Optically nonlinear energy transfer in light-harvesting dendrimers

Dendrimeric polymers are the subject of intense research activity geared towards their implementation in nanodevice applications such as energy harvesting systems,organic light-emitting diodes, photosensitizers, low-threshold lasers, and quantum logic elements, etc. A recent development in this area has been the construction of dendrimers specifically designed to exhibit novel forms of optical nonlinearity, exploiting the unique properties of these materials at high levels of photon flux. Starting from a thorough treatment of the underlying theory based on the principles of molecular quantum electrodynamics, it is possible to identify and characterize several optically nonlinear mechanisms for directed energy transfer and energy pooling in multichromophore dendrimers. Such mechanisms fall into two classes: first, those where two-photon absorption by individual donors is followed by transfer of the net energy to an acceptor; second, those where the excitation of two electronically distinct but neighboring donor groups is followed by a collective migration of their energy to a suitable acceptor. Each transfer process is subject to minor dissipative losses. In this paper we describe in detail the balance of factors and the constraints that determines the favored mechanism, which include the excitation statistics, structure of the energy levels, laser coherence factors, chromophore selection rules and architecture, possibilities for the formation of delocalized excitons, spectral overlap, and the overall distribution of donors and acceptors. Furthermore, it transpires that quantum interference between different mechanisms can play an important role. Thus, as the relative importance of each mechanism determines the relevant nanophotonic characteristics, the results reported here afford the means for optimizing highly efficient light-harvesting dendrimer devices

FES rehabilitation platform with real-time control and performance feedback.

Osteoporosis after spinal cord injury is associated with low-trauma fractures, and consequently with increased risk of morbidity and mortality. The loss of bone mass density (BMD) due to paraplegia can be reduced through cyclical electrically-induced muscle contractions. Here we propose an FES control system based on posture switching, that induces transient loading of the lower limbs during a set of standing postures. This aims to produce an increased, evenly distributed BMD, whilst minimising FES-induced muscle fatigue. Here we describe the design and assessment of the FES exercising platform, comprising a controllable multi-channel electrical stimulator and an instrumented standing frame. The platform supports standing and postural shifting, provides real-time human-in-the-loop FES control with on-line feedback to the user. The platforms is used to investigate the effect of regular exercise on the distribution of BMD in people with paraplegia

Manipulation of ultracold atoms in dressed adiabatic radio frequency potentials

We explore properties of atoms whose magnetic hyperfine sub-levels are coupled by an external magnetic radio frequency (rf) field. We perform a thorough theoretical analysis of this driven system and present a number of systematic approximations which eventually give rise to dressed adiabatic radio frequency potentials. The predictions of this analytical investigation are compared to numerically exact results obtained by a wave packet propagation. We outline the versatility and flexibility of this new class of potentials and demonstrate their potential use to build atom optical elements such as double-wells, interferometers and ringtraps. Moreover, we perform simulations of interference experiments carried out in rf induced double-well potentials. We discuss how the nature of the atom-field coupling mechanism gives rise to a decrease of the interference contrast

Interparticle interactions:Energy potentials, energy transfer, and nanoscale mechanical motion in response to optical radiation

In the interactions between particles of material with slightly different electronic levels, unusually large shifts in the pair potential can result from photoexcitation, and on subsequent electronic excitation transfer. To elicit these phenomena, it is necessary to understand the fundamental differences between a variety of optical properties deriving from dispersion interactions, and processes such as resonance energy transfer that occur under laser irradiance. This helps dispel some confusion in the recent literature. By developing and interpreting the theory at a deeper level, one can anticipate that in suitable systems, light absorption and energy transfer will be accompanied by significant displacements in interparticle separation, leading to nanoscale mechanical motion

Laser-controlled fluorescence in two-level systems

The ability to modify the character of fluorescent emission by a laser-controlled, optically nonlinear process has recently been shown theoretically feasible, and several possible applications have already been identified. In operation, a pulse of off-resonant probe laser beam, of sufficient intensity, is applied to a system exhibiting fluorescence, during the interval of excited- state decay following the initial excitation. The result is a rate of decay that can be controllably modified, the associated changes in fluorescence behavior affording new, chemically specific information. In this paper, a two-level emission model is employed in the further analysis of this all-optical process; the results should prove especially relevant to the analysis and imaging of physical systems employing fluorescent markers, these ranging from quantum dots to green fluorescence protein. Expressions are presented for the laser-controlled fluorescence anisotropy exhibited by samples in which the fluorophores are randomly oriented. It is also shown that, in systems with suitably configured electronic levels and symmetry properties, fluorescence emission can be produced from energy levels that would normally decay nonradiatively. © 2010 American Chemical Society