Fine-tuning the Microstructure and Photophysical Characteristics of Fluorescent Conjugated Copolymers Using Photoalignment and Liquid-crystalline Ordering
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arXiv
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| Natura: | Preprint |
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2024
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| _version_ | 1866909185543766016 |
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| author | Shi, Yuping Landfester, Katharina Morris, Stephen M. |
| author_facet | Shi, Yuping Landfester, Katharina Morris, Stephen M. |
| contents | Replicating the microstructure and near-unity excitation energy transfer efficiency in natural light-harvesting complexes (LHCs) remains a major challenge for synthetic energy-harvesting devices. Biological photosynthesis can spontaneously regulate the active ensembles of involved energy absorbing and funnelling chlorophyll-containing proteins in response to fluctuating sunlight. Here we utilize liquid crystalline (LC) ordering to fine-tune the polymer packing and photophysical properties in liquid crystalline conjugated polymer (LCCP) films for LHC biomimicry and optimizing photoluminescence quantum efficiency (PLQE). We show that the long-range orientational ordering present in a LC phase of poly(9,9-dioctylfluorene-co-benzothiadiazole) (F8BT) stabilizes a small fraction of randomly-oriented F8BT nanocrystals dispersed in an amorphous matrix of disordered F8BT chains, hence resembling a self-doped host-guest system whereby excitation energy funnelling and PLQE are reinforced significantly by three-dimensional donor-to-acceptor Forster resonance energy transfer (FRET) and dominant intrachain emission in the nano-crystalline acceptor. Furthermore, the photoalignment of nematic F8BT layers is combined to fabricate long-sought large-area-extended monodomains which exhibit >60% crystallinity and ~20 nm-long interchain packing order, whilst also promoting linearly polarized emission, a new band-edge absorption species, and an extra emissive interchain excited state. Our micro-PL spectral results support the feasibility of making use of self-doped F8BT nematic films for bio-mimicry of certain structural basis and light-harvesting properties of naturally occurring LHCs. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2404_19435 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Fine-tuning the Microstructure and Photophysical Characteristics of Fluorescent Conjugated Copolymers Using Photoalignment and Liquid-crystalline Ordering Shi, Yuping Landfester, Katharina Morris, Stephen M. Soft Condensed Matter Replicating the microstructure and near-unity excitation energy transfer efficiency in natural light-harvesting complexes (LHCs) remains a major challenge for synthetic energy-harvesting devices. Biological photosynthesis can spontaneously regulate the active ensembles of involved energy absorbing and funnelling chlorophyll-containing proteins in response to fluctuating sunlight. Here we utilize liquid crystalline (LC) ordering to fine-tune the polymer packing and photophysical properties in liquid crystalline conjugated polymer (LCCP) films for LHC biomimicry and optimizing photoluminescence quantum efficiency (PLQE). We show that the long-range orientational ordering present in a LC phase of poly(9,9-dioctylfluorene-co-benzothiadiazole) (F8BT) stabilizes a small fraction of randomly-oriented F8BT nanocrystals dispersed in an amorphous matrix of disordered F8BT chains, hence resembling a self-doped host-guest system whereby excitation energy funnelling and PLQE are reinforced significantly by three-dimensional donor-to-acceptor Forster resonance energy transfer (FRET) and dominant intrachain emission in the nano-crystalline acceptor. Furthermore, the photoalignment of nematic F8BT layers is combined to fabricate long-sought large-area-extended monodomains which exhibit >60% crystallinity and ~20 nm-long interchain packing order, whilst also promoting linearly polarized emission, a new band-edge absorption species, and an extra emissive interchain excited state. Our micro-PL spectral results support the feasibility of making use of self-doped F8BT nematic films for bio-mimicry of certain structural basis and light-harvesting properties of naturally occurring LHCs. |
| title | Fine-tuning the Microstructure and Photophysical Characteristics of Fluorescent Conjugated Copolymers Using Photoalignment and Liquid-crystalline Ordering |
| topic | Soft Condensed Matter |
| url | https://arxiv.org/abs/2404.19435 |