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published_or_final_version / Physics / Doctoral / Doctor of Philosophy

Intensive research interests in condensed matter physics have been focused at the strongly correlated electron systems. Most of the efforts were devoted in hole-doped manganites with a double exchange interaction between Mn3+/Mn4+. Recently, tetravalent ions substitution has also stimuli much attention as a supplement for the hole-doping. Such electron-doped manganites may be of great potential for the development of all-manganites devices. Manganites are extremely sensitive to external disturbances, such as magnetic fields, electric fields, currents, mechanical strain, and photo illumination, etc. These extraordinary properties make manganites promising for practical applications. In this thesis, the field modulation on physical properties in electron/hole-doped manganites films and heterojunctions were investigated. The effects of tetravalent hafnium doping on the structural, transport, and magnetic properties of polycrystalline La1-xHfxMnO3(LHMO) (0.05 ≤x ≤0.3) were studied systematically. A phase diagram was obtained for the first time through magnetization and resistance measurements in a broad temperature range. An abnormal enhancement of magnetization was observed at about 42 K. It was further confirmed that the second magnetic phase MnO2in LHMO gives rise to such a phenomenon. The dynamic magnetic properties of LHMO, such as relaxation and aging processes, were studied, demonstrating a spin-glass state at low temperature accompanied by a ferromagnetic phase. Heterojunctions composed of n-type SrTiO3-δand p-type GaAs exhibited excellent rectifying behavior from 40K to room temperature. The photocarrier injection effect and a colossal photo-resistance were observed. Strong dependences on both temperature and bias voltage were found as well, which might be under stood by considering the band structure of the formed p-njunction. By employing an ultrathin SrTiO3buffer layer,La0.8Ca0.2MnO3films could be epitaxially grown on GaAs substrates. The heterostructures exhibit good rectifying behavior with a paramagnetic-ferromagnetic transition at ~200K. The variation of diffusion voltage with temperature in these heterostructures could be explained by the effects of the Hund’s rule coupling between the La0.8Ca0.2MnO3and the buffer layer. The effects of the strain induced by ferroelectric poling on the magnetic and electric properties have been investigated by using 0.67Pb(Mg1/3Nb2/3)O3-0.33PbTiO3(PMN-PT) substrates. The polarization of the PMN-PT crystal reduces the biaxial tensile strain in the formed La0.9Hf0.1MnO3layer.It results in a significant decrease in resistance and an enhancement of the phase transition temperature as well as the magnetization. The impact of the lattice strain on the charge/orbital ordering state was also been studied. The modification of charge/orbital ordering phase by the electric fields and ferroelectric polarization suggested that the unstable states in the manganites are sensitive to the strain. Heterojunctions of La1-xHfxMnO3/Nb:SrTiO3 were fabricated and investigated under different fields (electric, magnetic and optic). These heterojunctions exhibited excellent rectifying behavior in a wide temperature range. Their properties could be significantly modulated by magnetic fields. Prominent photovoltaic effect was also observed in the formed junctions. / published_or_final_version / Physics / Doctoral / Doctor of Philosophy

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A hybrid organic/inorganic heterojunction has been fabricated using an n-type silicon wafer (< 111 >, 3 < ρ < 6 Ω · cm) and a p-type polymer, PEDOT:PSS (ρ = 1 Ω · cm). Standard fabrication techniques such as vacuum deposition and spin coating are required for fabrication and have been employed. I-V characteristics have been measured under both dark and illuminated conditions for different thicknesses of PEDOT:PSS as defined by the spin rate at which the polymer has been spin coated. The data has been analyzed and figures of merit such as series resistance, short circuit current, open circuit voltage, fill factor and efficiency have been calculated. The efficiency ranges to values as high as 0.63%, while the fill factor has been observed to be as high as 57%, both of which are improvements on previously reported hybrid heterojunctions built on n-type silicon wafers.

Bulk heterojunction (BHJ) organic photovoltaic (OPV) is one of the most promising techniques to generate electricity with advantages of flexibility, solution processing and capability for large area device fabrication. Although the power conversion efficiency (PCE) of BHJ solar cells has already achieved over 13%, there are still problems remain to be solved. This thesis presents the binary and ternary organic BHJ devices with alternative donor:acceptor (D:A) ratios, and the charge transport properties and electronic interactions in their BHJ films. In a high performance BHJ solar cell, the commonly optimized D:A weight ratio is about 1:x, where x is commonly in excess of 1.5, when PC71BM is used as the acceptor. We demonstrated how to achieve high PCEs of BHJ solar cells by enriching the D:A weight ratios. The PCEs of the re-optimized cells were improved for the PTB7:PC71BM, PCDTBT:PC71BM, PDTSTPD:PC71BM devices. Current-voltage (JV) and admittance spectroscopy (AS) measurements indicate enhanced hole mobilities for the polymer-rich BHJs based on PTB7, PCDTBT, and PDTSTPD. At the same time, although the relative weight ratio of PC71BM is reduced, the electron mobilities are maintained due to the dispersion of fullerene domains by increased DIO concentrations. The active layer thickness of most optimized BHJ solar cells is about 100nm. The thin active layer is unfavorable for optical absorption and film coating. We employed a ternary strategy to address this problem, and the thick-film BHJ devices can retain 90% PCEs of their optimized thin-film devices. Three model systems were studied, involving PTB7:PC71BM, PTB7-Th:PC71BM and P3HT:PCBM BHJs. Into these BHJs, a ternary component, p-DTS(fbtth2)2 (DTS) is introduced. With DTS, the corresponding thick film devices have significantly improved PCEs. The ternary component DTS improves hole mobility and reduces sub-bandgap trap states. Both observations are well correlated with improved FFs of the ternary BHJ cells. Photothermal deflection spectroscopy (PDS) and 1H nuclear magnetic resonance (1H NMR) results indicate that DTS behaves as conducting bridges in between two neighboring polymer segments. Most lab-based BHJ solar cells are optimized by their power conversion efficiencies (PCEs). We challenge this conventional view by showing that BHJ cells using fullerene acceptors should be optimized by their fill-factors (FFs). With the optimized-FF approach, BHJ cells tend to have higher fullerene content when compared to the BHJ cells that are optimized by PCEs. The FF-optimized BHJ cells have slightly reduced PCEs (due to smaller Jscs) compared to the PCE-optimized cells. Yet, FF-optimized cells enjoy a much better thermal stability. We demonstrate that these FF-optimized BHJs possess better-balanced electron-to-hole mobility ratios due to weakly field-dependent electron mobilities. The improved mobility ratio suppresses carrier recombination. Our results suggest that BHJ cells optimized by their PCEs should be meta-stable, and other D:A ratios should be considered for practical BHJ cell development.

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published_or_final_version / Physics / Doctoral / Doctor of Philosophy

No description available.

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