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The development of high efficiency III-V solar cells is needed to meet the demands of a promising renewable energy source. Intermediate band solar cells (IBSCs) using semiconductor quantum dots (QDs) have been proposed to exceed the Shockley-Queisser efficiency limit [1]. The introduction of an IB in the forbidden gap of host material generates two additional carrier transitions for sub-bandgap photon absorption, leading to increased photocurrent of IBSCs while simultaneously allowing an open-circuit voltage of the highest band gap. To realize a high efficiency IBSC, QD structures should have high crystal quality and optimized electronic properties. This dissertation focuses on the investigation and optimization of the structural and optical properties of InAs/GaAsSb QDs and the development of InAs/GaAsSb QD-based IBSCs.
In the present dissertation, the interband optical transition and carrier lifetime of InAs/GaAsSb QDs with different silicon delta-doping densities have been first studied by time-integrated and time-resolved photoluminescence (PL). It is found that an optimized silicon delta-doping density in the QDs enables to fill the QD electronic states with electrons for sub-bandgap photon absorption and to improve carrier lifetime of the QDs.
After that, the crystal quality and QD morphology of single- and multi-stack InAs/GaAsSb QDs with different Sb compositions have been investigated by transmission electron microscopy (TEM) and x-ray diffraction (XRD). The TEM studies reveal that QD morphology of single-stack QDs is affected by Sb composition due to strain reducing effect of Sb incorporation. The XRD studies confirm that the increase of Sb composition increases the lattice mismatch between GaAs matrix and GaAsSb spacers, resulting in increase of the strain relaxation in GaAsSb of the multi-stack QDs. Furthermore, the increase of Sb composition causes a PL redshift and increases carrier lifetime of QDs.
Finally, the spacer layer thickness of multi-stack InAs/GaAsSb QDs is optimized for the growth of InAs/GaAsSb QD solar cells (QDSCs). The InAs/GaAsSb QDSCs with GaP strain compensating layer are grown and their device performances are characterized. The increase of GaP coverage is beneficial to improve the conversion efficiency of the QDSCs. However, the conversion efficiency is reduced when using a relatively large GaP coverage.
In the present dissertation, the interband optical transition and carrier lifetime of InAs/GaAsSb QDs with different silicon delta-doping densities have been first studied by time-integrated and time-resolved photoluminescence (PL). It is found that an optimized silicon delta-doping density in the QDs enables to fill the QD electronic states with electrons for sub-bandgap photon absorption and to improve carrier lifetime of the QDs.
After that, the crystal quality and QD morphology of single- and multi-stack InAs/GaAsSb QDs with different Sb compositions have been investigated by transmission electron microscopy (TEM) and x-ray diffraction (XRD). The TEM studies reveal that QD morphology of single-stack QDs is affected by Sb composition due to strain reducing effect of Sb incorporation. The XRD studies confirm that the increase of Sb composition increases the lattice mismatch between GaAs matrix and GaAsSb spacers, resulting in increase of the strain relaxation in GaAsSb of the multi-stack QDs. Furthermore, the increase of Sb composition causes a PL redshift and increases carrier lifetime of QDs.
Finally, the spacer layer thickness of multi-stack InAs/GaAsSb QDs is optimized for the growth of InAs/GaAsSb QD solar cells (QDSCs). The InAs/GaAsSb QDSCs with GaP strain compensating layer are grown and their device performances are characterized. The increase of GaP coverage is beneficial to improve the conversion efficiency of the QDSCs. However, the conversion efficiency is reduced when using a relatively large GaP coverage.
ContributorsKim, Yeongho (Author) / Honsberg, Christiana (Thesis advisor) / Goodnick, Stephen (Committee member) / Faleev, Nikolai (Committee member) / Smith, David (Committee member) / Arizona State University (Publisher)
Created2015
Description
Operando transmission electron microscopy (TEM) is an extension of in-situ TEM in which the performance of the material being observed is measured simultaneously. This is of great value, since structure-performance relationships lie at the heart of materials science. For catalyst materials, like the SiO2-supported Ru nanoparticles studied, the important performance metric, catalyst activity, is measured inside the microscope by determining the gas composition during imaging. This is accomplished by acquisition of electron energy loss spectra (EELS) of the gas in the environmental TEM while catalysis is taking place. In this work, automated methods for rapidly quantifying low-loss and core-loss EELS of gases were developed. A new sample preparation method was also established to increase catalytic conversion inside a differentially-pumped environmental TEM, and the maximum CO conversion observed was about 80%. A system for mixing gases and delivering them to the environmental TEM was designed and built, and a method for locating and imaging nanoparticles in zone axis orientations while minimizing electron dose rate was determined.
After atomic resolution images of Ru nanoparticles observed during CO oxidation were obtained, the shape and surface structures of these particles was investigated. A Wulff model structure for Ru particles was compared to experimental images both by manually rotating the model, and by automatically determining a matching orientation using cross-correlation of shape signatures. From this analysis, it was determined that most Ru particles are close to Wulff-shaped during CO oxidation. While thick oxide layers were not observed to form on Ru during CO oxidation, thin RuO2 layers on the surface of Ru nanoparticles were imaged with atomic resolution for the first time. The activity of these layers is discussed in the context of the literature on the subject, which has thus far been inconclusive. We conclude that disordered oxidized ruthenium, rather than crystalline RuO2 is the most active species.
After atomic resolution images of Ru nanoparticles observed during CO oxidation were obtained, the shape and surface structures of these particles was investigated. A Wulff model structure for Ru particles was compared to experimental images both by manually rotating the model, and by automatically determining a matching orientation using cross-correlation of shape signatures. From this analysis, it was determined that most Ru particles are close to Wulff-shaped during CO oxidation. While thick oxide layers were not observed to form on Ru during CO oxidation, thin RuO2 layers on the surface of Ru nanoparticles were imaged with atomic resolution for the first time. The activity of these layers is discussed in the context of the literature on the subject, which has thus far been inconclusive. We conclude that disordered oxidized ruthenium, rather than crystalline RuO2 is the most active species.
ContributorsMiller, Benjamin (Author) / Crozier, Peter (Thesis advisor) / Liu, Jingyue (Committee member) / McCartney, Martha (Committee member) / Rez, Peter (Committee member) / Arizona State University (Publisher)
Created2016
Description
Urbanization and woody plant encroachment, with subsequent brush management, are two significant land cover changes that are represented in the southwestern United States. Urban areas continue to grow, and rangelands are undergoing vegetation conversions, either purposely through various rangeland management techniques, or by accident, through inadvertent effects of climate and management. This thesis investigates how areas undergoing land cover conversions in a semiarid region, through urbanization or rangeland management, influences energy, water and carbon fluxes. Specifically, the following scientific questions are addressed: (1) what is the impact of different urban land cover types in Phoenix, AZ on energy and water fluxes?, (2) how does the land cover heterogeneity influence energy, water, and carbon fluxes in a semiarid rangeland undergoing woody plant encroachment?, and (3) what is the impact of brush management on energy, water, and carbon fluxes?
The eddy covariance technique is well established to measure energy, water, and carbon fluxes and is used to quantify and compare flux measurements over different land surfaces. Results reveal that in an urban setting, paved surfaces exhibit the largest sensible and lowest latent heat fluxes in an urban environment, while a mesic landscape exhibits the largest latent heat fluxes, due to heavy irrigation. Irrigation impacts flux sensitivity to precipitation input, where latent heat fluxes increase with precipitation in xeric and parking lot landscapes, but do not impact the mesic system. In a semiarid managed rangeland, past management strategies and disturbance histories impact vegetation distribution, particularly the distribution of mesquite trees. At the site with less mesquite coverage, evapotranspiration (ET) is greater, due to greater grass cover. Both sites are generally net sinks of CO2, which is largely dependent on moisture availability, while the site with greater mesquite coverage has more respiration and generally greater gross ecosystem production (GEP). Initial impacts of brush management reveal ET and GEP decrease, due to the absence of mesquite trees. However the impact appears to be minimal by the end of the productive season. Overall, this dissertation advances the understanding of land cover change impacts on surface energy, water, and carbon fluxes in semiarid ecosystems.
The eddy covariance technique is well established to measure energy, water, and carbon fluxes and is used to quantify and compare flux measurements over different land surfaces. Results reveal that in an urban setting, paved surfaces exhibit the largest sensible and lowest latent heat fluxes in an urban environment, while a mesic landscape exhibits the largest latent heat fluxes, due to heavy irrigation. Irrigation impacts flux sensitivity to precipitation input, where latent heat fluxes increase with precipitation in xeric and parking lot landscapes, but do not impact the mesic system. In a semiarid managed rangeland, past management strategies and disturbance histories impact vegetation distribution, particularly the distribution of mesquite trees. At the site with less mesquite coverage, evapotranspiration (ET) is greater, due to greater grass cover. Both sites are generally net sinks of CO2, which is largely dependent on moisture availability, while the site with greater mesquite coverage has more respiration and generally greater gross ecosystem production (GEP). Initial impacts of brush management reveal ET and GEP decrease, due to the absence of mesquite trees. However the impact appears to be minimal by the end of the productive season. Overall, this dissertation advances the understanding of land cover change impacts on surface energy, water, and carbon fluxes in semiarid ecosystems.
ContributorsTempleton, Nicole Pierini (Author) / Vivoni, Enrique R (Thesis advisor) / Archer, Steven R (Committee member) / Mascaro, Giuseppe (Committee member) / Scott, Russell L. (Committee member) / Wang, Zhi-Hua (Committee member) / Arizona State University (Publisher)
Created2017
Description
This study examines the spatial and temporal patterns of the surface urban heat island (SUHI) intensity in the Phoenix metropolitan area and the relationship with land use land cover (LULC) change between 2000 and 2014. The objective is to identify specific regions in Phoenix that have been increasingly heated and cooled to further understand how LULC change influences the SUHI intensity. The data employed include MODerate-resolution Imaging Spectroradiometer (MODIS) land surface temperature (LST) 8-day composite June imagery, and classified LULC maps generated using 2000 and 2014 Landsat imagery. Results show that the regions that experienced the most significant LST changes during the study period are primarily on the outskirts of the Phoenix metropolitan area for both daytime and nighttime. The conversion to urban, residential, and impervious surfaces from all other LULC types has been identified as the primary cause of the UHI effect in Phoenix. Vegetation cover has been shown to significantly lower LST for both daytime and nighttime due to its strong cooling effect by producing more latent heat flux and less sensible heat flux. We suggest that urban planners, decision-makers, and city managers formulate new policies and regulations that encourage residential, commercial, and industrial developers to include more vegetation when planning new construction.
ContributorsWang, Chuyuan (Author) / Myint, Soe (Author) / Wang, Zhi-Hua (Author) / Song, Jiyun (Author) / College of Liberal Arts and Sciences (Contributor)
Created2016-02-26
Description
Studies on urban heat island (UHI) have been more than a century after the phenomenon was first discovered in the early 1800s. UHI emerges as the source of many urban environmental problems and exacerbates the living environment in cities. Under the challenges of increasing urbanization and future climate changes, there is a pressing need for sustainable adaptation/mitigation strategies for UHI effects, one popular option being the use of reflective materials. While it is introduced as one effective method to reduce temperature and energy consumption in cities, its impacts on multi-dimensional environmental sustainability and large-scale non-local effect are inadequately explored. This paper provides a synthetic overview of potential environmental impacts of reflective materials at a variety of scales, ranging from energy load on a single building to regional hydroclimate. The review shows that mitigation potential of reflective materials depends on a portfolio of factors, including building characteristics, urban environment, meteorological and geographical conditions, to name a few. Precaution needs to be exercised by city planners and policy makers for large-scale deployment of reflective materials before their environmental impacts, especially on regional hydroclimates, are better understood. In general, it is recommended that optimal strategy for UHI needs to be determined on a city-by-city basis, rather than adopting a “one-solution-fits-all” strategy.
ContributorsYang, Jiachuan (Contributor) / Wang, Zhi-Hua (Correspondent) / Kaloush, Kamil (Contributor)
Created2015-06-11