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Modified Prompt and Delayed Kinetics in a Strongly Coupled Organic Microcavity Containing a Multiresonance TADF Emitter
ACS Photonics ( IF 6.5 ) Pub Date : 2024-09-10 , DOI: 10.1021/acsphotonics.4c00488 Tomohiro Ishii 1 , Juan B. Pérez-Sánchez 2 , Joel Yuen-Zhou 2 , Chihaya Adachi 3, 4 , Takuji Hatakeyama 5 , Stéphane Kéna-Cohen 1
ACS Photonics ( IF 6.5 ) Pub Date : 2024-09-10 , DOI: 10.1021/acsphotonics.4c00488 Tomohiro Ishii 1 , Juan B. Pérez-Sánchez 2 , Joel Yuen-Zhou 2 , Chihaya Adachi 3, 4 , Takuji Hatakeyama 5 , Stéphane Kéna-Cohen 1
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Exciton polaritons are collective matter–light excitations that can be spaced up to 1 eV away from the bare molecular excited states. This hints at their potential to modify molecular emission processes. In the vast majority of cases, however, the observed emission rates from exciton polaritons remain nearly unchanged from those of the bare molecule and can be explained through radiative pumping of polaritons by dark molecular excited states. In this study, we observe a reduction in the prompt and delayed emission rates from exciton polaritons in a microcavity containing molecules that show multiresonance thermally activated delayed fluorescence. We find that most of our experimental observations are due to the existence of molecular configurations supporting excimers in the film. In the presence of strong coupling, polariton emission at the excimer energy shows the same kinetics observed at the monomer energy. Using a semiclassical model to describe the polariton kinetics, we find that this can be explained by the transfer of polaritons initially populated by the monomers to the dark states, followed by re-emission at lower energies. At the lowest temperatures, the longest-lived component of the delayed emission lifetime still cannot be understood via this mechanism.
中文翻译：
包含多谐振 TADF 发射器的强耦合有机微腔中的修饰瞬时和延迟动力学
激子极化激元是集体物质-光激发，与裸分子激发态的间隔可达 1 eV。这暗示了它们改变分子发射过程的潜力。然而，在绝大多数情况下，观察到的激子极化激元的发射速率与裸分子的发射速率几乎没有变化，并且可以通过暗分子激发态对极化激元的辐射泵浦来解释。在这项研究中，我们观察到在包含显示多共振热激活延迟荧光的分子的微腔中激子极化激元的瞬时和延迟发射速率降低。我们发现，我们的大部分实验观察是由于存在支持薄膜中准分子的分子构型。在强耦合存在的情况下，准分子能量的极化激元发射显示出在单体能量下观察到的相同动力学。使用半经典模型来描述极化激元动力学，我们发现这可以通过最初由单体填充的极化激元转移到暗态，然后以较低能量重新发射来解释。在最低温度下，延迟发射寿命中寿命最长的分量仍然无法通过这种机制来理解。
更新日期：2024-09-10
中文翻译：
包含多谐振 TADF 发射器的强耦合有机微腔中的修饰瞬时和延迟动力学
激子极化激元是集体物质-光激发，与裸分子激发态的间隔可达 1 eV。这暗示了它们改变分子发射过程的潜力。然而，在绝大多数情况下，观察到的激子极化激元的发射速率与裸分子的发射速率几乎没有变化，并且可以通过暗分子激发态对极化激元的辐射泵浦来解释。在这项研究中，我们观察到在包含显示多共振热激活延迟荧光的分子的微腔中激子极化激元的瞬时和延迟发射速率降低。我们发现，我们的大部分实验观察是由于存在支持薄膜中准分子的分子构型。在强耦合存在的情况下，准分子能量的极化激元发射显示出在单体能量下观察到的相同动力学。使用半经典模型来描述极化激元动力学，我们发现这可以通过最初由单体填充的极化激元转移到暗态，然后以较低能量重新发射来解释。在最低温度下，延迟发射寿命中寿命最长的分量仍然无法通过这种机制来理解。
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