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1.
Chem Soc Rev ; 53(9): 4674-4706, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38529583

RESUMO

High power conversion efficiency (PCE) and long-term stability are essential prerequisites for the commercialization of polymer solar cells (PSCs). Small-molecule acceptors (SMAs) are core materials that have led to recent, rapid increases in the PCEs of the PSCs. However, a critical limitation of the resulting PSCs is their poor long-term stability. Blend morphology degradation from rapid diffusion of SMAs with low glass transition temperatures (Tgs) is considered the main cause of the poor long-term stability of the PSCs. The recent emergence of oligomerized SMAs (OSMAs), composed of two or more repeating SMA units (i.e., dimerized and trimerized SMAs), has shown great promise in overcoming these challenges. This innovation in material design has enabled OSMA-based PSCs to reach impressive PCEs near 19% and exceptional long-term stability. In this review, we summarize the evolution of OSMAs, including their research background and recent progress in molecular design. In particular, we discuss the mechanisms for high PCE and stability of OSMA-based PSCs and suggest useful design guidelines for high-performance OSMAs. Furthermore, we reflect on the existing hurdles and future directions for OSMA materials towards achieving commercially viable PSCs with high PCEs and operational stabilities.

2.
Nano Lett ; 24(31): 9544-9552, 2024 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-38968419

RESUMO

This study introduces wavelength-dependent multistate programmable optoelectronic logic-in-memory (OLIM) operation using a broadband photoresponsive pNDI-SVS floating gate. The distinct optical absorption of the relatively large bandgap DNTT channel (2.6 eV) and the narrow bandgap pNDI-SVS floating gate (1.37 eV) lead to varying light-induced charge carrier accumulation across different wavelengths. In the proposed OLIM device comprising the p-type pNDI-SVS-based optoelectronic memory (POEM) transistor and an IGZO n-type transistor, we achieve controllable output voltage signals by modulating the pull-up performance through optical wavelength and applied bias manipulation. Real-time OLIM operation yields four discernible output values. The device's high mechanical flexibility and seamless surface integration among the paper substrate, pNDI-SVS, parylene gate dielectric, and DNTT region render it compatible for integration into paper-based optoelectronics. Our flexible POEM device on name card substrates demonstrates stable operational performance, with minimal variation (8%) after 100 cycles of repeated memory operation, remaining reliable across various angle measurements.

3.
Nat Commun ; 15(1): 2977, 2024 Apr 06.
Artigo em Inglês | MEDLINE | ID: mdl-38582788

RESUMO

In blue phosphorescent dopants, the tetradentate platinum(II) complex is a promising material showing high efficiency and stability in devices. However, metal-metal-to-ligand charge transfer (MMLCT) formation leads to low photo-luminescence quantum yields (PLQYs), wide spectra, and intermolecular interaction. To suppress MMLCT, PtON-tb-TTB and PtON-tb-DTB are designed using theoretical simulation by modifying t-butyl in PtON-TBBI. Both materials effectively suppress MMLCT and exhibit high PLQYs of 99% and 78% in 5 wt% doped film, respectively. The PtON-tb-TTB and PtON-tb-DTB devices have maximum external quantum efficiencies of 26.3% and 20.9%, respectively. Additionally, the PtON-tb-DTB device has an extended lifetime of 169.3 h with an initial luminescence of 1200 nit, which is 8.5 times greater than the PtON-TBBI device. Extended lifetime because of suppressed MMLCT and smaller displacement between the lowest triplet and triplet metal-centered states compared to other dopants. The study provides an effective approach to designing platinum(II) complexes for long device lifetimes.

4.
Nat Commun ; 15(1): 6153, 2024 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-39039039

RESUMO

Glycol sidechains are often used to enhance the performance of organic photoconversion and electrochemical devices. Herein, we study their effects on electronic states and electronic properties. We find that polymer glycolation not only induces more disordered packing, but also results in a higher reorganisation energy due to more localised π-electron density. Transient absorption spectroscopy and femtosecond stimulated Raman spectroscopy are utilised to monitor the structural relaxation dynamics coupled to the excited state formation upon photoexcitation. Singlet excitons are initially formed, followed by polaron pair formation. The associated structural relaxation slows down in glycolated polymers (5 ps vs. 1.25 ps for alkylated), consistent with larger reorganisation energy. This slower vibrational relaxation is found to drive ultrafast formation of the polaron pair state (5 ps vs. 10 ps for alkylated). These results provide key experimental evidence demonstrating the impact of molecular structure on electronic state formation driven by strong vibrational coupling.

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