Перевод заглавия: Наноструктуры люминесцентных нульразмерных гибридных тиогалогенов свинца для высокого квантового выхода и широкополосного спектра возбуждения
Кл.слова (ненормированные):
Zero-dimensional hybrid metal halide -- Luminescence -- Quantum yield -- Mechanochemical synthesis -- X-ray diffraction -- Dimethylthiourea
Аннотация: Luminescent trans-[Pb(DMTU-S)4Cl2] (DMTU: N,N′-dimethylthiourea) was designed and prepared via either mechanochemical or solvothermal methods, and the structures of DMTU and trans-[Pb(DMTU-S)4Cl2] have been resolved using X-ray single-crystal diffraction. Upon excitation over broadband covering the range from 450 to 250 nm, trans-[Pb(DMTU-S)4Cl2] shows yellow-green emission peaking at 549 nm with a spectral width of 110 nm, which is assigned to the triplet–singlet transition of Pb2+ ions within distorted heterogeneous S4Cl2 octahedra. The broadband excitation comprised singlet–singlet transitions of Pb2+ ions and energy transfer from orbitals involving those of organic ligands. Simultaneous analysis of the luminescent bandwidth and Stokes shift gives for Pb2+ ions in S4Cl2 octahedra the value of the Huang–Rhys parameter S = 4.25 and the energy of phonon involved in the formation of the luminescence spectrum of the order of 90 meV. Quantum yield as high as 91% is detected for excitation at 365 nm. This high quantum yield indicates the absence of noticeable concentration quenching at an average distance of 9.4 Å between the Pb2+ ions within the structure of trans-[Pb(DMTU)4Cl2]. The weak spin–orbit intersystem crossing is deduced from a high photoluminescence quantum yield (PLQY) value. Time dependent-density functional theory (TD-DFT) calculations of the nanocluster indicate the red shift of absorption bands in Pb(DMTU)4Cl2 with respect to parent DMTU. The high-performance photoluminescence and stability demonstrated promising applications in photonics.
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Держатели документа:
Siberian Federal University, Krasnoyarsk, 660041, Russian Federation
Department of Chemistry, Lomonosov Moscow State University, Moscow, 119991, Russian Federation
The State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Fiber Laser Materials and Applied Techniques, School of Materials Science and Technology, South China University of Technology, Guangzhou, 510641, China
Laboratory of Crystal Physics, Kirensky Institute of Physics, Federal Research Center, KSC, SB, RAS, Krasnoyarsk, 660036, Russian Federation
Research and Development Department, Kemerovo State University, Kemerovo 650000, Russian Federation
Доп.точки доступа:
Golovnev, N. N.; Aleksandrovsky, A. S.; Александровский, Александр Сергеевич; Gerasimova, M. A.; Tomilin, F. N.; Томилин, Феликс Николаевич; Mironov, V. A.; Demina, A. V.; Xia, Z.; Molokeev, M. S.; Молокеев, Максим Сергеевич