KEYWORDS: Crystals, Ultrafast phenomena, System on a chip, Picosecond phenomena, Photovoltaics, Organic materials, Organic electronics, Near infrared, Crystallography, Americium
Singlet fission (SF), which allows one singlet state to be converted to 2 triplets, is one of the most perspective phenomena that may facilitate overcoming of the Shockley-Quiser limit in organic and hybrid photovoltaics.
Rubrene, mobility champion of organic electronics, is one of the most popular SF materials. Yet, despite its popularity, SF fundamentals in Rubrene remain strongly debated in the literature due to both experimental and computational limitations.
In this work we applied sub-10 fs transient absorption spectroscopy (TAS) to fully disentangle SF mechanism in low-defects high-quality Rubrene single crystals. We found that on 0.2 ps – 6 ns timescale, SF may be treated as 2 components process with half of the singlets to be converted into triplets at 10ps. Fascinatingly, at early times (<0.2 ps) we found additional component to be involved, which may be associated with hybrid state facilitating coherent SF. Based on our experimental findings, we have built a complete model of singlet fission in crystalline rubrene, which may help to resolve current debates on SF in the literature.
Recently, interactions between electronic and vibrational processes have been proposed to control various phenomena in a wide range of optoelectronic materials. Supposedly, these vibronic interactions may play the key role in physics of semiconducting materials for flexible soft photovoltaics by influencing optical, electrical, and other photovoltaic properties. Yet, their exact role in performance of real functional photovoltaic devices remains unclear, because of the current limitations of experimental and computational techniques. Here we develop a new method for studying vibronic interactions in functional optoelectronic materials based on the state-of-art combination of ultrafast spectroscopies and photocurrent detection techniques — photocurrent vibrationally promoted electronic resonance (photocurrent VIPER). The applicability of this technique is demonstrated by revealing the coupling of certain organic cation modes and inorganic lattice distortion in FaPbBr3 perovskite.
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