No description available.

No description available.

No description available.

Colloidal quantum dots (CQDs) are an inexpensive and solution processable photovoltaic(PV) material reaching modest efficiencies of 6%. However, doping quantum dots still remains a challenge. This thesis explores the level of doping in lead sulfide (PbS)CQDs by surface ligands and bulk doping within the quantum dot lattice using metals. In light of the knowledge that oxygen creates traps on the surface of PbS CQDs, we have turned to the use of oxygen-free fabrication. We find that under a nitrogen environment, PbS CQD films are n-type and tunable in doping by use of halide ions. We show for the first time control over the doping density of n-type CQD films over a wide range. We also show the ability to fabricate p-type PbS films with high doping density that are compatible with n-type films. This compatibility enabled us to make the world’s first CQD homojunction PV device.

Colloidal quantum dots (CQD) are used in the fabrication of efficient, low-cost solar cells synthesized in and deposited from solution. Breakthroughs in CQD materials have led to a record efficiency of 7.0%. Looking forward, any path toward increasing efficiency must address the trade-off between short charge extraction lengths and long absorption lengths in the near-infrared spectral region. Here we exploit the localized surface plasmon resonance of metal nanoparticles to enhance absorption in CQD films. Finite-difference time-domain analysis directs our choice of plasmonic nanoparticles with minimal parasitic absorption and broadband response in the infrared. We find that gold nanoshells (NS) enhance absorption by up to 100% at λ = 820 nm by coupling of the plasmonic near-field to the surrounding CQD film. We engineer this enhancement for PbS CQD solar cells and observe a 13% improvement in short-circuit current and 11% enhancement in power conversion efficiency.

Colloidal quantum dots (CQDs) are an inexpensive and solution processable photovoltaic(PV) material reaching modest efficiencies of 6%. However, doping quantum dots still remains a challenge. This thesis explores the level of doping in lead sulfide (PbS)CQDs by surface ligands and bulk doping within the quantum dot lattice using metals. In light of the knowledge that oxygen creates traps on the surface of PbS CQDs, we have turned to the use of oxygen-free fabrication. We find that under a nitrogen environment, PbS CQD films are n-type and tunable in doping by use of halide ions. We show for the first time control over the doping density of n-type CQD films over a wide range. We also show the ability to fabricate p-type PbS films with high doping density that are compatible with n-type films. This compatibility enabled us to make the world’s first CQD homojunction PV device.

Colloidal quantum dots (CQD) are used in the fabrication of efficient, low-cost solar cells synthesized in and deposited from solution. Breakthroughs in CQD materials have led to a record efficiency of 7.0%. Looking forward, any path toward increasing efficiency must address the trade-off between short charge extraction lengths and long absorption lengths in the near-infrared spectral region. Here we exploit the localized surface plasmon resonance of metal nanoparticles to enhance absorption in CQD films. Finite-difference time-domain analysis directs our choice of plasmonic nanoparticles with minimal parasitic absorption and broadband response in the infrared. We find that gold nanoshells (NS) enhance absorption by up to 100% at λ = 820 nm by coupling of the plasmonic near-field to the surrounding CQD film. We engineer this enhancement for PbS CQD solar cells and observe a 13% improvement in short-circuit current and 11% enhancement in power conversion efficiency.

Nanomaterial toxicity is a major concern and could potentially hamper the progress of biomedical nanotechnology development. Dispelling these concerns requires that the consequences of nanomaterial exposure are evaluated, and the findings will determine whether developmental hurdles can be overcome. This thesis evaluates the both in vivo and in vitro impact of quantum dots (QD , zinc sulphide capped cadmium selenide semiconductor nanocrystals) a fluorescent nanoparticle label with potential as an optical in vivo imaging agent. This work reviews nanoparticle characterization techniques and their importance to biological responses, and surveys QD interactions both in vivo and in vitro. We collected pharmacokinetic and toxicity data by a) quantitatively surveying the in vivo absorption, distribution , metabolism and excretion of QDs, and b) measuring the impacts of QDs on relevant organs (in vivo) and cells (in vitro). Neither of these areas had been explored when this thesis was started. In vivo, intravenous QD dosing in Sprague-Dawley rats showed uptake into reticuloendothelial cells with surface coating dependent kinetics, slow degradation, no excretion detected in feces or urine, and no indications of toxicity. The liver took up the majority of dose after 90 minutes and small amounts of QDs appeared in the spleen, kidney, and bone marrow. After 30 days, the cadmium concentration in the kidneys increased to 3µg/g without a proportional amount of zinc, indicating QD breakdown. In vitro we noted phagocytic capacity comparable to in vivo results, QD breakdown, and a retention of normal macrophage function thereby demonstrating that primary rat liver macrophages (Kupffer cells) are an appropriate in vitro system with which to investigate the cellular responses to quantum dots. Such an in vitro model will facilitate faster evaluation of individual nanotechnologies intended for in vivo use. This dissertation addresses a lack of in vivo background information needed to understand the consequences of QD exposure; though QD fail to demonstrate pharmacokinetics desirable for in vivo imaging agents, they are not toxic. Importantly, we provide in vitro data that will lead to the development of accurate and efficient in vitro primary screening methods that will be central to the further development of biomedical nanotechnologies.

No description available.

Nanomaterial toxicity is a major concern and could potentially hamper the progress of biomedical nanotechnology development. Dispelling these concerns requires that the consequences of nanomaterial exposure are evaluated, and the findings will determine whether developmental hurdles can be overcome. This thesis evaluates the both in vivo and in vitro impact of quantum dots (QD , zinc sulphide capped cadmium selenide semiconductor nanocrystals) a fluorescent nanoparticle label with potential as an optical in vivo imaging agent. This work reviews nanoparticle characterization techniques and their importance to biological responses, and surveys QD interactions both in vivo and in vitro. We collected pharmacokinetic and toxicity data by a) quantitatively surveying the in vivo absorption, distribution , metabolism and excretion of QDs, and b) measuring the impacts of QDs on relevant organs (in vivo) and cells (in vitro). Neither of these areas had been explored when this thesis was started. In vivo, intravenous QD dosing in Sprague-Dawley rats showed uptake into reticuloendothelial cells with surface coating dependent kinetics, slow degradation, no excretion detected in feces or urine, and no indications of toxicity. The liver took up the majority of dose after 90 minutes and small amounts of QDs appeared in the spleen, kidney, and bone marrow. After 30 days, the cadmium concentration in the kidneys increased to 3µg/g without a proportional amount of zinc, indicating QD breakdown. In vitro we noted phagocytic capacity comparable to in vivo results, QD breakdown, and a retention of normal macrophage function thereby demonstrating that primary rat liver macrophages (Kupffer cells) are an appropriate in vitro system with which to investigate the cellular responses to quantum dots. Such an in vitro model will facilitate faster evaluation of individual nanotechnologies intended for in vivo use. This dissertation addresses a lack of in vivo background information needed to understand the consequences of QD exposure; though QD fail to demonstrate pharmacokinetics desirable for in vivo imaging agents, they are not toxic. Importantly, we provide in vitro data that will lead to the development of accurate and efficient in vitro primary screening methods that will be central to the further development of biomedical nanotechnologies.