Unraveling the differences in disorder between flexible-chain and hairy-rod conjugated polymers

Henry Kantrow; Spencer Yeager; Hongmo Li; Sergei Tretiak; Carlos Silva; Erin Ratcliff; Natalie Stingelin

doi:10.1117/12.3028603

30 September 2024 Unraveling the differences in disorder between flexible-chain and hairy-rod conjugated polymers

Henry Kantrow, Spencer Yeager, Hongmo Li, Sergei Tretiak, Carlos Silva, Erin Ratcliff, Natalie Stingelin

Proceedings Volume 13123, Organic, Hybrid, and Perovskite Photovoltaics XXV; 131230W (2024) https://doi.org/10.1117/12.3028603
Event: Organic Photonics + Electronics, 2024, San Diego, California, United States

Abstract

Conjugated hairy-rod polymers, which have emerged as promising photocathode materials for solar-fuel production, are comprised of stiff, low-entropy backbones and complex side-chain substitutions, which collectively affect assembly compared to flexible-chain materials. Here, we unravel the relationship between structural and electronic disorder in a model hairy-rod polymer, PBTTT. We identify a narrow electronic density-of-states (DOS) distribution with weak spatial variations in PBTTT, while the prototypical flexible-chain polymer, P3HT, features an energetically broad, spatially variable DOS. We assign this observation to the fact that PBTTT is structurally homogeneous due to its liquid-crystalline-like behavior, contrary to the structurally heterogeneous, semi-crystalline P3HT. This view is further supported by 2D electronic spectroscopy, which reveals that PBTTT features dynamic electronic disorder, vs. P3HT, which exhibits primarily static electronic disorder. Collectively, our work provides understanding into the disordered energy landscape in conjugated hairy-rod polymers, towards accelerated materials discovery for renewable energy technologies.

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Henry Kantrow, Spencer Yeager, Hongmo Li, Sergei Tretiak, Carlos Silva, Erin Ratcliff, and Natalie Stingelin "Unraveling the differences in disorder between flexible-chain and hairy-rod conjugated polymers", Proc. SPIE 13123, Organic, Hybrid, and Perovskite Photovoltaics XXV, 131230W (30 September 2024); https://doi.org/10.1117/12.3028603

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KEYWORDS

Diseases and disorders

Polymers

Optoelectronics

Raman spectroscopy

Renewable energy

Spectral density

Spectroscopy

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