Low-Cost Nonfused-Ring Electron Acceptors Enabled by Noncovalent Conformational Locks

Accounts of Chemical Research, Journal Year: 2024, Volume and Issue: 57(6), P. 981 - 991

Published: March 3, 2024

ConspectusSince the first bilayer-structured organic solar cells (OSCs) in 1986, fullerenes and their derivatives have dominated landscape for two decades due to unique properties. In recent years, breakthrough nonfullerene acceptors (NFAs) was mainly attributed development of fused-ring electron (FREAs), whose photovoltaic performance surpassed that fullerene derivatives. Through unremitting efforts whole community, power conversion efficiencies (PCEs) 19% FREA-based OSCs. However, FREAs generally suffered from complex synthetic approaches high product costs, which hindered large-scale production. Therefore, many researchers are seeking a new type NFA achieve cost-effective, highly efficient OSCs.In collaboration with Marks Facchetti 2012, Huang et al. (Huang, H. J. Am. Chem. Soc. 134, 10966−10973, 10.1021/ja303401s) proposed concept "noncovalent conformational locks" (NoCLs). following our group has been focusing on theoretical experimental exploration NoCLs, revealing fundamental nature, formulating simple descriptor quantifying strength, employing this approach high-performance organic/polymeric semiconductors optoelectronics, such as OSCs, thin-film transistors, room-temperature phosphorescence, photodetectors. The NoCLs strategy proven be effective enhancing molecular rigidity planarity, thus improving charge transport mobilities semiconductors, reduced reorganization energy suppressed nonradiative decay.In 2018, Chen (Li, S. Adv. Mater. 30, 1705208, 10.1002/adma.201705208) reported example nonfused-ring (NFREAs) intramolecular noncovalent F···H interactions. is essential NFREAs, it simplifies conjugated structures while maintaining coplanarity comparable FREAs. Due concise synthesis routes, NFREAs show great potential achieving cost-effective Account, we provide an overview developing strategy. We begin discussion distinct features compared FREAs, structural simplification completely NFREAs. Next, examine several selected typical examples remarkable performance, aiming in-depth design principle structure–property–performance relationships. Then, discuss how balance among efficiency, stability, cost through two-in-one polymerized (PNFREAs). Finally, offer views current challenges future prospects hope Account will trigger intensive research interest field, propelling OSCs into stage.

Language: Английский

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Bis(benzoselenadiazol)ethane: A π‐Extended Acceptor‐Dimeric Unit for Ambipolar Polymer Transistors with Hole and Electron Mobilities Exceeding 10 cm² V⁻¹ s⁻¹

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(17)

Published: March 5, 2024

Abstract The lack of ambipolar polymers with balanced hole ( μ h ) and electron mobilities e >10 cm 2 V −1 s is the main bottleneck for developing organic integrated circuits. Herein, we show design synthesis a π‐extended selenium‐containing acceptor‐dimeric unit, namely benzo[ c ][1,2,5]selenadiazol‐4‐yl)ethane (BBSeE), to address this dilemma. In comparison its sulfur‐counterpart, BBSeE demonstrates enlarged co‐planarity, selective noncovalent interactions, polarized Se−N bond, higher affinity. successful stannylation offers great opportunity access acceptor‐acceptor copolymer pN‐BBSeE, which shows narrower band gap, lower‐lying lowest unoccupied molecular orbital level (−4.05 eV), degree backbone planarity. Consequently, pN‐BBSeE‐based transistors display an ideally transporting property 10.65 10.72 , respectively. To best our knowledge, simultaneous / values >10.0 are performances ever reported polymers. addition, pN‐BBSeE excellent shelf‐storage stability, retaining over 85 % initial mobility after two months storage. Our study promising acceptor building block constructing high‐performance applied in next‐generation circuit.

Language: Английский

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Recent developments in polymer semiconductors with excellent electron transport performances

Chemical Society Reviews, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This review describes the design considerations, bonding modes between monomers, structural modification strategies, and applications of polymer semiconductors with excellent electron transport performances.

Language: Английский

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Precise synthesis of advanced polyarylamines for efficient perovskite solar cells

Nature Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 3, 2025

Language: Английский

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The revival of 4H-cyclopenta[2,1-b:3,4-b′]dithiophene (CPDT) driven by low-cost and high-performance nonfused-ring electron acceptors

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(29), P. 17973 - 17991

Published: Jan. 1, 2024

This review comprehensively summarizes the development history of CPDT-based organic photovoltaic materials, which contributes to a deeper understanding revival CPDT driven by low-cost acceptors.

Language: Английский

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Quantifying unit ratios in semiconducting copolymers and effect of structural deviations on photovoltaic performance

Communications Materials, Journal Year: 2025, Volume and Issue: 6(1)

Published: Feb. 26, 2025

Language: Английский

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Quantum Batteries: A Materials Science Perspective

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 26, 2025

Abstract In the context of quantum thermodynamics, batteries have emerged as promising devices for energy storage and manipulation. Over past decade, substantial progress is made in understanding fundamental properties batteries, with several experimental implementations showing great promise. This perspective provides an overview solid‐state materials platforms that can lead to fully operational batteries. After briefly introducing basic features organic microcavities are discussed, where superextensive charging already demonstrated experimentally. Now, this explores other materials, including inorganic nanostructures (such wells dots), perovskite systems, (normal high‐temperature) superconductors. Key achievements these areas, relevant realization highlighted. The challenges future research directions also addressed. Despite their enormous potential devices, into advanced still its infancy. paper aims stimulate interdisciplinarity convergence among different science communities accelerate development new device architectures

Language: Английский

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Chlorinated Dithiazole‐Based Polymer Donor Enables Over 18% Efficiency for Organic Photovoltaics

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 3, 2025

Abstract Forming an optimal donor:acceptor blend morphology with a low trap state density is highly desired to reach perfect compromise between charge generation and recombination for organic photovoltaics (OPVs), wherein polymer donor plays key role. Here, two wide bandgap donors of PN‐HD PN‐BO are reported, featuring the same low‐cost chlorinated dithiazole as electron‐withdrawing unit but varied alkyl chains on π‐bridged thiophene ring. It found that shorter chain endows merits better miscibility acceptor longer crystallization time, leading more favorable phase separation lower states (tDOS) in resulting active layer. Notably, tDOS 3.51 × 10 15 cm −3 eV −1 PN‐BO:BTP‐eC9‐based device has enabled exceptionally high photocurrent 28.59 mA −2 , thereby efficiency 18.01%, far beyond those (24.64 15.51%) PN‐HD:BTP‐eC9‐based one higher value. The work reveals relationship flexible density, providing new route efficient OPVs.

Language: Английский

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Turning Lemons into Lemonade: One‐Step Synthesized Dual‐Acceptor Organic Photosensitizer to Boost the Photodynamic Therapy

Small, Journal Year: 2025, Volume and Issue: unknown

Published: March 23, 2025

Reactive oxygen species (ROS) are crucial in photodynamic therapy (PDT), but their generation is highly dependent on the S-T bandgap (ΔEST), spin-orbit coupling (SOC), intersystem crossing rate (kISC), and also excited triplet-states lifetime (τTriplet) organic photosensitizers (PSs). In contrast to widely reported donor-acceptor-donor (D-A-D) type PSs, D-A-A-D typed PSs seldomly developed for time-consuming complicated synthesis, show great potential enhancing ROS phototheranostics. This work here presents a one-step synthetic procedure of 2DMeTPA-2BT with high yield 47%, which significantly different from previously dual-acceptor cases. 2DMeTPA-BT, display much smaller ΔEST value large SOC constants. Also, (ISC) dynamics indicate that fast kISC, long τTriplet, triplet population observed 2DMeTPA-2BT-based nanoparticles (NPs), contributing superior ROS. NPs then finally utilized imaging-guided PDT vivo tumor inhibition 90%. method offers an efficient way produce via reaction, providing new avenues high-performance

Language: Английский

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High‐Performance n‐Type Semiconducting Polymers via Synergistic Heteroannulated Acceptor Dimerization and Direct Arylation Polymerization

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 25, 2025

Abstract Developing unipolar n‐type semiconducting polymers with electron mobility ( µ e ) exceeding 10 cm 2 V −1 s presents a significant challenge in organic electronics. In response to this challenge, novel molecular architecture‐tailoring approach known as the heteroannulated acceptor dimerization strategy is introduced. Through theoretical framework that integrates heteroatom substitution and based on parent hexylthiophene‐flanked benzothiadiazole, our establishes modulate frontier orbital (FMO) levels while enhancing planarity. The removal of alkyl side chains flanking thiophene units leads more planar polymer backbone, evidenced by dihedral angles 0°. prediction deeper FMO oxadiazole‐containing experimentally validated, demonstrating efficacy design principles. Using strategy, new copolymers are synthesized via modified palladium/copper co‐catalyzed direct arylation polymerization protocol 10‐gram scale. Compared its hexylthiophene‐counterpart pN‐BBOE‐C6, pN‐BBOE‐H exhibits exceptional structural electronic properties, including π–π stacking distance 3.5 Å 11.2 , among highest for polymers. This work not only advances understanding materials but also provides robust designing high‐performance

Language: Английский

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