聚合物P3HT和PFDTBT与富勒烯共混光伏体系的电荷产生动力学
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摘要
聚合物太阳能电池近年来取得了很大进展，最高能量转换效率已超过9%。但是，该效率距理论值仍有一定距离，并限制了该类太阳能电池的商业化应用。为了进一步提高光能转换效率，深入认识光电转换过程、找出其关键限制因素非常重要。本论文采用可见-近红外瞬态吸收光谱技术，研究了聚合物P3HT和PFDTBT与富勒烯共混光伏体系的原初电荷产生过程，考察了溶剂蒸汽退火处理、给受体最低未占分子轨道（LUMO）能级差和电场强度对光电转换过程的影响，为聚合物光伏材料设计和器件结构优化提供了实验和理论依据。
首先研究了P3HT纯膜和P3HT/PC_(61)BM共混膜中激子和极化子的原初动力学过程，着重考察了激发光波长、激发光通量以及溶剂蒸汽退火处理对极化子产生机制的影响规律。结合光谱电化学结果和不同波长光激发下的瞬态吸收光谱，指认了P3HT结晶相中的离域极化子（DP2）和无序相中的局域极化子（P2），并首次指认了P3HT阴离子和电荷转移激子的特征谱。通过研究P3HT/PC_(61)BM薄膜中激子和极化子的超快过程，确认了极化子产生的“瞬时”和“延迟”两种方式；发现P3HT/PC_(61)BM共混薄膜中P3HT结晶相波长依存的极化子产生机制；发现相对于热退火，溶剂蒸汽退火处理可减小P3HT结晶相与PC_(61)BM结晶相之间的无序相厚度，从而减少极化子俘获态。
随后研究了P3HT/PC_(61)BM共混膜中超快电荷复合动力学过程，定量分析了溶剂蒸汽退火处理对电荷俘获态，以及对超快时间尺度上载流子迁移率的影响。结合空穴限制的Langevin双分子复合模型分析了极化子复合过程，发现与CS2旋涂的P3HT/PC_(61)BM薄膜相比，溶剂蒸汽退火处理的P3HT/PC_(61)BM薄膜的空穴迁移率提高了2～3倍、局域俘获态密度减少了5倍，结果与真实器件的光电流、填充因子、外量子产率和能量转换效率等性能相符，表明优化活性层形貌对提高能量转换效率具有重要意义。
针对窄带聚合物光伏材料，我们以D-A型共聚物PFDTBT为给体、以四种LUMO能级不同的富勒烯衍生物为受体（给受体LUMO能级差调节范围为110～320meV），系统研究了给受体LUMO能级差对电荷产生过程的影响。通过拆分时间分辨光谱数据矩阵，获得了激子和带电物种的特征动力学演化曲线。发现纯PFDTBT薄膜中光激发可直接产生链间电荷转移态和电荷分离态，但最主要的原初激发仍是S1激子（>50%）。对于PFDTBT/PC_(61)BM共混膜，发现界面电荷转移态和电荷分离态并行产生，且界面电荷转移态对形成电荷分离态有重要贡献，从而纠正了以往关于电荷载流子产生的串行机制；发现由激子解离成电荷分离态的过程符合Marcus电荷转移机制，电子耦合强度为55±7cm1，重组能为0.33±0.02eV；发现由界面电荷转移态解离成电荷分离态遵从Braun-Onsager机制；得出最佳给-受体LUMO能级差为～0.33eV。本工作揭示了给受体LUMO能级差与电荷分离的关联规律，结果有助于新型窄带共聚物给体材料的设计。
最后研究了宏观电场对PFDTBT/PC_(61)BM太阳能电池器件超快电荷产生过程的影响，发现在器件工作条件下，电场对超快电荷产生和复合过程无显著影响；但若外加负偏压超过2V，电场可显著抑制界面电荷转移态复合，促进其解离成电荷分离态。
The recent development of polymer solar cell (PSC) has achieved a powerconversion efficiency (PCE) exceeding9%, yet PSCs still have significantmargins for further improvement, which is needed for practical applications.Accordingly, it is important to deepen the understandings in the light conversionmechanisms, which may be helpful for revealing the critical PCE-limitingfactors. This thesis has investigated, by the use of visible-to-near infraredtransient absorption (TA) spectroscopy, the influence of the solvent vaporannealing (SVA) treatment, the LUMO level offset and the macroscopicelectrical field strength on the processes of primary charge photogeneration inthe photovoltaic blends of P3HT and PFDTBT with fullerenes. The results mayshed light on the design of new polymeric photovoltaic materials, and on theoptimization of device configurations.
First, we investigated the primary dynamics of exciton and chargephotogeneration in the neat P3HT and the blend P3HT/PC_(61)BM films, andexamined the effects of solvent vapor annealing treatment, excitationwavelength and photon fluence on the ultrafast charge photogenerationprocesses. Spectroelectrochemistry and time-resolved spectroscopy revealedtwo different types of polarons, the delocalized and the localized ones,inhabiting the crystalline and the disordered P3HT phases, respectively. Thefingerprint absorption spectrum of anionic P3HT polaron was revealed for thefirst time to the best of our knowledge. By studying the dynamics of exciton andpolarons in P3HT/PC_(61)BM films, we found that polaron photogenerationprocesses can be categorized into the prompt and the delayed ones, andproposed the detailed mechanisms of polaron photogeneration from the P3HTcrystallites in the P3HT/PC_(61)BM blend films. Moreover, we found that thedimension of disordered intermediate between the P3HT crystallite and thePC_(61)BM aggregate of the SVA films was less than that for thermally annealedfilms, and thereby to be advantageous in minimizing the traps and/or blocks ofcharge carriers.
Second, we investigated the charge recombination (CR) dynamics ofP3HT/PC_(61)BM blend films in the initial ultrafast timescale. Quantitativeanalyses of the influence of film morphology on the trap density and hole mobility in ultrafast timescale were achieved. The CR dynamics were analyzedby the use of trap filling and Langevin’s hole-limited models. We demonstratedthat, with reference to the CS2-cast, the SVA treatment improved the holemobility2～3folds and reduced the density of polymer-localized traps5foldsfor the P3HT/PC_(61)BM blend. The results are consistent with the deviceperformance including the photocurrent, the filling factor, the external quantumefficiency and the PCE, implying that the optimization of film morphology canimprove the device performance.
For the narrow bandgap polymers, we examined the influence of Lowestunoccupied molecular orbital (LUMO) level offset on the chargephotogeneration processes by using PFDTBT blended with four different kindsof fullerene derivatives, tuning systematically the LUMO level offset over110～320meV. The species-associated kinetics were derived via decomposingthe time-resolved data matrices. For neat PFDTBT films, the photoexcitaitoncan generate the interchain charge transfer state and charge seperated state.However, the neutral excitons rather than the charge states dominated theprimary photoexcitation (>50%). For PFDTBT/PC_(61)BM blend film, weestablished the mechanisms of paralleling interfacial charge transfer state (ICT)and the charge separated (CS) state formation, and found the critical role of ICT inyielding CS, redressing the sequential mechanism for this specificpolymer/fullerene. It is found that the exciton-to-CS and the ICT-to-CSconversion, respectively, obey Marcus’ nonadiabetic electron transfermechanism and Braun-Onsager’s escape probability for a coupled e-h+pair, andthat the optimized LUMO level offset for polymer/fullerene solar cells is0.33eV. The role of LUMO level offset in yielding charge species may shed light onthe development of new photovoltaic materials.
Finally, we examined the influence of macroscopic electric field on thesubnanosecond charge photogeneration dynamics in PFDTBT/PC_(61)BM solar cell.The results suggested that the macroscopic electric field of thePFDTBT/PC_(61)BM solar cell was ineffective in the subnanosecond chargephotogeneration/recombination dynamics under working condition. However,under the reverse biases of2V, significant enhancement of chargephotogeneration and apparent suppression of ICT recombination were observed.
首先研究了P3HT纯膜和P3HT/PC_(61)BM共混膜中激子和极化子的原初动力学过程，着重考察了激发光波长、激发光通量以及溶剂蒸汽退火处理对极化子产生机制的影响规律。结合光谱电化学结果和不同波长光激发下的瞬态吸收光谱，指认了P3HT结晶相中的离域极化子（DP2）和无序相中的局域极化子（P2），并首次指认了P3HT阴离子和电荷转移激子的特征谱。通过研究P3HT/PC_(61)BM薄膜中激子和极化子的超快过程，确认了极化子产生的“瞬时”和“延迟”两种方式；发现P3HT/PC_(61)BM共混薄膜中P3HT结晶相波长依存的极化子产生机制；发现相对于热退火，溶剂蒸汽退火处理可减小P3HT结晶相与PC_(61)BM结晶相之间的无序相厚度，从而减少极化子俘获态。
随后研究了P3HT/PC_(61)BM共混膜中超快电荷复合动力学过程，定量分析了溶剂蒸汽退火处理对电荷俘获态，以及对超快时间尺度上载流子迁移率的影响。结合空穴限制的Langevin双分子复合模型分析了极化子复合过程，发现与CS2旋涂的P3HT/PC_(61)BM薄膜相比，溶剂蒸汽退火处理的P3HT/PC_(61)BM薄膜的空穴迁移率提高了2～3倍、局域俘获态密度减少了5倍，结果与真实器件的光电流、填充因子、外量子产率和能量转换效率等性能相符，表明优化活性层形貌对提高能量转换效率具有重要意义。
针对窄带聚合物光伏材料，我们以D-A型共聚物PFDTBT为给体、以四种LUMO能级不同的富勒烯衍生物为受体（给受体LUMO能级差调节范围为110～320meV），系统研究了给受体LUMO能级差对电荷产生过程的影响。通过拆分时间分辨光谱数据矩阵，获得了激子和带电物种的特征动力学演化曲线。发现纯PFDTBT薄膜中光激发可直接产生链间电荷转移态和电荷分离态，但最主要的原初激发仍是S1激子（>50%）。对于PFDTBT/PC_(61)BM共混膜，发现界面电荷转移态和电荷分离态并行产生，且界面电荷转移态对形成电荷分离态有重要贡献，从而纠正了以往关于电荷载流子产生的串行机制；发现由激子解离成电荷分离态的过程符合Marcus电荷转移机制，电子耦合强度为55±7cm1，重组能为0.33±0.02eV；发现由界面电荷转移态解离成电荷分离态遵从Braun-Onsager机制；得出最佳给-受体LUMO能级差为～0.33eV。本工作揭示了给受体LUMO能级差与电荷分离的关联规律，结果有助于新型窄带共聚物给体材料的设计。
最后研究了宏观电场对PFDTBT/PC_(61)BM太阳能电池器件超快电荷产生过程的影响，发现在器件工作条件下，电场对超快电荷产生和复合过程无显著影响；但若外加负偏压超过2V，电场可显著抑制界面电荷转移态复合，促进其解离成电荷分离态。
The recent development of polymer solar cell (PSC) has achieved a powerconversion efficiency (PCE) exceeding9%, yet PSCs still have significantmargins for further improvement, which is needed for practical applications.Accordingly, it is important to deepen the understandings in the light conversionmechanisms, which may be helpful for revealing the critical PCE-limitingfactors. This thesis has investigated, by the use of visible-to-near infraredtransient absorption (TA) spectroscopy, the influence of the solvent vaporannealing (SVA) treatment, the LUMO level offset and the macroscopicelectrical field strength on the processes of primary charge photogeneration inthe photovoltaic blends of P3HT and PFDTBT with fullerenes. The results mayshed light on the design of new polymeric photovoltaic materials, and on theoptimization of device configurations.
First, we investigated the primary dynamics of exciton and chargephotogeneration in the neat P3HT and the blend P3HT/PC_(61)BM films, andexamined the effects of solvent vapor annealing treatment, excitationwavelength and photon fluence on the ultrafast charge photogenerationprocesses. Spectroelectrochemistry and time-resolved spectroscopy revealedtwo different types of polarons, the delocalized and the localized ones,inhabiting the crystalline and the disordered P3HT phases, respectively. Thefingerprint absorption spectrum of anionic P3HT polaron was revealed for thefirst time to the best of our knowledge. By studying the dynamics of exciton andpolarons in P3HT/PC_(61)BM films, we found that polaron photogenerationprocesses can be categorized into the prompt and the delayed ones, andproposed the detailed mechanisms of polaron photogeneration from the P3HTcrystallites in the P3HT/PC_(61)BM blend films. Moreover, we found that thedimension of disordered intermediate between the P3HT crystallite and thePC_(61)BM aggregate of the SVA films was less than that for thermally annealedfilms, and thereby to be advantageous in minimizing the traps and/or blocks ofcharge carriers.
Second, we investigated the charge recombination (CR) dynamics ofP3HT/PC_(61)BM blend films in the initial ultrafast timescale. Quantitativeanalyses of the influence of film morphology on the trap density and hole mobility in ultrafast timescale were achieved. The CR dynamics were analyzedby the use of trap filling and Langevin’s hole-limited models. We demonstratedthat, with reference to the CS2-cast, the SVA treatment improved the holemobility2～3folds and reduced the density of polymer-localized traps5foldsfor the P3HT/PC_(61)BM blend. The results are consistent with the deviceperformance including the photocurrent, the filling factor, the external quantumefficiency and the PCE, implying that the optimization of film morphology canimprove the device performance.
For the narrow bandgap polymers, we examined the influence of Lowestunoccupied molecular orbital (LUMO) level offset on the chargephotogeneration processes by using PFDTBT blended with four different kindsof fullerene derivatives, tuning systematically the LUMO level offset over110～320meV. The species-associated kinetics were derived via decomposingthe time-resolved data matrices. For neat PFDTBT films, the photoexcitaitoncan generate the interchain charge transfer state and charge seperated state.However, the neutral excitons rather than the charge states dominated theprimary photoexcitation (>50%). For PFDTBT/PC_(61)BM blend film, weestablished the mechanisms of paralleling interfacial charge transfer state (ICT)and the charge separated (CS) state formation, and found the critical role of ICT inyielding CS, redressing the sequential mechanism for this specificpolymer/fullerene. It is found that the exciton-to-CS and the ICT-to-CSconversion, respectively, obey Marcus’ nonadiabetic electron transfermechanism and Braun-Onsager’s escape probability for a coupled e-h+pair, andthat the optimized LUMO level offset for polymer/fullerene solar cells is0.33eV. The role of LUMO level offset in yielding charge species may shed light onthe development of new photovoltaic materials.
Finally, we examined the influence of macroscopic electric field on thesubnanosecond charge photogeneration dynamics in PFDTBT/PC_(61)BM solar cell.The results suggested that the macroscopic electric field of thePFDTBT/PC_(61)BM solar cell was ineffective in the subnanosecond chargephotogeneration/recombination dynamics under working condition. However,under the reverse biases of2V, significant enhancement of chargephotogeneration and apparent suppression of ICT recombination were observed.
引文
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