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RuII complexes incorporating both amide-linked bithiophene donor ancillary ligands and laminate acceptor ligands; dipyrido[3,2-a:2',3'-c]phenazine (dppz), tetrapyrido[3,2-a:2',3'-c:3'',2''-h:2''',3'''-j]phenazine (tpphz), and 9,11,20,22-tetraazatetrapyrido[3,2-a:2',3'-c:3'',2''-l:2''',3''']-pentacene (tatpp) exhibit long-lived charge separated (CS) states, which have been analyzed using time-resolved transient absorption (TA), fluorescence, and electronic absorption spectroscopy in addition to ground state electrochemical and spectroelectrochemical measurements. These complexes possess two electronically relevant ³MLCT states related to electron occupation of MOs localized predominantly on the proximal "bpy-like" portion and central (or distal) "phenazine-like" portion of the acceptor ligand as well as energetically similar ³LC and ³ILCT states. The unusually long excited state lifetimes (τ up to 7 μs) observed in these complexes reflect an equilibration of the ³MLCTprox or ³MLCTdist states with additional triplet states, including a ³LC state and a ³ILCT state that formally localizes a hole on the bithiophene moiety and an electron on the laminate acceptor ligand. Coordination of a ZnII ion to the open coordination site of the laminate acceptor ligand is observed to significantly lower the energy of the ³MLCTdist state by decreasing the magnitude of the excited state dipole and resulting in much shorter excited state lifetimes. The presence of the bithiophene donor group is reported to substantially extend the lifetime of these Zn adducts via formation of a ³ILCT state that can equilibrate with the ³MLCTdist state. In tpphz complexes, ZnII coordination can reorder the energy of the ³MLCTprox and ³MLCTdist states such that there is a distinct switch from one state to the other. The net result is a series of complexes that are capable of forming CS states with electron-hole spatial separation of up to 14 Å and possess exceptionally long lifetimes by equilibration with other triplet states.
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http://dx.doi.org/10.1002/chem.201203786 | DOI Listing |
ACS Sens
September 2024
Key Laboratory of Applied Surface and Colloid Chemistry of Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an 710119, P. R. China.
Efficient and reliable technologies for the on-site detection of illicit drugs are important in drug-facilitated crime investigations. However, the development of such technologies is challenging. Based on the synthetic optimization, introducing a boron ester functional group to the two furanic indicators endows the stimulus-responsive properties synergistically.
View Article and Find Full Text PDFNanotechnology
July 2024
State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou 510640, People's Republic of China.
To overcome the severe problems arising from the insufficient light absorption of ultrathin self-assembly active layers and the high cost use of atomic force deposition (ALD)-grown low-leakage-current transport layers, we successfully developed a low-cost, simple and facile strategy of floating-film transfer and multilayer lamination (FFTML) for constructing highly-efficient ALD-free broadband polarization-sensitive organic photodetectors (OPDs) with the two commonly used structures of donor/acceptor planar heterojunction (PHJ) and donor:acceptor multilayer bulk heterojunction (BHJ). It was found that the PHJ-based polarization-sensitive OPD by FFTML possesses a low dark current due to the high carrier injection barrier, indicating it is more suitable to be applied in low polarized light detection scenarios. In contrast, the BHJ-based device by FFTML has a higher spectral responsivity in the whole wavelength due to more photo-excitons transferred to the donor:acceptor interface and dissociated into photoexcited carrirers.
View Article and Find Full Text PDFNat Commun
May 2023
PCFM and LIFM Lab, School of Chemistry, Sun Yat-sen University, Guangzhou, 510275, P.R. China.
Photosensitizers (PSs) with nano- or micro-sized pore provide a great promise in the conversion of light energy into chemical fuel due to the excellent promotion for transporting singlet oxygen (O) into active sites. Despite such hollow PSs can be achieved by introducing molecular-level PSs into porous skeleton, however, the catalytic efficiency is far away from imagination because of the problems with pore deformation and blocking. Here, very ordered porous PSs with excellent O generation are presented from cross-linking of hierarchical porous laminates originated by co-assembly of hydrogen donative PSs and functionalized acceptor.
View Article and Find Full Text PDFJ Mater Chem A Mater
May 2022
Biomolecular and Organic Electronics, Department of Physics, Chemistry and Biology, Linköping University Linköping 58183 Sweden
The desired attributes of organic photovoltaics (OPV) as a low cost and sustainable energy harvesting technology demand the use of non-halogenated solvent processing for the photoactive layer (PAL) materials, preferably of low synthetic complexity (SC) and without compromising the power conversion efficiency (PCE). Despite their record PCEs, most donor-acceptor conjugated copolymers in combination with non-fullerene acceptors are still far from upscaling due to their high cost and SC. Here we present a non-halogenated and low SC ink formulation for the PAL of organic solar cells, comprising PTQ10 and PCBM as donor and acceptor materials, respectively, showing a record PCE of 7.
View Article and Find Full Text PDFNanomaterials (Basel)
April 2022
Shandong Provincial Key Laboratory of Molecular Engineering, School of Chemistry and Chemical Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, China.
Interface engineering is usually considered to be an efficient strategy to promote the separation and migration of photoexcited electron-hole pairs and improve photocatalytic performance. Herein, reduced graphene oxide/mesoporous titanium dioxide nanotube heterojunction assemblies (rGO/TiO) are fabricated via a facile hydrothermal method. The rGO is anchored on the surface of TiO nanosheet assembled nanotubes in a tightly manner due to the laminated effect, in which the formed heterojunction interface becomes efficient charge transfer channels to boost the photocatalytic performance.
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