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

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