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1.
Chem Commun (Camb) ; 60(8): 988-991, 2024 Jan 23.
Artículo en Inglés | MEDLINE | ID: mdl-38167668

RESUMEN

Delamination of the electron-transporting polymer N2200 from indium tin oxide (ITO) in aqueous electrolytes is mitigated by modifying ITO with an azide-functionalized phosphonic acid (PA) which, upon UV irradiation, reacts with the polymer. The optical, electrochemical, and spectroelectrochemical properties of N2200 thin films are retained in aqueous and non-aqueous media.

2.
J Phys Chem C Nanomater Interfaces ; 128(15): 6392-6400, 2024 Apr 18.
Artículo en Inglés | MEDLINE | ID: mdl-38655059

RESUMEN

Conjugated polymers composed of alternating electron donor and acceptor segments have come to dominate the materials being considered for organic photoelectrodes and solar cells, in large part because of their favorable near-infrared absorption. The prototypical electron-transporting push-pull polymer poly(NDI2OD-T2) (N2200) is one such material. While reasonably efficient organic solar cells can be fabricated with N2200 as the acceptor, it generally fails to contribute as much photocurrent from its absorption bands as the donor with which it is paired. Moreover, transient absorption studies have shown N2200 to have a consistently short excited-state lifetime (∼100 ps) that is dominated by a ground-state recovery. In this paper, we investigate whether these characteristics are intrinsic to the backbone structure of this polymer or if these are extrinsic effects from ubiquitous solution-phase and thin-film aggregates. We compare the solution-phase photophysics of N2200 with those of a pair of model compounds composed of alternating bithiophene (T2) donor and naphthalene diimide (NDI) acceptor units, NDI-T2-NDI and T2-NDI-T2, in a dilute solution. We find that the model compounds have even faster ground-state recovery dynamics (τ = 45, 27 ps) than the polymer (τ = 133 ps), despite remaining molecularly isolated in solution. In these molecules, as in the case of the N2200 polymer, the lowest excited state has a T2 to NDI charge-transfer (CT) character. Electronic-structure calculations indicate that the short lifetime of this state is due to fast nonradiative decay to the ground state (GS) promoted by strong CT-GS electronic coupling and strong electron-vibrational coupling with high-frequency (quantum) normal modes.

3.
J Phys Chem Lett ; 14(29): 6601-6609, 2023 Jul 27.
Artículo en Inglés | MEDLINE | ID: mdl-37459166

RESUMEN

The ternary blend approach accomplished improved spectral coverage and enhanced the power conversion efficiency (PCE) of organic solar cells (OSCs). However, the role of the third component in improving the photovoltaic parameters needs critical analysis. Here, we introduced a wide band gap n-type twisted perylene diimide (TPDI) into the PM6:Y6 blend as a third component that improves spectral coverage and morphology, resulting in an overall increase in the efficiency of the OSCs. TPDI acts as an antenna for efficient energy- and charge-transfer processes. A systematic study compared charge- and energy-transfer dynamics and the orientational dependence nanomorphology of ternary blends with those of their binary counterparts. Femtosecond transient absorption measurements reveal enhanced hole-transfer efficiency in finely tuned ternary mixtures. This study provides a rational approach to identifying a third component to improve light management and morphology. These parameters enhance the energy and charge-transfer processes, improving the PCE of OSCs.

4.
ACS Appl Mater Interfaces ; 15(21): 25224-25231, 2023 May 31.
Artículo en Inglés | MEDLINE | ID: mdl-37191283

RESUMEN

The introduction of nonfullerene acceptors (NFA) facilitated the realization of high-efficiency organic solar cells (OSCs); however, OSCs suffer from relatively large losses in open-circuit voltage (VOC) as compared to inorganic or perovskite solar cells. Further enhancement in power conversion efficiency requires an increase in VOC. In this work, we take advantage of the high dipole moment of twisted perylene-diimide (TPDI) as a nonfullerene acceptor (NFA) to enhance the VOC of OSCs. In multiple bulk heterojunction solar cells incorporating TPDI with three polymer donors (PTB7-Th, PM6 and PBDB-T), we observed a VOC enhancement by modifying the cathode with a polyethylenimine (PEIE) interlayer. We show that the dipolar interaction between the TPDI NFA and PEIE─enhanced by the general tendency of TPDI to form J-aggregates─plays a crucial role in reducing nonradiative voltage losses under a constant radiative limit of VOC. This is aided by comparative studies with PM6:Y6 bulk heterojunction solar cells. We hypothesize that incorporating NFAs with significant dipole moments is a feasible approach to improving the VOC of OSCs.

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