this exciton method enables radiation with a helical wave-front to be produced directly. To achieve this end, a number of important polarisation and symmetry-based criteria need to be satisfied. It emerges that the phase structure of the optical field produced by degenerate excitons in a propeller-shaped array can exhibit precisely the sought character of an optical vortex – one with unit topological charge. Practical considerations for the further development of this technique are discussed, and potential new applications are identified

Expanded horizons for generating and exploring optical angular momentum in vortex structures

Spin provides for a well-known extension to the information capacity of nanometer-scale electronic devices. Spin transfer can be effected with high fidelity between quantum dots, this type of emission being primarily associated with emission dipoles. However, in seeking to extend the more common spectroscopic connection of dipole transitions with orbital angular momentum, it has been shown impossible to securely transmit information on any other multipolar basis – partly because point detectors are confined to polarization measurement. Standard polarization methods in optics provide for only two independent degrees of freedom, such as the circular states of opposing handedness associated with photon spin. Complex light beams with structured wave-fronts or vector polarization do, however, offer a basis for additional degrees of freedom, enabling individual photons to convey far more information content. A familiar example is afforded by Laguerre-Gaussian modes, whose helically twisted wave-front and vortex fields are associated with orbital angular momentum. Each individual photon in such a beam has been shown to carry the entire spatial helical-mode information, supporting an experimental basis for sorting beams of different angular momentum content. One very recent development is a scheme for such optical vortices to be directly generated through electronic relaxation processes in structured molecular chromophore arrays. © (2013) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE)

Symmetry analysis of Raman scattering mediated by neighboring molecules

Raman spectroscopy is a key technique for the identification and structural interrogation of molecules. It generally exploits changes in vibrational state within individual molecules which produce, in the scattered light, frequencies that are absent in the incident light. Considered as a quantum optical process, each Raman scattering event involves the concurrent annihilation and creation of photons of two differing radiation modes, accompanying vibrational excitation or decay. For molecules of sufficiently high symmetry, certain transitions may be forbidden by the two-photon selection rules, such that corresponding frequency shifts may not appear in the scattered light. By further developing the theory on a formal basis detailed in other recent work [J. Chem. Phys. 144, 174304 (2016)], the present analysis now addresses cases in which expected selection rule limitations are removed as a result of the electronic interactions between neighboring molecules. In consequence, new vibrational lines may appear – even some odd parity (ungerade) vibrations may then participate in the Raman process. Subtle differences arise according to whether the input and output photon events occur at either the same or different molecules, mediated by intermolecular interactions. For closely neighboring molecules, within near-field displacement distances, it emerges that the radiant intensity of Raman scattering can have various inverse-power dependences on separation distance. A focus is given here to the newly permitted symmetries, and the results include an extended list of irreducible representations for each point group in which such behavior can arise

Hyper-Rayleigh scattering in centrosymmetric systems

Hyper-Rayleigh scattering (HRS) is an incoherent mechanism for optical second harmonic generation. The frequency-doubled light that emerges from this mechanism is not emitted in a laser-like manner, in the forward direction; it is scattered in all directions. The underlying theory for this effect involves terms that are quadratic in the incident field and involves an even-order optical susceptibility (for a molecule, its associated hyperpolarizability). In consequence, HRS is often regarded as formally forbidden in centrosymmetric media. However, for the fundamental three-photon interaction, theory based on the standard electric dipole approximation, representable as E13, does not account for all experimental observations. The relevant results emerge upon extending the theory to include E12M1 and E12E2 contributions, incorporating one magnetic dipolar or electric quadrupolar interaction, respectively, to a consistent level of multipolar expansion. Both additional interactions require the deployment of higher orders in the multipole expansion, with the E12E2 interaction analogous in rank and parity to a four-wave susceptibility. To elicit the correct form of response from fluid or disordered media invites a tensor representation which does not oversimplify the molecular components, yet which can produce results to facilitate the interpretation of experimental observations. The detailed derivation in this work leads to results which are summarized for the following: perpendicular detection of polarization components both parallel and perpendicular to the pump radiation, leading to distinct polarization ratio results, as well as a reversal ratio for forward scattered circular polarizations. The results provide a route to handling data with direct physical interpretation, to enable the more sophisticated design of molecules with sought nonlinear optical properties