Fluorination-Induced Conversion of the Quasi- to the Normal Interchain Packing in Push–Pull Conjugated Polymer Aggregates

Yun, Hyuk Gu; Nho, Hak-Won; Han, Se Gyo; Cho, Jun Sang; Bang, Jieun; Yoon, Tae Woong; Mun, Jungho; Noh, Jaebum; Jeong, Minyoung; Kim, Dong Hyeon; Kim, Bora; Hwang, Hyeongjin; Jeong, Mun Seok; Lee, Hansol; Rho, Junsuk; Kang, Boseok; Park, JaeHong; Jang, Joon I.; Cho, Kilwon; Kwon, Oh-Hoon; Lee, Dongki

doi:10.1021/acs.macromol.3c00995

Macromolecules

2023

DOI: 10.1021/acs.macromol.3c00995

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Fluorination-Induced Conversion of the Quasi- to the Normal Interchain Packing in Push–Pull Conjugated Polymer Aggregates

Hyuk Gu Yun,

Hak-Won Nho,

Se Gyo Han

et al.

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2024

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Cited by 3 publications

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High Thickness Tolerance in All‐Polymer‐Based Organic Photovoltaics Enables Efficient and Stable In‐Door Operation

Zhang,

Lee,

Park

et al. 2024

Advanced Science

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Organic photovoltaics (OPVs) have great potential to drive low‐power consumption electronic devices under indoor light due to their highly tunable optoelectronic properties. Thick devices (>300 nm photo‐active junctions) are desirable to maximize photocurrent and to manufacture large‐scale modules via solution‐processing. However, thick devices usually suffer from severe charge recombination, deteriorating device performances. Herein, the study demonstrates excellent thickness tolerance of all‐polymer‐based PVs for efficient and stable indoor applications. Under indoor light, device performance is less dependent on photoactive layer thickness, exhibiting the best maximum power output in thick devices (34.7 µW cm−2 in 320–475 nm devices). Thick devices also exhibit much better photostability compared with thin devices. Such high thickness tolerance of all‐polymer‐based PV devices under indoor operation is attributed to strongly suppressed space‐charge effects, leading to reduced bimolecular recombination losses in thick devices. The unbalanced charge carrier mobilities are identified as the main cause for significant space‐charge effects, which is confirmed by drift‐diffusion simulations. This work suggests that all‐polymer‐based PVs, even with unbalanced mobilities, are highly desirable for thick, efficient, and stable devices for indoor applications.

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High Thickness Tolerance in All‐Polymer‐Based Organic Photovoltaics Enables Efficient and Stable In‐Door Operation

Zhang,

Lee,

Park

et al. 2024

Advanced Science

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Two‐Step Design Rule for Simultaneously High Conductivity and Seebeck Coefficient in Conjugated Polymer‐Based Thermoelectrics

Li,

Fu,

Scheunemann

et al. 2024

Advanced Science

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The trade‐off between enhancing conductivity (σ) through doping while concurrently observing a reduction in the Seebeck coefficient (S) presents a key challenge in organic thermoelectrics. Here, a two‐step structural design strategy is developed, where the first step enhances the backbone planarity which enhances the conductivity by an improved ordering of conjugated polymers (CPs). The second step, which is fluorination of the backbone, improves the Seebeck coefficient by the controlled induction of energetic disorder, stemming from the fluorine's disruption of the homogeneous electrostatic potential across the CP backbone. This strategy is applied to two series of donor‐acceptor (D‐A) types of CPs based on the BDT donor unit and BDD and TT as acceptor units, respectively. A maximum power factor (PF) over 155 (142.7 ± 12.7) µW m−1 K−2, coupled with S ≈202 (194.6 ± 7.6) µV K−1 is achieved, leading to up to 32‐fold enhancement of the PF compared to the initial non‐planar and non‐fluorinated polymer. This study provides valuable conceptual insights for designing CPs with high conductivity and Seebeck coefficient.

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Polaron Pair-Mediated Radiative Recombination of Singlet Excitons in a Conjugated Polymer Aggregate by Plasmonic and Semiconductor Nanocrystals

Kim,

Han,

Shao

et al. 2024

J. Phys. Chem. Lett.

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We investigated the excited-state dynamics of a conjugated polymer (CP:P3HT)-based ternary hybrid system containing P3HTcoated gold nanoparticles and quantum dots. Transient absorption spectroscopy results revealed that polaron pairs (PPs) originating from nonrelaxed singlet (S 1 ) excitons of the CP aggregate in the ternary system have shorter electron−hole separation distances than those of PPs in the neat CP aggregate because of the photophysical effects of plasmonic and semiconductor nanocrystals. In particular, the shorter electron−hole distances of PPs led to more back-recombination to S 1 excitons than dissociation into positive polarons in the ternary system, resulting in increased S 1 radiative recombination compared with that in the neat CP system. Thus, the photoluminescence intensity of the CP aggregate in the ternary system increased. Our findings provide new insights into the excited-state dynamics of CPs and pave the way for the development of next-generation high-efficiency optoelectronic devices.

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Fluorination-Induced Conversion of the Quasi- to the Normal Interchain Packing in Push–Pull Conjugated Polymer Aggregates

Cited by 3 publications

References 51 publications

High Thickness Tolerance in All‐Polymer‐Based Organic Photovoltaics Enables Efficient and Stable In‐Door Operation

High Thickness Tolerance in All‐Polymer‐Based Organic Photovoltaics Enables Efficient and Stable In‐Door Operation

Two‐Step Design Rule for Simultaneously High Conductivity and Seebeck Coefficient in Conjugated Polymer‐Based Thermoelectrics

Polaron Pair-Mediated Radiative Recombination of Singlet Excitons in a Conjugated Polymer Aggregate by Plasmonic and Semiconductor Nanocrystals

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