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- Title
Structural Dynamics upon Photoexcitation in a Spin Crossover Crystal Probed with Femtosecond Electron Diffraction.
- Authors
Jiang, Yifeng; Liu, Lai Chung; Müller ‐ Werkmeister, Henrike M.; Lu, Cheng; Zhang, Dongfang; Field, Ryan L.; Sarracini, Antoine; Moriena, Gustavo; Collet, Eric; Miller, R. J. Dwayne
- Abstract
Photoexcitation of spin crossover (SCO) complexes can trigger extensive electronic spin transitions and transformation of molecular structure. However, the precise nature of the associated ultrafast structural dynamics remains elusive, especially in the solid state. Here, we studied a single-crystal SCO material with femtosecond electron diffraction (FED). The unique capability of FED allows us to directly probe atomic motions and to track ultrafast structural changes within a crystal lattice. By monitoring the time-dependent changes of the Bragg reflections, we observed the formation of a photoinduced structure similar to the thermally induced high-spin state. The data and refinement calculations indicate the global structural reorganization within 2.3 ps, as the metal-ligand bond distribution narrows during intramolecular vibrational energy redistribution (IVR) driving the intermolecular rearrangement. Three independent dynamical group are identified to model the structural dynamics upon photoinduced SCO.
- Subjects
PHOTOEXCITATION; SPIN crossover; MOLECULAR structure; STRUCTURAL dynamics; CRYSTAL lattices
- Publication
Angewandte Chemie, 2017, Vol 129, Issue 25, p7236
- ISSN
0044-8249
- Publication type
Article
- DOI
10.1002/ange.201702497