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Increasing the conversion efficiencies of photovoltaic (PV) cells beyond the single junction theoretical limit is the driving force behind much of third generation solar cell research. Over the last half century, the experimental conversion efficiency of both single junction and tandem solar cells has plateaued as manufacturers and researchers have

Increasing the conversion efficiencies of photovoltaic (PV) cells beyond the single junction theoretical limit is the driving force behind much of third generation solar cell research. Over the last half century, the experimental conversion efficiency of both single junction and tandem solar cells has plateaued as manufacturers and researchers have optimized various materials and structures. While existing materials and technologies have remarkably good conversion efficiencies, they are approaching their own limits. For example, tandem solar cells are currently well developed commercially but further improvements through increasing the number of junctions struggle with various issues related to material interfacial defects. Thus, there is a need for novel theoretical and experimental approaches leading to new third generation cell structures. Multiple exciton generation (MEG) and intermediate band (IB) solar cells have been proposed as third generation alternatives and theoretical modeling suggests they can surpass the detailed balance efficiency limits of single junction and tandem solar cells. MEG or IB solar cell has a variety of advantages enabling the use of low bandgap materials. Integrating MEG and IB with other cell types to make novel solar cells (such as MEG with tandem, IB with tandem or MEG with IB) potentially offers improvements by employing multi-physics effects in one device. This hybrid solar cell should improve the properties of conventional solar cells with a reduced number of junction, increased light-generated current and extended material selections. These multi-physics effects in hybrid solar cells can be achieved through the use of nanostructures taking advantage of the carrier confinement while using existing solar cell materials with excellent characteristics. This reduces the additional cost to develop novel materials and structures. In this dissertation, the author develops thermodynamic models for several novel types of solar cells and uses these models to optimize and compare their properties to those of existing PV cells. The results demonstrate multiple advantages from combining MEG and IB technology with existing solar cell structures.
ContributorsLee, Jongwon (Author) / Honsberg, C. (Christiana B.) (Thesis advisor) / Bowden, Stuart (Committee member) / Roedel, Ronald (Committee member) / Goodnick, Stephen (Committee member) / Schroder, Dieter (Committee member) / Arizona State University (Publisher)
Created2014
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Description
Zinc oxide (ZnO), a naturally n-type semiconductor has been identified as a promising candidate to replace indium tin oxide (ITO) as the transparent electrode in solar cells, because of its wide bandgap (3.37 eV), abundant source materials and suitable refractive index (2.0 at 600 nm). Spray deposition is a convenient

Zinc oxide (ZnO), a naturally n-type semiconductor has been identified as a promising candidate to replace indium tin oxide (ITO) as the transparent electrode in solar cells, because of its wide bandgap (3.37 eV), abundant source materials and suitable refractive index (2.0 at 600 nm). Spray deposition is a convenient and low cost technique for large area and uniform deposition of semiconductor thin films. In particular, it provides an easier way to dope the film by simply adding the dopant precursor into the starting solution. In order to reduce the resistivity of undoped ZnO, many works have been done by doping in the ZnO with either group IIIA elements or VIIA elements using spray pyrolysis. However, the resistivity is still too high to meet TCO's resistivity requirement. In the present work, a novel co-spray deposition technique is developed to bypass a fundamental limitation in the conventional spray deposition technique, i.e. the deposition of metal oxides from incompatible precursors in the starting solution. With this technique, ZnO films codoped with one cationic dopant, Al, Cr, or Fe, and an anionic dopant, F, have been successfully synthesized, in which F is incompatible with all these three cationic dopants. Two starting solutions were prepared and co-sprayed through two separate spray heads. One solution contained only the F precursor, NH 4F. The second solution contained the Zn and one cationic dopant precursors, Zn(O 2CCH 3) 2 and AlCl 3, CrCl 3, or FeCl 3. The deposition was carried out at 500 &degC; on soda-lime glass in air. Compared to singly-doped ZnO thin films, codoped ZnO samples showed better electrical properties. Besides, a minimum sheet resistance, 55.4 Ω/sq, was obtained for Al and F codoped ZnO films after vacuum annealing at 400 &degC;, which was lower than singly-doped ZnO with either Al or F. The transmittance for the Al and F codoped ZnO samples was above 90% in the visible range. This co-spray deposition technique provides a simple and cost-effective way to synthesize metal oxides from incompatible precursors with improved properties.
ContributorsZhou, Bin (Author) / Tao, Meng (Thesis advisor) / Goryll, Michael (Committee member) / Vasileska, Dragica (Committee member) / Yu, Hongbin (Committee member) / Arizona State University (Publisher)
Created2013
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Description
This dissertation aims to demonstrate a new approach to fabricating solar cells for spectrum-splitting photovoltaic systems with the potential to reduce their cost and complexity of manufacturing, called Monolithically Integrated Laterally Arrayed Multiple Band gap (MILAMB) solar cells. Single crystal semiconductor alloy nanowire (NW) ensembles are grown with the alloy

This dissertation aims to demonstrate a new approach to fabricating solar cells for spectrum-splitting photovoltaic systems with the potential to reduce their cost and complexity of manufacturing, called Monolithically Integrated Laterally Arrayed Multiple Band gap (MILAMB) solar cells. Single crystal semiconductor alloy nanowire (NW) ensembles are grown with the alloy composition and band gap changing continuously across a broad range over the surface of a single substrate in a single, inexpensive growth step by the Dual-Gradient Method. The nanowire ensembles then serve as the absorbing materials in a set of solar cells for spectrum-splitting photovoltaic systems.

Preliminary design and simulation studies based on Anderson's model band line-ups were undertaken for CdPbS and InGaN alloys. Systems of six subcells obtained efficiencies in the 32-38% range for CdPbS and 34-40% for InGaN at 1-240 suns, though both materials systems require significant development before these results could be achieved experimentally. For an experimental demonstration, CdSSe was selected due to its availability. Proof-of-concept CdSSe nanowire ensemble solar cells with two subcells were fabricated simultaneously on one substrate. I-V characterization under 1 sun AM1.5G conditions yielded open-circuit voltages (Voc) up to 307 and 173 mV and short-circuit current densities (Jsc) up to 0.091 and 0.974 mA/cm2 for the CdS- and CdSe-rich cells, respectively. Similar thin film cells were also fabricated for comparison. The nanowire cells showed substantially higher Voc than the film cells, which was attributed to higher material quality in the CdSSe absorber. I-V measurements were also conducted with optical filters to simulate a simple form of spectrum-splitting. The CdS-rich cells showed uniformly higher Voc and fill factor (FF) than the CdSe-rich cells, as expected due to their larger band gaps. This suggested higher power density was produced by the CdS-rich cells on the single-nanowire level, which is the principal benefit of spectrum-splitting. These results constitute a proof-of-concept experimental demonstration of the MILAMB approach to fabricating multiple cells for spectrum-splitting photovoltaics. Future systems based on this approach could help to reduce the cost and complexity of manufacturing spectrum-splitting photovoltaic systems and offer a low cost alternative to multi-junction tandems for achieving high efficiencies.
ContributorsCaselli, Derek (Author) / Ning, Cun-Zheng (Thesis advisor) / Tao, Meng (Committee member) / Yu, Hongbin (Committee member) / Vasileska, Dragica (Committee member) / Arizona State University (Publisher)
Created2014
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Description
As the 3rd generation solar cell, quantum dot solar cells are expected to outperform the first 2 generations with higher efficiency and lower manufacture cost. Currently the main problems for QD cells are the low conversion efficiency and stability. This work is trying to improve the reliability as well as

As the 3rd generation solar cell, quantum dot solar cells are expected to outperform the first 2 generations with higher efficiency and lower manufacture cost. Currently the main problems for QD cells are the low conversion efficiency and stability. This work is trying to improve the reliability as well as the device performance by inserting an interlayer between the metal cathode and the active layer. Titanium oxide and a novel nitrogen doped titanium oxide were compared and TiOxNy capped device shown a superior performance and stability to TiOx capped one. A unique light anneal effect on the interfacial layer was discovered first time and proved to be the trigger of the enhancement of both device reliability and efficiency. The efficiency was improved by 300% and the device can retain 73.1% of the efficiency with TiOxNy when normal device completely failed after kept for long time. Photoluminescence indicted an increased charge disassociation rate at TiOxNy interface. External quantum efficiency measurement also inferred a significant performance enhancement in TiOxNy capped device, which resulted in a higher photocurrent. X-ray photoelectron spectrometry was performed to explain the impact of light doping on optical band gap. Atomic force microscopy illustrated the effect of light anneal on quantum dot polymer surface. The particle size is increased and the surface composition is changed after irradiation. The mechanism for performance improvement via a TiOx based interlayer was discussed based on a trap filling model. Then Tunneling AFM was performed to further confirm the reliability of interlayer capped organic photovoltaic devices. As a powerful tool based on SPM technique, tunneling AFM was able to explain the reason for low efficiency in non-capped inverted organic photovoltaic devices. The local injection properties as well as the correspondent topography were compared in organic solar cells with or without TiOx interlayer. The current-voltage characteristics were also tested at a single interested point. A severe short-circuit was discovered in non capped devices and a slight reverse bias leakage current was also revealed in TiOx capped device though tunneling AFM results. The failure reason for low stability in normal devices was also discussed comparing to capped devices.
ContributorsYu, Jialin (Author) / Jabbour, Ghassan E. (Thesis advisor) / Alford, Terry L. (Thesis advisor) / Yu, Hongbin (Committee member) / Arizona State University (Publisher)
Created2011
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Description
GaAs single-junction solar cells have been studied extensively in recent years, and have reached over 28 % efficiency. Further improvement requires an optically thick but physically thin absorber to provide both large short-circuit current and high open-circuit voltage. By detailed simulation, it is concluded that ultra-thin GaAs cells with hundreds

GaAs single-junction solar cells have been studied extensively in recent years, and have reached over 28 % efficiency. Further improvement requires an optically thick but physically thin absorber to provide both large short-circuit current and high open-circuit voltage. By detailed simulation, it is concluded that ultra-thin GaAs cells with hundreds of nanometers thickness and reflective back scattering can potentially offer efficiencies greater than 30 %. The 300 nm GaAs solar cell with AlInP/Au reflective back scattering is carefully designed and demonstrates an efficiency of 19.1 %. The device performance is analyzed using the semi-analytical model with Phong distribution implemented to account for non-Lambertian scattering. A Phong exponent m of ~12, a non-radiative lifetime of 130 ns, and a specific series resistivity of 1.2 Ω·cm2 are determined.

Thin-film CdTe solar cells have also attracted lots of attention due to the continuous improvements in their device performance. To address the issue of the lower efficiency record compared to detailed-balance limit, the single-crystalline Cd(Zn)Te/MgCdTe double heterostructures (DH) grown on InSb (100) substrates by molecular beam epitaxy (MBE) are carefully studied. The Cd0.9946Zn0.0054Te alloy lattice-matched to InSb has been demonstrated with a carrier lifetime of 0.34 µs observed in a 3 µm thick Cd0.9946Zn0.0054Te/MgCdTe DH sample. The substantial improvement of lifetime is due to the reduction in misfit dislocation density. The recombination lifetime and interface recombination velocity (IRV) of CdTe/MgxCd1-xTe DHs are investigated. The IRV is found to be dependent on both the MgCdTe barrier height and width due to the thermionic emission and tunneling processes. A record-long carrier lifetime of 2.7 µs and a record-low IRV of close to zero have been confirmed experimentally.

The MgCdTe/Si tandem solar cell is proposed to address the issue of high manufacturing costs and poor performance of thin-film solar cells. The MBE grown MgxCd1-xTe/MgyCd1-yTe DHs have demonstrated the required bandgap energy of 1.7 eV, a carrier lifetime of 11 ns, and an effective IRV of (1.869 ± 0.007) × 103 cm/s. The large IRV is attributed to thermionic-emission induced interface recombination. These understandings can be applied to fabricating the high-efficiency low-cost MgCdTe/Si tandem solar cell.
ContributorsLiu, Shi (Author) / Zhang, Yong-Hang (Thesis advisor) / Johnson, Shane R (Committee member) / Vasileska, Dragica (Committee member) / Yu, Hongbin (Committee member) / Arizona State University (Publisher)
Created2015
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Description
Photovoltaic (PV) energy has shown tremendous improvements in the past few decades showing great promises for future sustainable energy sources. Among all PV energy sources, III-V-based solar cells have demonstrated the highest efficiencies. This dissertation investigates the two different III-V solar cells with low (III-antimonide) and high (III-nitride) bandgaps.

III-antimonide semiconductors,

Photovoltaic (PV) energy has shown tremendous improvements in the past few decades showing great promises for future sustainable energy sources. Among all PV energy sources, III-V-based solar cells have demonstrated the highest efficiencies. This dissertation investigates the two different III-V solar cells with low (III-antimonide) and high (III-nitride) bandgaps.

III-antimonide semiconductors, particularly aluminum (indium) gallium antimonide alloys, with relatively low bandgaps, are promising candidates for the absorption of long wavelength photons and thermophotovoltaic applications. GaSb and its alloys can be grown metamorphically on non-native substrates such as GaAs allowing for the understanding of different multijunction solar cell designs. The work in this dissertation presents the molecular beam epitaxy growth, crystal quality, and device performance of AlxGa1−xSb solar cells grown on GaAs substrates. The motivation is on the optimization of the growth of AlxGa1−xSb on GaAs (001) substrates to decrease the threading dislocation density resulting from the significant lattice mismatch between GaSb and GaAs. GaSb, Al0.15Ga0.85Sb, and Al0.5Ga0.5Sb cells grown on GaAs substrates demonstrate open-circuit voltages of 0.16, 0.17, and 0.35 V, respectively. In addition, a detailed study is presented to demonstrate the temperature dependence of (Al)GaSb PV cells.

III-nitride semiconductors are promising candidates for high-efficiency solar cells due to their inherent properties and pre-existing infrastructures that can be used as a leverage to improve future nitride-based solar cells. However, to unleash the full potential of III-nitride alloys for PV and PV-thermal (PVT) applications, significant progress in growth, design, and device fabrication are required. In this dissertation, first, the performance of

ii

InGaN solar cells designed for high temperature application (such as PVT) are presented showing robust cell performance up to 600 ⁰C with no significant degradation.

In the final section, extremely low-resistance GaN-based tunnel junctions with different structures are demonstrated showing highly efficient tunneling characteristics with negative differential resistance (NDR). To improve the efficiency of optoelectronic devices such as UV emitters the first AlGaN tunnel diode with Zener characteristic is presented. Finally, enabled by GaN tunnel junction, the first tunnel contacted InGaN solar cell with a high VOC value of 2.22 V is demonstrated.
ContributorsVadiee, Ehsan (Author) / Honsberg, C. (Christiana B.) (Thesis advisor) / Doolittle, William A (Thesis advisor) / Arizona State University (Publisher)
Created2019
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Description
Semiconductor nanostructures are promising building blocks for light management in thin silicon solar cells and silicon-based tandems due their tunable optical properties. The present dissertation is organized along three main research areas: (1) characterization and modeling of III-V nanowires as active elements of solar cell tandems, (2) modeling of silicon

Semiconductor nanostructures are promising building blocks for light management in thin silicon solar cells and silicon-based tandems due their tunable optical properties. The present dissertation is organized along three main research areas: (1) characterization and modeling of III-V nanowires as active elements of solar cell tandems, (2) modeling of silicon nanopillars for reduced optical losses in ultra-thin silicon solar cells, and (3) characterization and modeling of nanoparticle-based optical coatings for light management.

First, the recombination mechanisms in polytype GaAs nanowires are studied through photoluminescence measurements coupled with rate equation analysis. When photons are absorbed in polytype nanowires, electrons and holes quickly thermalize to the band-edges of the zinc-blende and wurtzite phases, recombining indirectly in space across the type-II offset. Using a rate equation model, different configurations of polytype defects along the nanowire are investigated, which compare well with experiment considering spatially indirect recombination between different polytypes, and defect-related recombination due to twin planes and other defects. The presented analysis is a path towards predicting the performance of nanowire-based solar cells.

Following this topic, the optical mechanisms in silicon nanopillar arrays are investigated using full-wave optical simulations in comparison to measured reflectance data. The simulated electric field energy density profiles are used to elucidate the mechanisms contributing to the reduced front surface reflectance. Strong forward scattering and resonant absorption are observed for shorter- and longer- aspect ratio nanopillars, respectively, with the sub-wavelength periodicity causing additional diffraction. Their potential for light-trapping is investigated using full-wave optical simulation of an ultra-thin nanostructured substrate, where the conventional light-trapping limit is exceeded for near-bandgap wavelengths.

Finally, the correlation between the optical properties of silicon nanoparticle layers to their respective pore size distributions is investigated using optical and structural characterization coupled with full-wave optical simulation. The presence of

scattering is experimentally correlated to wider pore size distributions obtained from nitrogen adsorption measurements. The correlation is validated with optical simulation of random and clustered structures, with the latter approximating experimental. Reduced structural inhomogeneity in low-refractive-index nanoparticle inter-layers at the metal/semiconductor interface improves their performance as back reflectors, while reducing parasitic absorption in the metal.
ContributorsVulic, Natasa (Author) / Goodnick, Stephen M (Thesis advisor) / Honsberg, C. (Christiana B.) (Committee member) / Holman, Zachary C (Committee member) / Smith, David J. (Committee member) / Arizona State University (Publisher)
Created2019
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Description
The larger tolerance to lattice mismatch in growth of semiconductor nanowires (NWs) offers much more flexibility for achieving a wide range of compositions and bandgaps via alloying within a single substrate. The bandgap of III-V InGaAsP alloy NWs can be tuned to cover a wide range of (0.4, 2.25) eV,

The larger tolerance to lattice mismatch in growth of semiconductor nanowires (NWs) offers much more flexibility for achieving a wide range of compositions and bandgaps via alloying within a single substrate. The bandgap of III-V InGaAsP alloy NWs can be tuned to cover a wide range of (0.4, 2.25) eV, appealing for various optoelectronic applications such as photodetectors, solar cells, Light Emitting Diodes (LEDs), lasers, etc., given the existing rich knowledge in device fabrication based on these materials.

This dissertation explores the growth of InGaAsP alloys using a low-cost method that could be potentially important especially for III-V NW-based solar cells. The NWs were grown by Vapor-Liquid-Solid (VLS) and Vapor-Solid (VS) mechanisms using a Low-Pressure Chemical Vapor Deposition (LPCVD) technique. The concept of supersaturation was employed to control the morphology of NWs through the interplay between VLS and VS growth mechanisms. Comprehensive optical and material characterizations were carried out to evaluate the quality of the grown materials.

The growth of exceptionally high quality III-V phosphide NWs of InP and GaP was studied with an emphasis on the effects of vastly different sublimation rates of the associated III and V elements. The incorporation of defects exerted by deviation from stoichiometry was examined for GaP NWs, with an aim towards maximization of bandedge-to-defect emission ratio. In addition, a VLS-VS assisted growth of highly stoichiometric InP thin films and nano-networks with a wide temperature window from 560◦C to 720◦C was demonstrated. Such growth is shown to be insensitive to the type of substrates such as silicon, InP, and fused quartz. The dual gradient method was exploited to grow composition-graded ternary alloy NWs of InGaP, InGaAs, and GaAsP with different bandgaps ranging from 0.6 eV to 2.2 eV, to be used for making laterally-arrayed multiple bandgap (LAMB) solar cells. Furthermore, a template-based growth of the NWs was attempted based on the Si/SiO2 substrate. Such platform can be used to grow a wide range of alloy nanopillar materials, without being limited by typical lattice mismatch, providing a low cost universal platform for future PV solar cells.
ContributorsHashemi Amiri, Seyed Ebrahim (Author) / Ning, Cun-Zheng (Thesis advisor) / Petuskey, William (Committee member) / Yu, Hongbin (Committee member) / Arizona State University (Publisher)
Created2018
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Description
The state of the solar industry has reached a point where significant advancements in efficiency will require new materials and device concepts. The material class broadly known as the III-N's have a rich history as a commercially successful semiconductor. Since discovery in 2003 these materials have shown promise for the

The state of the solar industry has reached a point where significant advancements in efficiency will require new materials and device concepts. The material class broadly known as the III-N's have a rich history as a commercially successful semiconductor. Since discovery in 2003 these materials have shown promise for the field of photovoltaic solar technologies. However, inherent material issues in crystal growth and the subsequent effects on device performance have hindered their development. This thesis explores new growth techniques for III-N materials in tandem with new device concepts that will either work around the previous hindrances or open pathways to device technologies with higher theoretical limits than much of current photovoltaics. These include a novel crystal growth reactor, efforts in production of better quality material at faster rates, and development of advanced photovoltaic devices: an inversion junction solar cell, material work for hot carrier solar cell, ground work for a selective carrier contact, and finally a refractory solar cell for operation at several hundred degrees Celsius.
ContributorsWilliams, Joshua J (Author) / Honsberg, C. (Christiana B.) (Thesis advisor) / Goodnick, Stephen M. (Thesis advisor) / Williamson, Todd L. (Committee member) / Alford, Terry L. (Committee member) / King, Richard R. (Committee member) / Arizona State University (Publisher)
Created2016
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Description
III-V multijunction solar cells have demonstrated record efficiencies with the best device currently at 46 % under concentration. Dilute nitride materials such as GaInNAsSb have been identified as a prime choice for the development of high efficiency, monolithic and lattice-matched multijunction solar cells as they can be lattice-matched to both

III-V multijunction solar cells have demonstrated record efficiencies with the best device currently at 46 % under concentration. Dilute nitride materials such as GaInNAsSb have been identified as a prime choice for the development of high efficiency, monolithic and lattice-matched multijunction solar cells as they can be lattice-matched to both GaAs and Ge substrates. These types of cells have demonstrated efficiencies of 44% for terrestrial concentrators, and with their upright configuration, they are a direct drop-in product for today’s space and concentrator solar panels. The work presented in this dissertation has focused on the development of relatively novel dilute nitride antimonide (GaNAsSb) materials and solar cells using plasma-assisted molecular beam epitaxy, along with the modeling and characterization of single- and multijunction solar cells.

Nitrogen-free ternary compounds such as GaInAs and GaAsSb were investigated first in order to understand their structural and optical properties prior to introducing nitrogen. The formation of extended defects and the resulting strain relaxation in these lattice-mismatched materials is investigated through extensive structural characterization. Temperature- and power-dependent photoluminescence revealed an inhomogeneous distribution of Sb in GaAsSb films, leading to carrier localization effects at low temperatures. Tuning of the growth parameters was shown to suppress these Sb-induced localized states.

The introduction of nitrogen was then considered and the growth process was optimized to obtain high quality GaNAsSb films lattice-matched to GaAs. Near 1-eV single-junction GaNAsSb solar cells were produced. The best devices used a p-n heterojunction configuration and demonstrated a current density of 20.8 mA/cm2, a fill factor of 64 % and an open-circuit voltage of 0.39 V, corresponding to a bandgap-voltage offset of 0.57 V, comparable with the state-of-the-art for this type of solar cells. Post-growth annealing was found to be essential to improve Voc but was also found to degrade the material quality of the top layers. Alternatives are discussed to improve this process. Unintentional high background doping was identified as the main factor limiting the device performance. The use of Bi-surfactant mediated growth is proposed for the first time for this material system to reduce this background doping and preliminary results are presented.
ContributorsMaros, Aymeric (Author) / King, Richard R. (Thesis advisor) / Honsberg, C. (Christiana B.) (Committee member) / Goodnick, Stephen M. (Committee member) / Ponce, Fernando A. (Committee member) / Arizona State University (Publisher)
Created2017