Search results for "Excitation"
showing 10 items of 1290 documents
Theoretical investigation of electronic excitation energy transfer in bichromophoric assemblies.
2008
Electronic excitation energy transfer (EET) rates in rylene diimide dyads are calculated using second-order approximate coupled-cluster theory and time-dependent density functional theory. We investigate the dependence of the EET rates on the interchromophoric distance and the relative orientation and show that Forster theory works quantitatively only for donor-acceptor separations larger than roughly 5 nm. For smaller distances the EET rates are over- or underestimated by Forster theory depending on the respective orientation of the transition dipole moments of the chromophores. In addition to the direct transfer rates we consider bridge-mediated transfer originating from oligophenylene un…
A Theoretical Model for Excitation Energy Transfer in Chlorosomes: Lamellar and Rod-Shaped Antenna Structures
2008
A model based on exciton theory is presented for description of excitation energy transfer in chlorosomes. Three models to describe the internal organization of the pigments inside the chlorosome were considered, a stack of single-wall rods, a stack of double-wall rods and a stack of lamellae directed along the long axis of the chlorosome. Simulated absorption, circular dichroism and linear dichroism spectra of single-wall rod and the lamella structures turned out to be practically identical. It was shown that rod—rod interactions may localize the exciton states in the regions of a rod facing a neighboring rod. Such localized states provide a fast excitation energy transfer mechanism in per…
Exciton description of chlorosome to baseplate excitation energy transfer in filamentous anoxygenic phototrophs and green sulfur bacteria.
2013
A description of intra-chlorosome and from chlorosome to baseplate excitation energy transfer in green sulfur bacteria and in filamentous anoxygenic phototrophs is presented. Various shapes and sizes, single and multiwalled tubes, cylindrical spirals and lamellae of the antenna elements mimicking pigment organization in chlorosomes were generated by using molecular mechanics calculations, and the absorption, LD, and CD spectra of these were predicted by using exciton theory. Calculated absorption and LD spectra were similar for all modeled antenna structures; on the contrary, CD spectra turned out to be sensitive to the size and pigment orientations in the antenna. It was observed that, bri…
Modelling excitonic energy transfer in the photosynthetic unit of purple bacteria
2009
Abstract Molecular mechanics and quantum chemical configuration interaction calculations in combination with exciton theory were used to predict vibronic energies and eigenstates of light harvesting antennae and the reaction centre and to evaluate excitation energy transfer rates in the photosynthetic unit of purple bacteria. Excitation energy transfer rates were calculated by using the transition matrix formalism and exciton basis sets of the interacting antenna systems. Energy transfer rates of 600–800 fs from B800 ring to B850 ring in the LH2 antenna, 3–10 ps from LH2 to LH2 antenna, 2–8 ps from LH2 to LH1 antenna and finally 30–70 ps from LH1 to the reaction centre were obtained. Depend…
Control of the electronic energy transfer pathway between two single fluorophores by dual pulse excitation.
2009
We report on the control of the energy transfer pathway in individual donor-acceptor dyads by proper timing of light pulses matching the donor and acceptor transition frequencies, respectively. Excitation of both chromophores at virtually the same time induces efficient singlet-singlet annihilation, whereby excitation energy effectively flows from the acceptor to the donor. The dual pulse excitation scheme implemented here allows for all-optical switching of the fluorescence intensity at the single-molecule level. The population of higher excited states at the donor site was found to significantly increase the photobleaching probability.
Quasi-spherical focal spot in two-photon scanning microscopy by three-ring apodization
2005
International audience; We present a beam-shaping technique for two-photon excitation (TPE) fluorescence microscopy. We show that by inserting a properly designed three-ring pupil filter in the illumination beam of the microscope, the effective optical sectioning capacity of such a system improves so that the point spread function gets a quasi-spherical shape. Such an improvement, which allows the acquisition of 3D images with isotropic quality, is obtained at the expense of only a small increase of the overall energy in the axial sidelobes. The performance of this technique is illustrated with a scanning TPE microscopy experiment in which the image of small beads is obtained. We demonstrat…
Axial resolution in two-color excitation fluorescence microscopy by phase-only binary apodization
2005
We study the effect of a kind of binary phase-only filters, the Toraldo filters, in two-color excitation fluorescence microscopy. We show that by simple insertion of a properly designed Toraldo filter in one of the illumination arms the axial resolution of the system is significantly improved. Specifically, the main peak of the point spread function is narrowed by 22% along the axial direction.
Light Sheet Fluorescence Microscopy (LSFM) for Two-Photon Excitation Imaging of Thick Samples.
2015
Over the last decades, fluorescence microscopy techniques have been developed in order to provide a deeper, faster and higher resolution imaging of three-dimensional biological samples. Within this framework, Light Sheet Fluorescence Microscopy (LSFM) became an increasingly useful and popular imaging technique able to answer several biological questions in the field of developmental biology [1]. Thanks to the spatial confinement of the excitation process within a thin sheet in the focal plane, it provides an intrinsic optical sectioning and a reduced phototoxicity. On the other side, Two-Photon Excitation (2PE), thanks to the use of IR wavelengths, has become an invaluable tool to improve i…
Ship Roll Motion under Stochastic Agencies Using Path Integral Method
2009
The response of ship roll oscillation under random ice impulsive loads modeled by Poisson arrival process is very important in studying the safety of ships navigation in cold regions. Under both external and parametric random excitations the evolution of the probability density function of roll motion is evaluated using the path integral (PI) approach. The PI method relies on the Chapman-Kolmogorov equation, which governs the response transition probability density functions at two close intervals of time. Once the response probability density function at an early close time is specified, its value at later close time can be evaluated. The PI method is first demonstrated via simple dynamica…
Concentration dependence of the electro-optical spectra from two-dimensional aggregated chromophore systems
1991
The linear and the quadratic Stark effects have been employed to characterize aggregate formation of an amphiphilic cyanine dye mixed with arachidic acid in various concentrations within Langmuir-Blodgett multilayers. Two different electrode configurations with the electric field directions parallel and normal to the films have been employed to test the responses of the electronic spectra to external fields. The observations have been used to quantify the induced and static dipole moment changes on excitation of the chromophores. A comparison of the results obtained from different multilayer arrangements is suggestive of inter-layer couplings for the case of head-to-head configurations of t…