O, S, and N Bridged Atoms Screening on 2D Conjugated Central Units of High‐Performance Acceptors DOI

Xiangjian Cao,

Zheng Xu, Ruohan Wang

et al.

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

Published: May 6, 2025

Abstract Almost all of central cores in high‐performance acceptors are limited to the electron‐withdrawing diimide structure currently, which constrains further acceptor structural innovation greatly. Herein, oxygen (O), sulfur (S), and nitrogen (N) atoms adopted bridge 2D conjugated cores, yielding three platforms CH─O, CH─S, CH─N that differ by only two atoms. Because characteristic atomic outer electron configuration hybrid orbital orientation, O‐, S‐, N‐bridged display quite different conformations electronic properties, namely, dibenzodioxin (planar, non‐aromatic), thianthrene (puckered, non‐aromatic) phenazine aromatic), respectively. A systematic investigation discloses how core, especially its p‐π overlap between lone pair on O/S/N coterminous benzene planes, affect intrinsic photoelectronic properties for first time. Finally, CH─N‐based binary device affords highest fill factor 83.13% organic photovoltaics along with a first‐class efficiency 20.23%. By evaluating strictly controlled molecular comprehensively, work reveals potential uniqueness determining excellent photovoltaic outcomes acceptors.

Language: Английский

Rebuilding Peripheral F, Cl, Br Footprints on Acceptors Enables Binary Organic Photovoltaic Efficiency Exceeding 19.7% DOI

Xiangjian Cao,

Peiran Wang,

Xinyuan Jia

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 8, 2024

Abstract Given homomorphic fluorine (F), chlorine (Cl) and bromine (Br) atoms are featured with gradually enlarged polarizability/atomic radius but decreased electronegativity, the rational screen of halogen species locations on small molecular acceptors (SMAs) is quite essential for acquiring desirable packing to boost efficiency organic solar cells (OSCs). Herein, three isomeric SMAs (CH−F, CH−C CH−B) constructed by delicately rebuilding peripheral F, Cl, Br footprints both central end units. Such a re‐permutation halogens could not only maintain structural symmetry maximum, also acquire extra asymmetric benefits enhanced dipole moment intramolecular charge transfer, etc. Moreover, brominating enhances crystallinity CH−B without introducing undesirable steric hindrance groups, thus rendering better balance between high crystallization domain size control in PM6:CH−B blend. Further benefitting from large dielectric constant, exciton binding energy, optimized great electron transfer integral, affords first class binary OSC 19.78 %, moreover, highest 18.35 % far when increasing active layer thickness ~300 nm. Our successful screening provides valuable insight into further design record‐breaking OSCs.

Language: Английский

Citations

6
Optimizing Exciton Diffusion and Carrier Transport for Enhanced Efficiency in Q‐PHJ and BHJ Organic Solar Cells DOI
Hanjian Lai, Yiwu Zhu,

Yanni Ouyang

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 5, 2024

Abstract Exciton diffusion and carrier transport are two critical factors that determine the efficiency of organic photovoltaics (OPVs). However, relationship between these has not been extensively studied. Designing non‐fullerene acceptors (NFAs) with efficient coefficients high electronic transmittance is a key area focus. In this study, materials for bulk‐heterojunction (BHJ) quasiplanar‐heterojunction (Q‐PHJ) devices synthesized to validate desired differences in crystallinity. The single crystal BOBO4Cl‐ βδ demonstrated most compact packing structure, an improved planar configuration closer π···π distances, resulting higher electron mobility superior exciton coefficient. Consequently, ‐based achieved power conversion (PCE) 17.38% Q‐PHJ, compared lower PCE 14.75% BHJ devices. Furthermore, incorporating into D18/L8‐BO Q‐PHJ system increased from 17.98% 18.81%, one highest values recorded This improvement attributed strong crystallinity , which enhances arrangement improves Our work highlights importance molecular design tunable OPV architectures reveals them, contributes achievement high‐performance NFAs.

Language: Английский

Citations

4
Two compatible M-series acceptors form a well-mixed phase with improved exciton diffusion for efficient polymer solar cells DOI
Yi Li,

Yanni Ouyang,

Huiting Fu

et al.

Science China Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 6, 2024

Language: Английский

Citations

4
Instantaneous Marcus theory for photoinduced charge transfer dynamics in multistate harmonic model systems DOI
Zengkui Liu, Xiang Sun

Journal of Physics Condensed Matter, Journal Year: 2024, Volume and Issue: 36(31), P. 315201 - 315201

Published: April 24, 2024

Abstract Modeling the dynamics of photoinduced charge transfer (CT) in condensed phases presents challenges due to complicated many-body interactions and quantum nature electronic transitions. While traditional Marcus theory is a robust method for calculating CT rate constants between states, it cannot account nonequilibrium effects arising from initial nuclear state preparation. In this study, we employ instantaneous (IMT) simulate dynamics. IMT incorporates structural relaxation following vertical photoexcitation equilibrated ground state, yielding time-dependent coefficient. The multistate harmonic (MSH) model Hamiltonian characterizes an organic photovoltaic carotenoid-porphyrin-fullerene triad dissolved explicit tetrahydrofuran solvent, constructed by mapping all-atom inputs molecular simulations. Our calculations reveal that population MSH models obtained with agree more accurate quantum-mechanical Fermi’s golden rule. This alignment suggests provides practical approach understanding nonadiabatic condensed-phase systems.

Language: Английский

Citations

3
C-shaped A-D-A non-fullerene acceptor achieves efficient organic solar cells DOI Creative Commons
Hanjian Lai,

Zihao Deng,

Feng He

et al.

Joule, Journal Year: 2024, Volume and Issue: 8(3), P. 572 - 575

Published: March 1, 2024

Language: Английский

Citations

3
Cyclization Engineering of Electron-Deficient Maleimide Unit for Nonfused Ring Electron Acceptors Enables Efficient Organic Solar Cells DOI

Shenbo Zhu,

Li Lyu, Yiyang Li

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(26), P. 33928 - 33934

Published: June 18, 2024

Nonfused ring electron acceptors (NFREAs) have emerged as promising materials for commercial applications in organic solar cells due to their straightforward synthesis process and cost-effectiveness. The rational design of structural frameworks is crucial enhancing device efficiency. In this study, we explore the use maleimide thiophene key building blocks, employing cyclization engineering techniques. Additionally, cyclopentanedithiophene was chosen bridging unit, coupled with fluorinated terminals, fabricate NFREAs, namely, PI-DTS DPI-DTS. DPI-DTS demonstrated superior molecular planarity an upshifted lowest unoccupied orbital energy level. Moreover, DPI-DTS-based blend films display enhanced π–π interactions crystallinity, alongside a predominantly face-on orientation. Consequently, devices displayed more balanced carrier mobility, reduced bimolecular recombination, trap-assisted leading improved charge transfer Ultimately, led excellent efficiency 10.48%, open-circuit voltage high 0.914 V. These findings highlight significant promise aromatic imides constructing established structure-performance relationship provides theoretical basis performance NFREAs.

Language: Английский

Citations

3
Highly Crystalline Selenium‐Substituted C‐Shaped Ortho‐Benzodipyrrole‐Based A‐D‐A‐Type Nonfullerene Acceptor Enabling Solution‐Processed Single‐Crystal‐Like Thin Films for Air‐Stable, High‐Mobility N‐Type Transistors DOI Creative Commons
Kuo‐Hsiu Huang,

Chi‐Chun Tseng,

Chia‐Lin Tsai

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 20, 2024

Abstract C‐shaped ortho ‐benzodipyrrole‐based A‐D N B D‐A non‐fullerene acceptors (NFAs), derived from the removal of A′ thiadiazole moiety in Y6, emerge as a new class structurally simplified A‐D‐A‐type NFAs. In this work, selenium‐substitution strategy is applied to central D ladder‐π‐core, yielding asymmetric CB‐Se and symmetric CB‐2Se. Asymmetric demonstrates less ordered 3D trapezoid‐like packing structure, which promotes more favorable intermixed donor‐acceptor morphology with PM6 polymer, achieving higher power conversion efficiency (PCE) 17.87% organic photovoltaics (OPVs). This value represents highest reported among selenium‐incorporated Symmetric CB‐2Se forms kaleidoscope‐like single‐crystal structure enhanced intermolecular interactions. enables development single‐crystal‐like solution‐processed thin film, transitions kinetically trapped face‐on π–π stacking orientation thermodynamically stable edge‐on configuration upon thermal annealing. The CB‐2Se‐based field‐effect transistor (OFET) achieved remarkable electron mobility 1.18 cm 2 V −1 s exceptional n‐type air stability, outperformed corresponding D‐A‐type Y6‐based materials by two orders magnitudes for OFETs utilizing small molecules.

Language: Английский

Citations

3
Electron‐Rich Heptacyclic S,N Heteroacene Enabling C‐Shaped A‐D‐A‐type Electron Acceptors With Photoelectric Response beyond 1000 Nm for Highly Sensitive Near‐Infrared Photodetectors DOI Creative Commons
Kuo‐Hsiu Huang, Bing‐Huang Jiang,

Hancheng Lu

et al.

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

Published: Jan. 14, 2025

Abstract A highly electron‐rich S,N heteroacene building block is developed and condensed with FIC Cl‐IC acceptors to furnish CT‐F CT‐Cl, which exhibit near‐infrared (NIR) absorption beyond 1000 nm. The C‐shaped CT‐Cl self‐assemble into a ordered 3D intermolecular packing network via multiple π−π interactions in the single crystal structures. CT‐F‐based organic photovoltaic (OPV) achieved an impressive efficiency of 14.30% broad external quantum response extending from UV‐vis NIR (300–1050 nm) regions, outperforming most binary OPVs employing A‐D‐A‐type acceptors. possesses higher surface energy than CT‐F, promoting vertical phase segregation resulting its preferential accumulation near bottom interface blend. This arrangement, combined lower HOMO level effectively reduces undesired hole electron injection under reverse voltage. PM6:CT‐Cl‐based photodetectors (OPDs) devices ultra‐high shot‐noise‐limited specific detectivity ( D sh *) values exceeding 10 14 Jones region 620 nm, reaching unprecedentedly high value 1.3 × at 950 When utilizing 780 nm light source, OPDs show record‐high rise/fall times 0.33/0.11 µs exceptional cut‐off frequency f ‐3dB ) 590 kHz −1 V.

Language: Английский

Citations

0
Perovskite‐Coupled NIR Organic Hybrid Solar Cells Achieving an 84.2% Fill Factor and a 25.2% Efficiency: A Comprehensive Mechanistic Exploration DOI Open Access

Chieh‐Ming Hung,

Chia‐Jen Chih,

Kuo‐Hsiu Huang

et al.

Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown

Published: March 12, 2025

Abstract The integration of organic dyes in perovskite solar cells (PSCs) to utilize near‐infrared (NIR) photons remains a challenge. In this study, selenium‐incorporated ortho‐benzodipyrrole‐based NIR dye CB‐2Se was developed. CB‐2Se, featuring lower bandgap 1.35 eV, blended with PCBM form bulk‐heterojunction layer PSCs for electron extraction and transport. Compared Y6‐16 acceptor, the removal Tz unit suppresses self‐aggregation, improving its compatibility PCBM. A CB‐2Se:PCBM‐incorporated PSC achieved remarkable power conversion efficiency (PCE) 25.18% V OC 1.164 V, J SC 25.71 mA/cm 2 , Fill Factor 84.15%, outperforming that PCBM‐only reference device (24.35%) PCBM:Y6‐16‐based (24.49%). PCBM:CB‐2Se enhanced long‐term stability PSCs, retaining 88% initial after 1000 h under ambient air thermal conditions. photophysical interactions between have been comprehensively investigated by using femtosecond transient absorption spectroscopy. Ultrafast exciton separation into free charges occurs within 200 femtoseconds at interfaces CB‐2Se. For first time, transfer holes from back detected, providing valuable insights charge dynamics utilizing dyes.

Language: Английский

Citations

0
Effects of non-fused and fused substituents in quinoxaline-based central units on conformation, aggregation, and photovoltaic properties of non-fused ring electron acceptors DOI
Kenta Yamada, Wataru Suzuki,

Motohisa Kubota

et al.

Journal of Materials Chemistry C, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Substituents of the quinoxaline core influence aggregation properties S-shaped acceptors.

Language: Английский

Citations

0