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Exciton Relaxation in Highly Rigid Conjugated Polymers: Correlating Radiative Dynamics with Structural Heterogeneity and Wavefunction Delocalization
ACS Energy Letters ( IF 19.3 ) Pub Date : 2017-08-23 00:00:00 , DOI: 10.1021/acsenergylett.7b00535 William R. Hollingsworth 1 , Jongbok Lee 2 , Lei Fang 2 , Alexander L. Ayzner 1
ACS Energy Letters ( IF 19.3 ) Pub Date : 2017-08-23 00:00:00 , DOI: 10.1021/acsenergylett.7b00535 William R. Hollingsworth 1 , Jongbok Lee 2 , Lei Fang 2 , Alexander L. Ayzner 1
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Conjugated polymers are promising materials for solar cells and other electronic applications due to facile charge and electronic energy migration along the conjugated backbone. Torsional defects due to rotation around single bonds on the backbone are known to decrease the effective conjugation length of these materials, limiting their ability to shuttle charge and electronic energy. We investigated the radiative emission dynamics of a recently synthesized rigid conjugated ladder polymer (LP1) and nonrigid control (CP1) with a similar carbazole backbone moiety. LP1 was prepared using a recently reported synthesis under thermodynamic control, leading to a low backbone defect density. We find that the singlet emission lifetime of LP1 is longer than that of any previously reported ladder conjugated polymer, which we attribute to its low defect density. Further, the emission contains a large-amplitude long component with a lifetime that lasts as long as 5 ns. Our results imply that careful control of defects at the synthesis level can lead to processable polymers with large electronic wavefunction delocalization and correspondingly long fluorescence lifetimes. This indicates an avenue to further tune the rapid solid-state energy transport rate along the polymer backbone.
中文翻译：
高刚性共轭聚合物中的激子弛豫：辐射动力学与结构异质性和波函数离域的相关性。
共轭聚合物由于沿共轭骨架的易带电电荷和电子迁移，是用于太阳能电池和其他电子应用的有前途的材料。已知由于围绕主链上单键旋转而引起的扭转缺陷会减小这些材料的有效共轭长度，从而限制其传递电荷和电子能量的能力。我们研究了具有相似咔唑骨架部分的最近合成的刚性共轭梯形聚合物（LP1）和非刚性对照（CP1）的辐射发射动力学。LP1是在热力学控制下使用最近报道的合成方法制备的，导致低的骨架缺陷密度。我们发现LP1的单重态发射寿命比任何先前报道的梯形共轭聚合物更长，我们将其归因于其低缺陷密度。此外，发射中包含一个大振幅的长分量，其使用寿命长达5 ns。我们的结果表明，在合成水平上仔细控制缺陷会导致可加工的聚合物具有较大的电子波函数离域和相应的长荧光寿命。这表明了进一步调节沿着聚合物主链的快速固态能量传输速率的途径。
更新日期：2017-08-23
中文翻译：
高刚性共轭聚合物中的激子弛豫：辐射动力学与结构异质性和波函数离域的相关性。
共轭聚合物由于沿共轭骨架的易带电电荷和电子迁移，是用于太阳能电池和其他电子应用的有前途的材料。已知由于围绕主链上单键旋转而引起的扭转缺陷会减小这些材料的有效共轭长度，从而限制其传递电荷和电子能量的能力。我们研究了具有相似咔唑骨架部分的最近合成的刚性共轭梯形聚合物（LP1）和非刚性对照（CP1）的辐射发射动力学。LP1是在热力学控制下使用最近报道的合成方法制备的，导致低的骨架缺陷密度。我们发现LP1的单重态发射寿命比任何先前报道的梯形共轭聚合物更长，我们将其归因于其低缺陷密度。此外，发射中包含一个大振幅的长分量，其使用寿命长达5 ns。我们的结果表明，在合成水平上仔细控制缺陷会导致可加工的聚合物具有较大的电子波函数离域和相应的长荧光寿命。这表明了进一步调节沿着聚合物主链的快速固态能量传输速率的途径。
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