Exciton Polaritons Reveal “Hidden” Populations in Functionalized Pentacene Films
Exciton Polaritons Reveal “Hidden” Populations in Functionalized Pentacene Films
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激子极化子揭示功能化并五苯薄膜中的“隐藏”族群
DOI：
10.1021/acs.jpcc.1c08257
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发表时间：
2021
期刊：
影响因子：
--
通讯作者：
Ostroverkhova, Oksana
中科院分区：
文献类型：
--
作者：
Van Schenck, Jonathan D.;Goldthwaite, Winston T.;Puro, Richard;Anthony, John E.;Ostroverkhova, Oksana
我们提出了一个系统的调查强激子光子耦合功能化并五苯（TIPS-Pn）为基础的薄膜在全金属腔，取决于分子浓度和薄膜形态。拉比分裂高达270毫电子伏的观察，在原始的非晶TIPS-Pn膜中实现的最高值。最低能量（0-0）激发态的激子-光子相互作用强度与分子密度的平方根成比例，这与薄膜中是否存在长程分子有序无关。在所有的膜，包括原始的结晶膜的无序区域中的分子群体耦合到腔最强烈。这种具有有利于与腔电磁场相互作用的分子构型的群体在裸（即，不耦合到腔）膜，这突出了极化激元光谱学揭示这些分子系综的能力，这些分子系综“隐藏”在多晶膜中。线性缩放的激子-光子相互作用强度与振子强度的平方根观察到在稀释的TIPS-Pn：PMMA膜，但不是在原始的TIPS-Pn膜，无论是非晶或结晶。特别地，在原始膜中，基于从裸膜的光学光谱提取的振子强度，振动电子（0-m，m> 0）激子的激子-光子相互作用强度高于预期，这归因于由TIPS-Pn的2D砌砖图案促进的增强的激子离域。在官能化的蒽并噻吩（diF TES-ADT）膜（也表现出2D砌砖包装基序），但不是在官能化的并四苯（TIPS-Tc）膜，这表明，潜在的机制依赖于短程分子间相互作用的分子包装基序和所得的纳米形态。
We present a systematic investigation of strong exciton–photon coupling in functionalized pentacene (TIPS-Pn)-based films in all-metal cavities, depending on molecular concentration and film morphology. Rabi splittings of up to 270 meV are observed, with the highest values achieved in pristine amorphous TIPS-Pn films. The exciton–photon interaction strength for the lowest-energy (0–0) excited state scaled with the square root of the molecular density, which was independent of whether the long-range molecular order were present in films. The molecular populations in the disordered regions of the films coupled to the cavity most strongly in all films, including pristine crystalline films. Such populations, with molecular configurations favoring interaction with the cavity electromagnetic field, were not readily identifiable in optical absorption spectra of bare (i.e., not coupled to the cavity) films, which highlights the capability of polariton spectroscopy to reveal these molecular ensembles, which are “hidden” in polycrystalline films. The linear scaling of the exciton–photon interaction strength with the square root of the oscillator strengths was observed in dilute TIPS-Pn:PMMA films but not in pristine TIPS-Pn films, either amorphous or crystalline. In particular, in pristine films, the exciton–photon interaction strength for the vibronic (0–m,m> 0) excitons was higher than expected based on the oscillator strengths extracted from the optical spectra of bare films, which was attributed to enhanced exciton delocalization facilitated by the 2D brickwork motif of TIPS-Pn. Similar observations were made in functionalized anthradithiophene (diF TES-ADT) films (also exhibiting a 2D brickwork packing motif) but not in functionalized tetracene (TIPS-Tc) films, which suggests that the underlying mechanisms rely on short-range intermolecular interactions determined by the molecular packing motif and resulting nanomorphology.
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发表时间：
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影响因子：
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