TY - JOUR
T1 - Revealing Hot and Long-Lived Metastable Spin States in the Photoinduced Switching of Solvated Metallogrid Complexes with Femtosecond Optical and X-ray Spectroscopies
AU - Naumova, Maria A.
AU - Kalinko, Aleksandr
AU - Wong, Joanne W.L.
AU - Abdellah, Mohamed
AU - Geng, Huifang
AU - Domenichini, Edoardo
AU - Meng, Jie
AU - Gutierrez, Sol Alvarez
AU - Mante, Pierre Adrien
AU - Lin, Weihua
AU - Zalden, Peter
AU - Galler, Andreas
AU - Lima, Frederico
AU - Kubicek, Katharina
AU - Biednov, Mykola
AU - Britz, Alexander
AU - Checchia, Stefano
AU - Kabanova, Victoria
AU - Wulff, Michael
AU - Zimara, Jennifer
AU - Schwarzer, Dirk
AU - Demeshko, Serhiy
AU - Murzin, Vadim
AU - Gosztola, David
AU - Jarenmark, Martin
AU - Zhang, Jianxin
AU - Bauer, Matthias
AU - Lawson Daku, Max Latevi
AU - Gawelda, Wojciech
AU - Khakhulin, Dmitry
AU - Bressler, Christian
AU - Meyer, Franc
AU - Zheng, Kaibo
AU - Canton, Sophie E.
N1 - Publisher Copyright:
Copyright © 2020 American Chemical Society.
PY - 2020/3/19
Y1 - 2020/3/19
N2 - An atomistic understanding of the photoinduced spin-state switching (PSS) within polynuclear systems of d4-d7 transition metal ion complexes is required for their rational integration into light-driven reactions of chemical and biological interest. However, in contrast to mononuclear systems, the multidimensional dynamics of the PSS in solvated molecular arrays have not yet been elucidated due to the expected complications associated with the connectivity between the metal centers and the strong interactions with the surroundings. In this work, the PSS in a solvated triiron(II) metallogrid complex is characterized using transient optical absorption and X-ray emission spectroscopies on the femtosecond time scale. The complementary measurements reveal the photoinduced creation of energy-rich (hot) and long-lived quintet states, whose dynamics differ critically from their mononuclear congeners. This finding opens major prospects for developing novel schemes in solution-phase spin chemistry that are driven by the dynamic PSS process in compact oligometallic arrays.
AB - An atomistic understanding of the photoinduced spin-state switching (PSS) within polynuclear systems of d4-d7 transition metal ion complexes is required for their rational integration into light-driven reactions of chemical and biological interest. However, in contrast to mononuclear systems, the multidimensional dynamics of the PSS in solvated molecular arrays have not yet been elucidated due to the expected complications associated with the connectivity between the metal centers and the strong interactions with the surroundings. In this work, the PSS in a solvated triiron(II) metallogrid complex is characterized using transient optical absorption and X-ray emission spectroscopies on the femtosecond time scale. The complementary measurements reveal the photoinduced creation of energy-rich (hot) and long-lived quintet states, whose dynamics differ critically from their mononuclear congeners. This finding opens major prospects for developing novel schemes in solution-phase spin chemistry that are driven by the dynamic PSS process in compact oligometallic arrays.
UR - https://www.scopus.com/pages/publications/85082099243
U2 - 10.1021/acs.jpclett.9b03883
DO - 10.1021/acs.jpclett.9b03883
M3 - Article
C2 - 32069410
AN - SCOPUS:85082099243
SN - 1948-7185
VL - 11
SP - 2133
EP - 2141
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 6
ER -