有机—无机杂化光伏电池中的界面效应及调控研究
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摘要
本论文以硅-共轭导电聚合物杂化光伏器件为基础，研究了硅/聚合物的界面形貌和界面钝化对器件性能的影响，深入讨论了硅/聚合物的界面效应。通过对硅/聚合物界面的调控，制备了高效稳定的硅纳米线阵列-有机杂化光伏器件。其中，硅纳米线阵列的制备采用金属辅助催化湿法化学刻蚀的方法；硅纳米线阵列的表面形貌可以通过一种简单的化学反应刻蚀的方法进行有效的调控；硅纳米线阵列表面的能级结构、缺陷态密度、载流子复合速率和化学稳定性可以通过利用不同的钝化层对其表面进行钝化来进行有效的调控。利用这种表面形貌、电学性能和化学稳定性可控的硅纳米线阵列分别与共轭导电聚合物聚3-己基噻吩（P3HT）和聚苯乙烯磺酸掺杂的聚3,4二氧乙烯噻吩（PEDOT:PSS）制备了高效稳定的有机/无机杂化光伏器件，光电转换效率超过10%。通过扫描电子显微镜、透射电子显微镜、紫外-可见分光光度计、X射线光电子能谱、瞬态光电压（光电流）衰减等测试手段对器件的工作原理以及硅/聚合物的界面效应进行了系统的分析和表征。结果表明，硅纳米线阵列的表面形貌和表面钝化是影响硅-聚合物杂化光伏器件性能的重要因素。利用合适表面形貌的硅纳米线阵列和对其表面进行有效的钝化修饰是制备高效率杂化光伏器件的先决条件。这是由于硅纳米线阵列的表面形貌和表面钝化主导了硅-聚合物杂化光伏器件中界面的载流子复合速率和载流子寿命。主要工作包括：
1.采用金属辅助催化湿法化学反应刻蚀的方法制备了结构规整的硅纳米线阵列。通过对其进行氧化刻蚀反应使其表面形貌得到了有效的调控；通过对其表面进行不同的钝化处理使其表面的能级结构、缺陷态密度、载流子复合速率和化学稳定性得到了有效的调控。
2.利用表面形貌、电学性能和化学稳定性可控的单晶硅基底与共轭导电聚合物P3HT制备了有机-无机杂化光伏器件。通过电流-电压测试、外量子效率光谱响应等测试手段考察了器件的光伏性能；通过扫描电子显微镜、紫外-可见分光光度计、紫外光电子能谱等测试手段考察了器件中的界面效应。结果表明，通过对基底的表面形貌控制和表面进行钝化可以有效地提高器件的光伏性能。
3.利用不同表面形貌和不同表面钝化层的硅纳米线阵列和共轭导电聚合物P3HT制备了具有三维径向结构的杂化异质结光伏器件（HOT电池）。通过电流-电压测试、外量子效率光谱响应等测试手段考察了器件的光伏性能；通过对器件的暗电流拟合分析考察了器件的界面形貌和界面钝化对器件性能的影响。结果表明，硅纳米线阵列需要具有合适的密度使得聚合物能够更好地均匀覆盖其表面从而制备出高效率的光伏器件。
4.利用不同表面形貌的硅纳米线阵列和导电共轭聚合物PEDOT:PSS制备了杂化肖特基异质结光伏电池。通过电流-电压测试和外量子效率光谱响应等测试手段考察了器件的光伏性能；通过对器件的暗电流拟合分析和瞬态光电压衰减测试分析了界面形貌与器件性能的关系以及器件中载流子的分离及传输的理论依据。结果表明，在这种基于硅纳米线阵列和PEDOT:PSS的杂化光伏器件中，硅纳米线阵列基底需要具有合适的硅线长度和密度使器件具有较高的陷光性能和较低的表面载流子复合速率，从而使得杂化光伏器件具有较好的光伏性能。
5.采用不同的有机单分子层对硅纳米线阵列表面进行钝化修饰，利用略角反射-傅里叶转换红外光谱和X射线光电子能谱考察了其钝化效果。利用不同有机单分子层钝化修饰得到的具有不同钝化程度的硅纳米线阵列与共轭导电聚合物PEDOT:PSS制备了杂化肖特基光伏器件。通过电流-电压测试、外量子效率光谱响应等测试手段考察了器件的光伏性能；通过对器件的暗电流拟合分析和瞬态光电压（光电流）衰减测试分析了界面钝化与器件性能的关系以及器件中电荷的分离及传输的理论依据。结果表明，表面钝化程度完全的硅纳米线阵列基底具有较小的缺陷态密度和载流子复合速率，基于这种混合有机单分子层钝化修饰的硅纳米线阵列和PEDOT:PSS杂化光伏器件具有较高的效率和较好的稳定性。
This thesis was based on the silicon (Si)-conjugated polymer hybrid solar cells. Inthis thesis, the device performance influenced by the morphology and passivation ofsilicon substrates surfaces were investigated. The device with high performance andstability was fabricated by controling the interface of Si/polymer. Si nanowire arrays(SiNWs) were fabricated by metal-assisted chemical etching method, and their densitieswere tuned through slowly chemical etching. The surface density of trap states and thevelocity of surface carrier recombination were dramatically reduced utilizing a two-stepmethod of chloridization/alkylation. High efficiency of over10%and stableorganic/inorganic hybrid photovoltaic devices were fabricated based on the densitycontrollable, organic monolayer surface passivated SiNWs and poly(3-hexylthiophene)(P3HT) or poly(3,4-ethylenedioxythiophene)/poly(styrenesulfonate)(PEDOT:PSS).Scanning electron microscope (SEM), transmission electron microscope (TEM),UV-Vis spectrophotometer (UV-Vis), X-ray photoelectron spectroscopy (XPS), transientphotovoltage (photocurrent) decay were used to analyse the interface engineeringsystematically. The results indicated that the surface morphology and passivation playimportant roles on device performance because they dominate the charge recombinationprocess. My works maily consist of following parts:
1. Preparation of SiNWs with regular structure by metal-assisted chemical etchingmethod to fabricate. The controllable surface morphology of SiNWs was achievedthrough a simple and efficient chemical etching method. The controllable surface energydiagram, the density of trap states, charge recombination velocity and chemical stabilitywere achieved through the surface passivation.
2. Fabrication of Si/P3HT hybrid photovoltaic devices with different surfacemorphology and passivation layer. The device performance was characterized bycurrenet-volatage (J-V) and external quantum efficiency (EQE), and the interfacemorphology were measured by SEM, TEM, and UV-Vis. The results indicated thatdevice performance could be enhanced by optimizing the surface morphology and passivaiton of Si substrates.
3. Fabrication of devices with the structure of heterojuction with organic thinlayer were fabricated utilizing Si substrates and P3HT. SEM, TEM were used tocharacterize the device structure; J-V and EQE were used to evaluate the deviceperformance; the fitting of dark current was utilized to investigated the effect of deviceperformance influenced by the morphology and passivation of Si substrates surfaces.The results indicated that the desity of SiNWs should be suitable so as to formcontinuous organic films.
4. Fabrication of hybrid Schottky heterojunction photovoltaic solar cells based onSiNWswith different morphology and PEDOT:PSS. The device structure wascharacterized by SEM, UV-Vis etc.; the device performance was characterized by J-Vand EQE test; the interface quality was investigated by fitting dark current and transientphotovoltage decay test. The results indicated that the density and length of SiNWsshould be suitbale to balance the light trpping and surface trap states.
5. Passivation of the Si surfaces to suppress the charge recombination. The alkygroup coverage ratio was exactly demonstrated by grazing angle attenuated totalreflectance Fourier-transform infrared spectroscopy (GATR-FTIR) and XPS. HybridSchottky photovoltaic devices based on PEDOT:PSS and different coverage ratiopassivated SiNWs by varying organic monolayer were fabricated. The device structurewas characterized by SEM, TEM and UV-Vis. The device performance wascharacterized by J-V and EQE test; the interface engineering was investigated by fittingdark current and transient photovoltage (photocurrent) decay test. The results indicatedthat the mixed organic monolayer could passivate SiNWs surface completely andenhance the device performance efficiently.
1.采用金属辅助催化湿法化学反应刻蚀的方法制备了结构规整的硅纳米线阵列。通过对其进行氧化刻蚀反应使其表面形貌得到了有效的调控；通过对其表面进行不同的钝化处理使其表面的能级结构、缺陷态密度、载流子复合速率和化学稳定性得到了有效的调控。
2.利用表面形貌、电学性能和化学稳定性可控的单晶硅基底与共轭导电聚合物P3HT制备了有机-无机杂化光伏器件。通过电流-电压测试、外量子效率光谱响应等测试手段考察了器件的光伏性能；通过扫描电子显微镜、紫外-可见分光光度计、紫外光电子能谱等测试手段考察了器件中的界面效应。结果表明，通过对基底的表面形貌控制和表面进行钝化可以有效地提高器件的光伏性能。
3.利用不同表面形貌和不同表面钝化层的硅纳米线阵列和共轭导电聚合物P3HT制备了具有三维径向结构的杂化异质结光伏器件（HOT电池）。通过电流-电压测试、外量子效率光谱响应等测试手段考察了器件的光伏性能；通过对器件的暗电流拟合分析考察了器件的界面形貌和界面钝化对器件性能的影响。结果表明，硅纳米线阵列需要具有合适的密度使得聚合物能够更好地均匀覆盖其表面从而制备出高效率的光伏器件。
4.利用不同表面形貌的硅纳米线阵列和导电共轭聚合物PEDOT:PSS制备了杂化肖特基异质结光伏电池。通过电流-电压测试和外量子效率光谱响应等测试手段考察了器件的光伏性能；通过对器件的暗电流拟合分析和瞬态光电压衰减测试分析了界面形貌与器件性能的关系以及器件中载流子的分离及传输的理论依据。结果表明，在这种基于硅纳米线阵列和PEDOT:PSS的杂化光伏器件中，硅纳米线阵列基底需要具有合适的硅线长度和密度使器件具有较高的陷光性能和较低的表面载流子复合速率，从而使得杂化光伏器件具有较好的光伏性能。
5.采用不同的有机单分子层对硅纳米线阵列表面进行钝化修饰，利用略角反射-傅里叶转换红外光谱和X射线光电子能谱考察了其钝化效果。利用不同有机单分子层钝化修饰得到的具有不同钝化程度的硅纳米线阵列与共轭导电聚合物PEDOT:PSS制备了杂化肖特基光伏器件。通过电流-电压测试、外量子效率光谱响应等测试手段考察了器件的光伏性能；通过对器件的暗电流拟合分析和瞬态光电压（光电流）衰减测试分析了界面钝化与器件性能的关系以及器件中电荷的分离及传输的理论依据。结果表明，表面钝化程度完全的硅纳米线阵列基底具有较小的缺陷态密度和载流子复合速率，基于这种混合有机单分子层钝化修饰的硅纳米线阵列和PEDOT:PSS杂化光伏器件具有较高的效率和较好的稳定性。
This thesis was based on the silicon (Si)-conjugated polymer hybrid solar cells. Inthis thesis, the device performance influenced by the morphology and passivation ofsilicon substrates surfaces were investigated. The device with high performance andstability was fabricated by controling the interface of Si/polymer. Si nanowire arrays(SiNWs) were fabricated by metal-assisted chemical etching method, and their densitieswere tuned through slowly chemical etching. The surface density of trap states and thevelocity of surface carrier recombination were dramatically reduced utilizing a two-stepmethod of chloridization/alkylation. High efficiency of over10%and stableorganic/inorganic hybrid photovoltaic devices were fabricated based on the densitycontrollable, organic monolayer surface passivated SiNWs and poly(3-hexylthiophene)(P3HT) or poly(3,4-ethylenedioxythiophene)/poly(styrenesulfonate)(PEDOT:PSS).Scanning electron microscope (SEM), transmission electron microscope (TEM),UV-Vis spectrophotometer (UV-Vis), X-ray photoelectron spectroscopy (XPS), transientphotovoltage (photocurrent) decay were used to analyse the interface engineeringsystematically. The results indicated that the surface morphology and passivation playimportant roles on device performance because they dominate the charge recombinationprocess. My works maily consist of following parts:
1. Preparation of SiNWs with regular structure by metal-assisted chemical etchingmethod to fabricate. The controllable surface morphology of SiNWs was achievedthrough a simple and efficient chemical etching method. The controllable surface energydiagram, the density of trap states, charge recombination velocity and chemical stabilitywere achieved through the surface passivation.
2. Fabrication of Si/P3HT hybrid photovoltaic devices with different surfacemorphology and passivation layer. The device performance was characterized bycurrenet-volatage (J-V) and external quantum efficiency (EQE), and the interfacemorphology were measured by SEM, TEM, and UV-Vis. The results indicated thatdevice performance could be enhanced by optimizing the surface morphology and passivaiton of Si substrates.
3. Fabrication of devices with the structure of heterojuction with organic thinlayer were fabricated utilizing Si substrates and P3HT. SEM, TEM were used tocharacterize the device structure; J-V and EQE were used to evaluate the deviceperformance; the fitting of dark current was utilized to investigated the effect of deviceperformance influenced by the morphology and passivation of Si substrates surfaces.The results indicated that the desity of SiNWs should be suitable so as to formcontinuous organic films.
4. Fabrication of hybrid Schottky heterojunction photovoltaic solar cells based onSiNWswith different morphology and PEDOT:PSS. The device structure wascharacterized by SEM, UV-Vis etc.; the device performance was characterized by J-Vand EQE test; the interface quality was investigated by fitting dark current and transientphotovoltage decay test. The results indicated that the density and length of SiNWsshould be suitbale to balance the light trpping and surface trap states.
5. Passivation of the Si surfaces to suppress the charge recombination. The alkygroup coverage ratio was exactly demonstrated by grazing angle attenuated totalreflectance Fourier-transform infrared spectroscopy (GATR-FTIR) and XPS. HybridSchottky photovoltaic devices based on PEDOT:PSS and different coverage ratiopassivated SiNWs by varying organic monolayer were fabricated. The device structurewas characterized by SEM, TEM and UV-Vis. The device performance wascharacterized by J-V and EQE test; the interface engineering was investigated by fittingdark current and transient photovoltage (photocurrent) decay test. The results indicatedthat the mixed organic monolayer could passivate SiNWs surface completely andenhance the device performance efficiently.
引文
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