期刊
JOURNAL OF PHYSICS-CONDENSED MATTER
卷 28, 期 20, 页码 -出版社
IOP PUBLISHING LTD
DOI: 10.1088/0953-8984/28/20/206002
关键词
spin-crossover; Fe(II) spin-crossover; molecular magnetism; spin state locking
资金
- National Science Foundation through the Nebraska MRSEC [DMR-1420645]
- Agence Nationale de la Recherche [11-BS08-06, 11-LABX-0058_NIE, ANR-10-IDEX-0002-02, 11-JS07-013-01]
- International Center for Frontier Research in Chemistry (icFRC, Strasbourg)
- U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]
Temperature-and coverage-dependent studies of the Au(1 1 1)-supported spin crossover Fe(II) complex (SCO) of the type [Fe(H2B(pz)(2))(2)(bipy)] with a suite of surface-sensitive spectroscopy and microscopy tools show that the substrate inhibits thermally induced transitions of the molecular spin state, so that both high-spin and low-spin states are preserved far beyond the spin transition temperature of free molecules. Scanning tunneling microscopy confirms that [Fe(H2B(pz) 2) 2(bipy)] grows as ordered, molecular bilayer islands at sub-monolayer coverage and as disordered film at higher coverage. The temperature dependence of the electronic structure suggest that the SCO films exhibit a mixture of spin states at room temperature, but upon cooling below the spin crossover transition the film spin state is best described as a mix of high-spin and low-spin state molecules of a ratio that is constant. This locking of the spin state is most likely the result of a substrate-induced conformational change of the interfacial molecules, but it is estimated that also the intra-atomic electron-electron Coulomb correlation energy, or Hubbard correlation energy U, could be an additional contributing factor.
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