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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
21

Two-Photon Excited Fluorescence Depolarisation : Experimental and Theoretical Development

Ryderfors, Linus January 2008 (has links)
<p>We have studied fundamental aspects of time-resolved two-photon excited fluorescence depolarisation. The thesis presents experimental as well as theoretical progress. We show that a multi-photon induced instrumental response function obtained from a suspension of gold nanoparticles is appropriate for the analysis of two-photon excited fluorescence decays obtained using time-correlated single photon counting detection. Theoretical expressions have been derived for the fluorescence anisotropy decay obtained upon two-photon excitation of various molecular systems in liquid solutions: a) an anisotropic rigid rotor that undergoes rotational diffusion in the presence of ultrafast unresolved restricted reorientations, e.g. librations. b) a molecular group covalently attached to a stationary macromolecule, and undergoing local reorientation in a uniaxial ordering potential. A new approach to the analysis of two-photon excited fluorescence depolarisation experiments was developed, which combines data obtained by using linearly and circularly polarised excitation light, in a global manner. In the analysis, knowledge about unresolved reorientations was obtained from one-photon excitation studies of the corresponding systems. By means of this procedure it has been possible to obtain quantitative information about the molecular two-photon absorption tensor for perylene and two of its derivatives. Thereby the symmetry of the final excited and intermediate vibronic states could be assigned. The analysis reveals that the two-photon transition studied with the 800 nm laser exhibits mixed character. An important finding from the experiments was that the two-photon absorption tensor appears to be solvent dependent. Furthermore, the thesis presents the first theoretical treatment of two-photon excited donor-donor energy migration in the presence of molecular reorientation and which applies the extended Förster theory. Explicit expressions for molecules that belong to the point groups D<sub>2h</sub>, D<sub>2</sub> and C<sub>2v</sub> are given. Preliminary experiments are finally also reported on a two-photon excited donor-donor energy migration system consisting of a bisanthryl-bisteroid. </p>
22

Energy transfer processes in supramolecular light-harvesting systems

Stevens, Amy L. January 2011 (has links)
This dissertation attempts to understand how energy transfer in a molecular wire and a spherical organic assembly are affected by molecular structure. The molecular wire is a DNA-hybrid structure composed of a strand of thymine bases appended by a cyanine dye. Hydrogen bonded to each base is a naphthalene-derivative molecule. Using time-integrated photoluminescence and time-correlated single photon counting measurements, energy transfer from the naphthalene donors to the cyanine acceptors was confirmed, and its dependence on temperature and DNA-template length investigated. Donor-thymine bonding was disrupted at temperatures above about 25 degrees Celcius resulting in poor donor template decoration and low rates of energy transfer. Increasing numbers of donors attach to the scaffold, forming an orderly array, as the template length increases due to the stabilising effects of the donor-donor pi-stacking interactions. Conversely, modelled energy transfer rates fall as the scaffold length increases because of the longer donor-acceptor distances involved. Therefore, the energy transfer rate was greatest for a template built from 30 thymines. The spherical organic assemblies (nanoparticles) are formed by fast injection of a small volume of molecularly dissolved fluorene-derivative amphiphilic molecules into a polar solvent. The amphiphilic molecules contained either a naphthalene (donor) or a benzothiadiazole (acceptor) core. The donor-acceptor mixed nanoparticles resemble an amorphous polymer film and were modelled as such using the Foerster resonance energy transfer theory. The Foerster radii extracted from the measurements depends intricately on the donor-acceptor spectral overlap and distance. The latter effect was controlled by the stacking interactions between the molecules. Altering the morphology of the structural units is the key to optimising energy transfer in molecular structures. To achieve efficient organic molecule-based devices, the importance of this property needs to be fully appreciated and effectively exploited.
23

3D imaging using time-correlated single photon counting

Neimert-Andersson, Thomas January 2010 (has links)
<p>This project investigates a laser radar system. The system is based on the principles of time-correlated single photon counting, and by measuring the times-of-flight of reflected photons it can find range profiles and perform three-dimensional imaging of scenes. Because of the photon counting technique the resolution and precision that the system can achieve is very high compared to analog systems. These properties make the system interesting for many military applications. For example, the system can be used to interrogate non-cooperative targets at a safe distance in order to gather intelligence. However, signal processing is needed in order to extract the information from the data acquired by the system. This project focuses on the analysis of different signal processing methods.</p><p>The Wiener filter and the Richardson-Lucy algorithm are used to deconvolve the data acquired by the photon counting system. In order to find the positions of potential targets different approaches of non-linear least squares methods are tested, as well as a more unconventional method called ESPRIT. The methods are evaluated based on their ability to resolve two targets separated by some known distance and the accuracy with which they calculate the position of a single target, as well as their robustness to noise and their computational burden.</p><p>Results show that fitting a curve made of a linear combination of asymmetric super-Gaussians to the data by a method of non-linear least squares manages to accurately resolve targets separated by 1.75 cm, which is the best result of all the methods tested. The accuracy for finding the position of a single target is similar between the methods but ESPRIT has a much faster computation time.</p>
24

Two-Photon Excited Fluorescence Depolarisation : Experimental and Theoretical Development

Ryderfors, Linus January 2008 (has links)
We have studied fundamental aspects of time-resolved two-photon excited fluorescence depolarisation. The thesis presents experimental as well as theoretical progress. We show that a multi-photon induced instrumental response function obtained from a suspension of gold nanoparticles is appropriate for the analysis of two-photon excited fluorescence decays obtained using time-correlated single photon counting detection. Theoretical expressions have been derived for the fluorescence anisotropy decay obtained upon two-photon excitation of various molecular systems in liquid solutions: a) an anisotropic rigid rotor that undergoes rotational diffusion in the presence of ultrafast unresolved restricted reorientations, e.g. librations. b) a molecular group covalently attached to a stationary macromolecule, and undergoing local reorientation in a uniaxial ordering potential. A new approach to the analysis of two-photon excited fluorescence depolarisation experiments was developed, which combines data obtained by using linearly and circularly polarised excitation light, in a global manner. In the analysis, knowledge about unresolved reorientations was obtained from one-photon excitation studies of the corresponding systems. By means of this procedure it has been possible to obtain quantitative information about the molecular two-photon absorption tensor for perylene and two of its derivatives. Thereby the symmetry of the final excited and intermediate vibronic states could be assigned. The analysis reveals that the two-photon transition studied with the 800 nm laser exhibits mixed character. An important finding from the experiments was that the two-photon absorption tensor appears to be solvent dependent. Furthermore, the thesis presents the first theoretical treatment of two-photon excited donor-donor energy migration in the presence of molecular reorientation and which applies the extended Förster theory. Explicit expressions for molecules that belong to the point groups D2h, D2 and C2v are given. Preliminary experiments are finally also reported on a two-photon excited donor-donor energy migration system consisting of a bisanthryl-bisteroid.
25

Electronic Energy Transfer within Asymmetric Pairs of Fluorophores: Partial Donor-Donor Energy Migration (PDDEM)

Kalinin, Stanislav January 2004 (has links)
A kinetic model of electronic energy migration within pairs of photophysically non-identical fluorophores has been developed. The model applies to fluorescent groups that exhibit different photophysical and spectral properties when attached to different positions in a macromolecule. The energy migration within such asymmetric pairs is partially reversible, which leads to the case of partial donor-donor energy migration (PDDEM). The model of PDDEM is an extension of the recently developed donor-donor energy migration model (DDEM, F. Bergström et al, PNAS 96 (1999) 12477), and applies to quantitative measurements of energy migration rates and distances within macromolecules. One important distinction from the DDEM model is that the distances can be obtained from fluorescence lifetime measurements. A model of fluorescence depolarisation in the presence of PDDEM is also presented. To experimentally test the PDDEM approach, different model systems were studied. The model was applied to measure distances between rhodamine and fluorescein groups within on-purpose synthesised molecules that were solubilised in lipid bilayers. Moreover, distances were measured between BODIPY groups in mutant forms of the plasminogen activator inhibitor of type 2 (PAI-2). Measurements of both the fluorescence intensity decays and the time-resolved depolarisation were performed. The obtained distances were in good agreement with independent determinations. Finally, the PDDEM within pairs of donors is considered, for which both donors exhibit a nonexponential fluorescence decay. In this case it turns out that the fluorescence relaxation of a coupled system contains distance information even if the photophysics of the donors is identical. It is also demonstrated that the choice of relaxation model has a negligible effect on the obtained distances. The latter conclusion holds also for the case of donor-acceptor energy transfer.
26

3D imaging using time-correlated single photon counting

Neimert-Andersson, Thomas January 2010 (has links)
This project investigates a laser radar system. The system is based on the principles of time-correlated single photon counting, and by measuring the times-of-flight of reflected photons it can find range profiles and perform three-dimensional imaging of scenes. Because of the photon counting technique the resolution and precision that the system can achieve is very high compared to analog systems. These properties make the system interesting for many military applications. For example, the system can be used to interrogate non-cooperative targets at a safe distance in order to gather intelligence. However, signal processing is needed in order to extract the information from the data acquired by the system. This project focuses on the analysis of different signal processing methods. The Wiener filter and the Richardson-Lucy algorithm are used to deconvolve the data acquired by the photon counting system. In order to find the positions of potential targets different approaches of non-linear least squares methods are tested, as well as a more unconventional method called ESPRIT. The methods are evaluated based on their ability to resolve two targets separated by some known distance and the accuracy with which they calculate the position of a single target, as well as their robustness to noise and their computational burden. Results show that fitting a curve made of a linear combination of asymmetric super-Gaussians to the data by a method of non-linear least squares manages to accurately resolve targets separated by 1.75 cm, which is the best result of all the methods tested. The accuracy for finding the position of a single target is similar between the methods but ESPRIT has a much faster computation time.
27

[pt] CONTAGEM DE FÓTONS NO INFRAVERMELHO PRÓXIMO E MÉDIO VIA CONVERSÃO DE FREQÜÊNCIAS APLICADA A COMUNICAÇÕES QUÂNTICAS / [en] SINGLE PHOTON COUNTING IN THE NEAR- AND MID-INFRARED VIA FREQUENCY UP-CONVERSION APPLIED TO QUANTUM COMMUNICATIONS

06 September 2007 (has links)
[pt] Dois dispositivos de contagem de fótons únicos, sensíveis a comprimentos de onda no infravermelho próximo e médio, são propostos e experimentalmente investigados. Ambos utilizam uma técnica de dois estágios, composta de uma etapa inicial de conversão de freqüências em um cristal não-linear seguida de detecção por um fotodiodo avalanche de silício. Enquanto o primeiro projeto é voltado à detecção de fótons únicos a 1.55 &#956;m para comunicações quânticas via fibra óptica, usando um processo intra-cavidade, o segundo projeto prevê o desenvolvimento de um contador de fótons operando a 4.65 &#956;m para sistemas de espaço livre. Neste caso, um estudo de viabilidade para um sistema prático de criptografia quântica operando em um comprimento de onda no infravermelho médio é realizado. Os resultados mostram que, usando a tecnologia disponível na atualidade, tal sistema pode ser construído, embora sua utilidade se mostre restrita a enlaces possuindo certas condições meteorológicas específicas. / [en] Two single photon counting devices, operating at near- and mid-infrared wavelengths, are introduced and experimentally investigated. Both use a twostage technique, comprised of an initial frequency up-conversion procedure inside a nonlinear crystal followed by a silicon avalanche photodiode. Whereas the first project consists on detection of single photons at 1.55 ìm for fiber-optic-based quantum communications, using a cavity-enhanced procedure, the second project envisions the development of a single-photon counter operating at 4.65 ìm for free-space systems. In this case, a feasibility study for a practical quantum key distribution system operating in a mid-infrared wavelength is performed. The results show that, using present-day technology, such a system can be constructed, albeit its usefulness would be restricted to operation under very specific weather conditions.
28

Development of Time-Resolved Diffuse Optical Systems Using SPAD Detectors and an Efficient Image Reconstruction Algorithm

Alayed, Mrwan January 2019 (has links)
Time-Resolved diffuse optics is a powerful and safe technique to quantify the optical properties (OP) for highly scattering media such as biological tissues. The OP values are correlated with the compositions of the measured objects, especially for the tissue chromophores such as hemoglobin. The OP are mainly the absorption and the reduced scattering coefficients that can be quantified for highly scattering media using Time-Resolved Diffuse Optical Spectroscopy (TR-DOS) systems. The OP can be retrieved using Time-Resolved Diffuse Optical Imaging (TR-DOI) systems to reconstruct the distribution of the OP in measured media. Therefore, TR-DOS and TR-DOI can be used for functional monitoring of brain and muscles, and to diagnose some diseases such as detection and localization for breast cancer and blood clot. In general, TR-DOI systems are non-invasive, reliable, and have a high temporal resolution. TR-DOI systems have been known for their complexity, bulkiness, and costly equipment such as light sources (picosecond pulsed laser) and detectors (single photon counters). Also, TR-DOI systems acquire a large amount of data and suffer from the computational cost of the image reconstruction process. These limitations hinder the usage of TR-DOI for widespread potential applications such as clinical measurements. The goals of this research project are to investigate approaches to eliminate two main limitations of TR-DOI systems. First, building TR-DOS systems using custom-designed free-running (FR) and time-gated (TG) SPAD detectors that are fabricated in low-cost standard CMOS technology instead of the costly photon counting and timing detectors. The FR-TR-DOS prototype has demonstrated comparable performance (for homogeneous objects measurements) with the reported TR-DOS prototypes that use commercial and expensive detectors. The TG-TR-DOS prototype has acquired raw data with a low level of noise and high dynamic range that enable this prototype to measure multilayered objects such as human heads. Second, building and evaluating TR-DOI prototype that uses a computationally efficient algorithm to reconstruct high quality 3D tomographic images by analyzing a small part of the acquired data. This work indicates the possibility to exploit the recent advances in the technologies of silicon detectors, and computation to build low-cost, compact, portable TR-DOI systems. These systems can expand the applications of TR-DOI and TR-DOS into several fields such as oncology, and neurology. / Thesis / Doctor of Philosophy (PhD)
29

Novel fabrication and testing of light confinement devices

Ring, Josh January 2016 (has links)
The goal of this project is to study novel nanoscale excitation volumes, sensitive enoughto study individual chromophores and go on to study new and exciting self assemblyapproaches to this problem. Small excitation volumes may be engineered using light con-finement inside apertures in metal films. These apertures enhance fluorescence emissionrates, quantum yields, decrease fluorescence quenching, enable higher signal-to-noiseratios and allow higher concentration single chromophore fluorescence, to be studied byrestricting this excitation volume. Excitation volumes are reported on using the chro-mophore's fluorescence by utilising fluorescence correlation spectroscopy, which monitorsfluctuations in fluorescence intensity. From the correlation in time, we can find the res-idence time, the number of chromophores, the volume in which they are diffusing andtherefore the fluorescence emission efficiency. Fluorescence properties are a probe ofthe local environment, a particularly powerful tool due to the high brightness (quantumyield) fluorescent dyes and sensitive photo-detection equipment both of which are readilyavailable, (such as avalanche photodiodes and photomultiplier tubes). Novel materialscombining the properties of conducting and non-conducting materials at scales muchsmaller than the incident wavelength are known as meta-materials. These allow combi-nations of properties not usually possible in natural materials at optical frequencies. Theproperties reported so far include; negative refraction, negative phase velocity, fluorescenceemission enhancement, lensing and therefore light confinement has also been proposed tobe possible. Instead of expensive and slow lithography methods many of these materialsmay be fabricated with self assembly techniques, which are truly nanoscopic and otherwiseinaccessible with even the most sophisticated equipment. It was found that nanoscaled volumes from ZMW and HMMs based on NW arrays wereall inefficient at enhancing fluorescence. The primary cause was the reduced fluorescencelifetime reducing the fluorescence efficiency, which runs contrary to some commentatorsin the literature. NW based lensing was found to possible in the blue region of the opticalspectrum in a HMM, without the background fluorescence normally associated with a PAAtemplate. This was achieved using a pseudo-ordered array of relatively large nanowireswith a period just smaller than lambda / 2 which minimised losses. Nanowires in the traditionalregime lambda / 10 produced significant scattering and lead to diffraction, such that they werewholly unsuitable for an optical lensing application.
30

Solvatationsdynamik an biologischen Grenzschichten / Solvation dynamics at biological interfaces

Seidel, Marco Thomas 05 November 2003 (has links)
No description available.

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