Optical binding in nanoparticle assembly: Potential energy landscapes

Optical binding is an optomechanical effect exhibited by systems of micro- and nanoparticles, suitably irradiated with off-resonance laser light. Physically distinct from standing-wave and other forms of holographic optical traps, the phenomenon arises as a result of an interparticle coupling with individual radiation modes, leading to optically induced modifications to Casmir-Polder interactions. To better understand how this mechanism leads to the observed assemblies and formation of patterns in nanoparticles, we develop a theory in terms of optically induced energy landscapes exhibiting the three-dimensional form of the potential energy field. It is shown in detail that the positioning and magnitude of local energy maxima and minima depend on the configuration of each particle pair, with regards to the polarization and wave vector of the laser light. The analysis reveals how the positioning of local minima determines the energetically most favorable locations for the addition of a third particle to each equilibrium pair. It is also demonstrated how the result of such an addition subtly modifies the energy landscape that will, in turn, determine the optimum location for further particle additions. As such, this development represents a rigorous and general formulation of the theory, paving the way toward full comprehension of nanoparticle assembly based on optical binding

A retarded coupling approach to intermolecular interactions

A wide range of physical phenomena such as optical binding and resonance energy transfer involve electronic coupling between adjacent molecules. A quantum electrodynamical description of these intermolecular interactions reveals the presence of retardation effects. The clarity of the procedure associated with the construction of the quantum amplitudes and the precision of the ensuing results for observable energies and rates are widely acknowledged. However, the length and complexity of the derivations involved in such quantum electrodynamical descriptions increase rapidly with the order of the process under study. Whether through the use of time-ordering approaches, or the more expedient state-sequence method, time-consuming calculations cannot usually be bypassed. A simple and succinct method is now presented, which provides for a direct and still entirely rigorous determination of the quantum electrodynamical amplitudes for processes of arbitrarily high order. Using the approach, new results for optical binding in two- and three-particle systems are secured and discussed

Circular dichroism of cholesteric polymers and the orbital angular momentum of light

We explore experimentally if the light's orbital angular momentum (OAM) interacts with chiral nematic polymer films. Specifically, we measure the circular dichroism of such a material using light beams with different OAM. We investigate the case of strongly focussed, non-paraxial light beams, where the spatial and polarization degrees of freedom are coupled. Within the experimental accuracy, we cannot find any influence of the OAM on the circular dichroism of the cholesteric polymer.Comment: 3 pages, 4 figure

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

Local coherence and the temporal development of second harmonic emission

In a variety of mesoscopically disordered systems, high levels of optical excitation resulting from pulsed laser irradiation can establish optical coherence within separate particles or locally ordered domains, leading to second harmonic emission whose temporal signature characterizes the decay of the excited state population. Examples of such systems will include colloids, cell and membrane suspensions, and many plastics, glasses and other modern materials. With pulsed excitation of sufficient intensity to elicit the onset of saturation, second harmonic emission on the throughput of a subsequent probe beam exhibits a characteristic decay and recovery. Detailed calculations show that such features arise not only in systems whose optical response involves two discrete levels, but also in systems of considerably greater electronic complexity. Deconvolution of the temporal trace of the harmonic signal serves as an independent means of monitoring the decay of the excited state. The extent of recovery in the harmonic signal also serves to register the extent of local coherence, and hence in many systems the localization of structural order. Finally, the principles introduced in the theory are shown to be applicable to other types of system such as certain photochromic materials

Influence of the state of light on the optically induced interparticle interaction

A general expression for the energy of interparticle interaction induced by an arbitrary mode of light is determined using quantum electrodynamics, and it is shown that the Casimir-Polder potential is included within this quantum result. Equations are also derived for the corresponding coupling induced by multimode number states of light, and the dependence of the pair energy on the Poynting vector and polarization state is determined. Attention is then focused on the interactions between particles trapped in counterpropagating coherent beams, both with and without interference, and it is shown that the results afford insights into the multiparticle structures that can be optically fabricated with counterpropagating input. Brief consideration is also given to the effect of squeezing the optical coherent state. Extending previous studies of optical binding in Laguerre-Gaussian beams, results are given for the case of particles trapped at radially different locations within the beam structure. Finally, consideration is given to interparticle interactions induced by broadband light, and it is shown how the length of optically fabricated particle chains can be controlled by the use of wavelength filters

A back-to-front derivation: the equal spacing of quantum levels is a proof of simple harmonic oscillator physics

The dynamical behaviour of simple harmonic motion can be found in numerous natural phenomena. Within the quantum realm of atomic, molecular and optical systems, two main features are associated with harmonic oscillations: a finite ground-state energy and equally spaced quantum energy levels. Here it is shown that there is in fact a one-to-one mapping between the provision of equally spaced quantum energy levels and simple harmonic motion. The analysis establishes that the Hamiltonian of any system featuring quantized energy levels in an evenly spaced, infinite set must have a quadratic dependence on a pair of canonically conjugate variables. Moreover, specific physical inferences can be drawn. For example, exploiting this 'back-to-front' derivation, and based on the known existence of photons, it can be proved that an electromagnetic energy density is quadratic in both the electric and magnetic fields