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)

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)

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

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

Quantum theory for the nanoscale propagation of light through stacked thin film layers

Stacked multi-layer films have a range of well-known applications as optical elements. The various types of theory commonly used to describe optical propagation through such structures rarely take account of the quantum nature of light, though phenomena such as Anderson localization can be proven to occur under suitable conditions. In recent and ongoing work based on quantum electrodynamics, it has been shown possible to rigorously reformulate, in photonic terms, the fundamental mechanisms that are involved in reflection and optical transmission through stacked nanolayers. Accounting for sum-over-pathway features in the quantum mechanical description, this theory treats the sequential interactions of photons with material boundaries in terms of individual scattering events. The study entertains an arbitrary number of reflections in systems comprising two or three internally reflective surfaces. Analytical results are secured, without recourse to FTDT (finite-difference time-domain) software or any other finite-element approximations. Quantum interference effects can be readily identified. The new results, which cast the optical characteristics of such structures in terms of simple, constituent-determined properties, are illustrated by model calculations

Raman scattering mediated by neighboring molecules

Raman scattering is most commonly associated with a change in vibrational state within individual molecules, the corresponding frequency shift in the scattered light affording a key way of identifying material structures. In theories where both matter and light are treated quantum mechanically, the fundamental scattering process is represented as the concurrent annihilation of a photon from one radiation mode and creation of another in a different mode. Developing this quantum electrodynamical formulation, the focus of the present work is on the spectroscopic consequences of electrodynamic coupling between neighboring molecules or other kinds of optical center. To encompass these nanoscale interactions, through which the molecular states evolve under the dual influence of the input light and local fields, this work identifies and determines two major mechanisms for each of which different selection rules apply. The constituent optical centers are considered to be chemically different and held in a fixed orientation with respect to each other, either as two components of a larger molecule or a molecular assembly that can undergo free rotation in a fluid medium or as parts of a larger, solid material. The two centers are considered to be separated beyond wavefunction overlap but close enough together to fall within an optical near-field limit, which leads to high inverse power dependences on their local separation. In this investigation, individual centers undergo a Stokes transition, whilst each neighbor of a different species remains in its original electronic and vibrational state. Analogous principles are applicable for the anti-Stokes case. The analysis concludes by considering the experimental consequences of applying this spectroscopic interpretation to fluid media; explicitly, the selection rules and the impact of pressure on the radiant intensity of this process

Nanoarrays for the generation of complex optical wave-forms

Light beams with unusual forms of wavefront offer a host of useful features to extend the repertoire of those developing new optical techniques. Complex, non-uniform wavefront structures offer a wide range of optomechanical applications, from microparticle rotation, traction and sorting, through to contactless microfluidic motors. Beams combining transverse nodal structures with orbital angular momentum, or vector beams with novel polarization profiles, also present new opportunities for imaging and the optical transmission of information, including quantum entanglement effects. Whilst there are numerous well-proven methods for generating light with complex wave-forms, most current methods work on the basis of modifying a conventional Hermite-Gaussian beam, by passage through suitably tailored optical elements. It has generally been considered impossible to directly generate wave-front structured beams either by spontaneous or stimulated emission from individual atoms, ions or molecules. However, newly emerged principles have shown that emitter arrays, cast in an appropriately specified geometry, can overcome the obstacles: one possibility is a construct based on the electronic excitation of nanofabricated circular arrays. Recent experimental work has extended this concept to a phase-imprinted ring of apertures holographically encoded in a diffractive mask, generated by a programmed spatial light modulator. These latest advances are potentially paving the way for creating new sources of structured light

Optical vortex generation from molecular chromophore arrays

The generation of light endowed with orbital angular momentum, frequently termed optical vortex light, is commonly achieved by passing a conventional beam through suitably constructed optical elements. This Letter shows that the necessary phase structure for vortex propagation can be directly produced through the creation of twisted light from the vacuum. The mechanism is based on optical emission from a family of chromophore nanoarrays that satisfy specific geometric and symmetry constraints. Each such array can support pairs of electronically delocalized doubly degenerate excitons whose azimuthal phase progression is responsible for the helical wave front of the emitted radiation. The exciton symmetry dictates the maximum magnitude of topological charge; detailed analysis secures the conditions necessary to deliver optical vortices of arbitrary order

Direct generation of optical vortices

A detailed scheme is established for the direct generation of optical vortices, signifying light endowed with orbital angular momentum. In contrast to common techniques based on the tailored conversion of the wave front in a conventional beam, this method provides for the direct spontaneous emission of photons with the requisite field structure. This form of optical emission results directly from the electronic relaxation of a delocalized exciton state that is supported by a ringlike array of three or more nanoscale chromophores. An analysis of the conditions leads to a general formulation revealing a requirement for the array structure to adhere to one of a restricted set of permissible symmetry groups. It is shown that the coupling between chromophores within each array leads to an energy level splitting of the exciton structure, thus providing for a specific linking of exciton phase and emission wavelength. For emission, arrays conforming to one of the given point-group families’ doubly degenerate excitons exhibit the specific phase characteristics necessary to support vortex emission. The highest order of exciton symmetry, corresponding to the maximum magnitude of electronic orbital angular momentum supported by the ring, provides for the most favored emission. The phase properties of the emission produced by the relaxation of such excitons are exhibited on plots which reveal the azimuthal phase progression around the ring, consistent with vortex emission. It is proven that emission of this kind produces electromagnetic fields that map with complete fidelity onto the phase structure of a Laguerre-Gaussian optical mode with the corresponding topological charge. The prospect of direct generation paves the way for practicable devices that need no longer rely on the modification of a conventional laser beam by a secondary optical element. Moreover, these principles hold promise for the development of a vortex laser, also based on nanoscale exciton decay, enabling the production of coherent radiation with a tailor-made helical wave front