We report the precise design and synthesis of a fluorescent ligand(E)-4(((2,6-di(1H-pyrazol-1-yl)pyridin-4yl)methylene)amino)-N,N diphenylaniline(bpp-TPA),achieved through the covalent integration of a fluorophore tri...We report the precise design and synthesis of a fluorescent ligand(E)-4(((2,6-di(1H-pyrazol-1-yl)pyridin-4yl)methylene)amino)-N,N diphenylaniline(bpp-TPA),achieved through the covalent integration of a fluorophore triphenylamine(TpA)with the coordination subunit 2,6-bis(pyrazol-1-yl)pyridine(bpp),which provides a Nsoctahedral coordination environment optimized for Fe(Ⅱ),allowing us to prepare a mononuclear complex[Fe(bpp-TPA)_(2)]·(CFSO_(3))_(2)bpp-TPA-Fe.This complex exhibits a reversible thermally induced spin-state switching with a T12 of 311 K Meanwhile,the fluorescent intensity of bpp-TPA-Fe intensified distinctly upon spin-state conversion,reaching its maximum emission at 360 K,clearly indicative of a synergistic coupling between the SCO process and luminescent behavior.Benefiting from its carefully engineered intramolecular motional dynamics and donor-acceptor(D-A)molecuar architecture,bpp-TPA-Fe simultaneously ehibits pronounced aeerazztinindxed exziinn and thixted intamolecular change transter(TICT)r properties.Furthermore,large bathochromic shifts in the emission spectra with the increase in solution polarity are realized in this complex.This work exemplifies a highly precise molecular design strategy to construct multifunctional molecular materials with tunable magneto-optical properties,opening avenues for next-generation smart material applications.展开更多
基金supported by the National Science and Technology Major Project(2020YFE0204500)the National Natural Science Foundation of China(92261103 and 22301247)the Natural Science Foundation of Jilin Province State Key Laboratory Major Project(SKL202302037).
文摘We report the precise design and synthesis of a fluorescent ligand(E)-4(((2,6-di(1H-pyrazol-1-yl)pyridin-4yl)methylene)amino)-N,N diphenylaniline(bpp-TPA),achieved through the covalent integration of a fluorophore triphenylamine(TpA)with the coordination subunit 2,6-bis(pyrazol-1-yl)pyridine(bpp),which provides a Nsoctahedral coordination environment optimized for Fe(Ⅱ),allowing us to prepare a mononuclear complex[Fe(bpp-TPA)_(2)]·(CFSO_(3))_(2)bpp-TPA-Fe.This complex exhibits a reversible thermally induced spin-state switching with a T12 of 311 K Meanwhile,the fluorescent intensity of bpp-TPA-Fe intensified distinctly upon spin-state conversion,reaching its maximum emission at 360 K,clearly indicative of a synergistic coupling between the SCO process and luminescent behavior.Benefiting from its carefully engineered intramolecular motional dynamics and donor-acceptor(D-A)molecuar architecture,bpp-TPA-Fe simultaneously ehibits pronounced aeerazztinindxed exziinn and thixted intamolecular change transter(TICT)r properties.Furthermore,large bathochromic shifts in the emission spectra with the increase in solution polarity are realized in this complex.This work exemplifies a highly precise molecular design strategy to construct multifunctional molecular materials with tunable magneto-optical properties,opening avenues for next-generation smart material applications.
