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Intermolecular Interaction Tuning of Spin-Crossover Iron(III) Complexes with Aromatic Counteranions.
Asami Tsukiashi1, Manabu Nakaya1, Fumiya Kobayashi1
1Department of Chemistry, Faculty of Advanced Science and Technology , Kumamoto University , 2-39-1 Kurokami , Chuo-ku, Kumamoto 860-8555 , Japan.
Inorganic Chemistry
|February 21, 2018
Summary
New iron(III) spin-crossover (SCO) complexes were synthesized. Some complexes exhibit the light-induced excited spin-state trapping (LIESST) effect, with one showing high conversion to a metastable state.
Area of Science:
- Coordination Chemistry
- Materials Science
- Solid-State Physics
Background:
- Spin-crossover (SCO) complexes are molecular materials exhibiting a reversible switch between low-spin (LS) and high-spin (HS) states.
- Tuning intermolecular interactions via counteranions is crucial for controlling SCO properties and light-induced phenomena.
- The light-induced excited spin-state trapping (LIESST) effect offers a pathway to stabilize metastable HS states at low temperatures.
Purpose of the Study:
- To synthesize and characterize novel Iron(III) spin-crossover complexes with aromatic counteranions.
- To investigate the influence of aromatic counteranions (benzenesulfonate, naphthalenesulfonate, pyrenesulfonate) on SCO behavior and intermolecular interactions.
- To explore the occurrence and efficiency of the LIESST effect in these newly synthesized SCO complexes.
Main Methods:
- Synthesis of four Iron(III) complexes: [Fe(qsal)2]BS·MeOH·H2O (1), [Fe(qsal)2](NS)·MeOH (2), [Fe(qnal)2](NS) (3), and [Fe(qnal)2]PS·MeOH·CH2Cl2 (4).
- Characterization using X-ray structure determination to analyze crystal packing and intermolecular interactions.
- Temperature-dependent magnetic susceptibility measurements to confirm SCO behavior and low-temperature illumination experiments (λ 808 nm, 5 K) to study the LIESST effect.
Main Results:
- All synthesized complexes exhibit temperature-dependent SCO behavior.
- The LIESST effect was observed in complexes 1, 3, and 4 upon illumination at 5 K.
- Complex 1 showed a high conversion rate (59%) to the metastable HS state, among the highest reported for [Fe(qsal)2]+ derivatives. Complex 2 lacked a LIESST effect, potentially due to weaker cation-anion interactions and larger Fe···Fe distances.
Conclusions:
- Aromatic counteranions effectively tune intermolecular coupling in Iron(III) SCO complexes.
- The presence and efficiency of the LIESST effect are strongly influenced by crystal packing and cation-anion interactions.
- These findings contribute to the design of molecular switches with tunable SCO properties and light-responsive behavior.
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