本論文研究主題是利用不同金屬氧化物奈米結構作為反式高分子混摻太陽能電池中的電子接受材料與傳輸通道。其中，電池內的載子動力學（如：載子的分離、再結合與傳輸特性）則分別利用時間解析螢光光譜(time-resolved photoluminescence, TRPL)、阻抗光譜(impedance spectroscopy, IS)與光強度調致光電流光譜(intensity-modulated photocurrent spectroscopy, IMPS)等分析方法來鑑定與了解載子於元件中的運作特性。
本研究的第一部份中，我們以TiO2奈米結構陣列與共軛高分子P3HT建構混摻太陽能電池。藉由染料分子（如：Z907與D149）修飾混摻太陽能電池中的TiO2/P3HT之界面，能夠有效地提升整體電池效率。此外，我們整合循環伏安法(cyclic voltammetry, CV)與Kelvin原子力顯微鏡(Kelvin probe force microscope, KPM)兩項實驗，成功地建立平衡狀態下的元件能階圖。由平衡狀態的元件能階圖顯示，作為界面修飾的染料分子在元件中，不僅能夠符合在TiO2/P3HT界面中，作為分別傳遞電子與電洞成為載子傳輸橋梁，還能夠因染料分子兩端的親疏水端，成功降低有機/無機界面的化學不匹配性，並提升高分子的排列規則性。除此之外，本研究導入三維擬單晶的TiO2樹枝狀奈米結構陣列於混摻太陽能電池當中，以藉由三維TiO2結構，有效地增加激子(exciton)解離面積。因此，由染料分子D149所修飾之TiO2奈米樹枝狀結構陣列/P3HT混摻太陽能電池可得到電池效率3.12%。
在第二部份，本研究整合規則奈米結構陣列與塊材異質接面(bulk heterojunction, BHJ)兩項結構優點於同一個混摻太陽能電池當中。此元件是利用旋轉塗佈(spin-coating)內含ZnO反應前驅物與高分子P3HT的主動層溶液至TiO2奈米柱陣列上。在塗佈期間，ZnO奈米網絡則能夠成功地即時(in situ)合成於高分子P3HT當中，並滲入至TiO2奈米柱的間隙當中，成功建構混摻太陽能電池。TiO2奈米柱陣列在此元件中，不僅作為從導電基板所延伸之電子傳輸與接收通道，且作為有效程載ZnO/P3HT混摻膜之骨架。由於此即時形成的ZnO/P3HT混摻膜擁有良好的載子分離效率，藉由增加TiO2奈米柱陣列的厚度來提升此ZnO/P3HT混摻膜厚度，能夠有效地增加光捕獲效率，使此電池在無任何界面修飾的情況下電池效率增加至2.46%。
最後一部份，本研究導入核殼結構的金與二氧化矽(Au@silica)奈米顆粒至金屬氧化物奈米網絡/P3HT的混摻膜當中。其中，由時域有限差分法(finite difference time domain, FDTD)模擬結果顯示，當Au@silica奈米顆粒在照光情況下，會產生不對稱的四極(quadrupole)之Fano共振於奈米顆粒表面。此奈米顆粒表面的Fano共振所誘發電場能夠有效地提升載子分離效率，本研究則以TRPL實驗中，額外掛載綠光雷射，能夠直接地證明此結果。此外，添加Au@silica奈米顆粒至混摻膜中會額外提升P3HT的結晶度，這也是提高電池電流的原因之一。相對於未添加Au@silica奈米顆粒的混摻太陽能電池，有導入奈米顆粒的電池之短路電流能夠提升30%。

In this work, we demonstrated metal oxide nanoarchitectures as electron acceptors and transport channels in inverted-type poly(3-hexylthiophene) (P3HT)-based hybrid solar cells. Photocarrier dynamics (charge separation, recombination, and transport properties) of hybrid solar cells are investigated and characterized by time-resolved photoluminescence (TRPL), impedance spectroscopy (IS), and intensity-modulated photocurrent spectroscopy (IMPS) measurements.
In the first part, we demonstrated ordered hybrid polymer solar cells fabricated by using rutile TiO2 nanoarchitecture (nanorod (NR) and nanodendrite (ND)) arrays and P3HT. Interfacial modification with dye molecules in this work can significantly improve the cell performance of ordered TiO2 nanorod (NR)–P3HT hybrid solar cells. Equilibrium energy band diagrams of dye-modified TiO2 NR−P3HT hybrid solar cells are established by integrating cyclic voltammetry (CV) and Kelvin probe force microscope (KPM) measurements. The dye molecules, Z907 and D149, in the hybrid solar cells not only provide an appropriate band alignment between TiO2/P3HT interfaces, but also improve the chemical compatibility of interface morphology of the hybrids. Besides, three-dimensional TiO2 nanodendrite (ND) arrays are employed to further increase the interfacial area in hybrid solar cells. A power conversion efficiency (PCE) of 3.12% is achieved in the D149-modified TiO2 ND array/P3HT hybrid solar cell.
Second, we demonstrated a nanoarchitectural hybrid solar cell, integrating an ordered TiO2 NR array and a bulk heterojunction (BHJ) of ZnO nanoparticle (NP)/P3HT into cells. The cell was fabricated by infiltrating a solution containing diethylzinc (DEZ) and P3HT into the interstices of TiO2 NRs. An inorganic network composed of tiny ZnO nanocrystals is in situ generated in the active layer within the interstices of TiO2 NRs. The TiO2 NR arrays in hybrid solar cell not only serve as an electron transporter/collector extended from the FTO electrode to sustain the efficient electron collection, but also serve as a scaffold to hold the sufficient amount of ZnO/P3HT hybrid. The in-situ-generated ZnO NP/P3HT hybrid with superior charge separation efficiency can be thickened in the presence of a TiO2 NR array for increasing the light-harvesting efficiency. An efficiency of 2.46% is therefore attained in the TiO2 NR−ZnO/P3HT hybrid solar cell without interfacial modification.
At last, we incorporated a gold−silica core−shell (Au@silica) nanoparticle (NP) into the metal oxide nanoarchitecture/P3HT hybrid. Finite difference time domain (FDTD) simulation shows the existence of an asymmetric quadrupole of Fano resonance on the Au@silica-NP surface. The charge separation enhancement in the Au@silica-NP-incorporated hybrid contributed to the Fano resonance induced electric field is directly evidenced by TRPL measurements with an additional green light illumination. The increase of the degree of P3HT order in the hybrid by adding Au@silica NPs into the hybrid active layer may also enhance current density in the cell. Compared to the metal oxide nanoarchitecture/P3HT hybrid solar cell, a 30% enhancement of short-circuit current density (Jsc) is attained in the P3HT-based nanoarchitectural Fano solar cell (NAFSC) with Au@silica NPs.

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