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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(25):7236-7240
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. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(46):14880-14885
Oxidative fusion reactions of ortho ‐phenylene‐bridged cyclic hexapyrroles and hexathiophenes furnished novel closed helicenes in a selective manner. X‐Ray diffraction analysis unambiguously revealed the structures to be a closed pentaaza[9]helicene, the longest azahelicene reported so far, and an unexpected double‐helical structure of hexathia[9]/[5]helicene, whose formation was assumed to result from multiple oxidative fusion along with a 1,2‐aryl shift. The pentaaza[9]helicene exhibited well‐defined emission with high fluorescence quantum yield (Φ F=0.31) among the known [9]helicenes. Chiral resolution of the racemic pentaaza[9]helicene and hexathia[9]/[5]helicene were achieved by chiral‐phase HPLC and the enantiomers were characterized by circular dichroism spectra and DFT calculations. 相似文献
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