Тип публикации: статья из журнала
Год издания: 2021
Идентификатор DOI: 10.1021/acsanm.1c00162
Ключевые слова: zero-dimensional hybrid metal halide, luminescence, quantum yield, mechanochemical synthesis, x-ray diffraction, dimethylthiourea
Аннотация: Luminescent trans-[Pb(DMTU-S)(4)Cl-2] (DMTU: N,N'-dimethylthiourea) was designed and prepared via either mechanochemical or solvothermal methods, and the structures of DMTU and trans-[Pb(DMTU-S)(4)Cl-2] have been resolved using Xray single-crystal diffraction. Upon excitation over broadband covering the range from 450 to 250 nm, trПоказать полностьюans-[Pb(DMTUS)(4)Cl-2] 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 angstrom between the Pb2+ ions within the structure of trans-[Pb(DMTU)(4)Cl-2]. 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)(4)Cl-2 with respect to parent DMTU. The high-performance photoluminescence and stability demonstrated promising applications in photonics.
Журнал: ACS APPLIED NANO MATERIALS
Выпуск журнала: Vol. 4, Is. 4
Номера страниц: 3654-3663
ISSN журнала: 25740970
Место издания: WASHINGTON
Издатель: AMER CHEMICAL SOC