Journal
PHYSICAL REVIEW B
Volume 102, Issue 8, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevB.102.081122
Keywords
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Funding
- Winton Programme for the Physics of Sustainability
- Engineering and Physical Sciences Research Council [EP/L015552/1]
- NWO Vidi Grant [016.Vidi.179.005]
- Simons Foundation [601946]
- Agence Nationale de la Recherche [ANR-19-CE24-0028]
- Gianna Angelopoulos Programme for Science, Technology, and Innovation
- EPSRC Tier-2 capital Grant [EP/P020259/1]
- EPSRC [EP/P020259/1] Funding Source: UKRI
- Agence Nationale de la Recherche (ANR) [ANR-19-CE24-0028] Funding Source: Agence Nationale de la Recherche (ANR)
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Organic semiconductors exhibit properties of individual molecules and extended crystals simultaneously. The strongly bound excitons they host are typically described in the molecular limit, but excitons can delocalize over many molecules, raising the question of how important the extended crystalline nature is. Using accurate Green's function based methods for the electronic structure and nonperturbative finite difference methods for exciton-vibration coupling, we describe exciton interactions with molecular and crystal degrees of freedom concurrently. We find that exciton delocalization controls these interactions, with thermally activated crystal phonons predominantly coupling to delocalized states, and molecular quantum fluctuations predominantly coupling to localized states. Based on this picture, we quantitatively predict and interpret the temperature and pressure dependence of excitonic peaks in the acene series of organic semiconductors, which we confirm experimentally, and we develop a simple experimental protocol for probing exciton delocalization. Overall, we provide a unified picture of exciton delocalization and vibrational effects in organic semiconductors, reconciling the complementary views of finite molecular clusters and periodic molecular solids.
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