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  1. Free, publicly-accessible full text available February 1, 2024
  2. The [Co(SQ) 2 (4-CN-py) 2 ] complex exhibits dynamical effects over a wide range of temperature. The orbital moment, determined by X-ray magnetic circular dichroism (XMCD) with decreasing applied magnetic field, indicates a nonzero critical field for net alignment of magnetic moments, an effect not seen with the spin moment of [Co(SQ) 2 (4-CN-py) 2 ].
  3. Future molecular microelectronics require the electronic conductivity of the device to be tunable without impairing the voltage control of the molecular electronic properties. This work reports the influence of an interface between a semiconducting polyaniline polymer or a polar poly-D-lysine molecular film and one of two valence tautomeric complexes, i.e. , [Co III (SQ)(Cat)(4-CN-py) 2 ] ↔ [Co II (SQ) 2 (4-CN-py) 2 ] and [Co III (SQ)(Cat)(3-tpp) 2 ] ↔ [Co II (SQ) 2 (3-tpp) 2 ]. The electronic transitions and orbitals are identified using X-ray photoemission, X-ray absorption, inverse photoemission, and optical absorption spectroscopy measurements that are guided by density functional theory. Except for slightly modified binding energies and shifted orbital levels, the choice of the underlying substrate layer has little effect on the electronic structure. A prominent unoccupied ligand-to-metal charge transfer state exists in [Co III (SQ)(Cat)(3-tpp) 2 ] ↔ [Co II (SQ) 2 (3-tpp) 2 ] that is virtually insensitive to the interface between the polymer and tautomeric complexes in the Co II high-spin state.
  4. The X-ray-induced spin crossover transition of an Fe (II) molecular thin film in the presence and absence of a magnetic field has been investigated. The thermal activation energy barrier in the soft X-ray activation of the spin crossover transition for [Fe{H2B(pz)2}2(bipy)] molecular thin films is reduced in the presence of an applied magnetic field, as measured through X-ray absorption spectroscopy at various temperatures. The influence of a 1.8 T magnetic field is sufficient to cause deviations from the expected exponential spin state transition behavior which is measured in the field free case. We find that orbital moment diminishes with increasing temperature, relative to the spin moment in the vicinity of room temperature.