Electronic Structure and Slow Magnetic Relaxation of Low-Coordinate Cyclic Alkyl(amino) Carbene Stabilized Iron(I) Complexes
Cyclic alkyl(amino) carbene stabilized two- and three-coordinate Fe(I) complexes, (cAAC)2FeCl (2) and [(cAAC)2Fe][B(C6F5)4] (3), respectively, were prepared and thoroughly studied by a bouquet of analytical techniques as well as theoretical calculations. Magnetic susceptibility and Mössbauer spectr...
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| Published in | Journal of the American Chemical Society Vol. 136; no. 34; pp. 11964 - 11971 |
|---|---|
| Main Authors | , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
27.08.2014
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| Subjects | |
| Online Access | Get full text |
| ISSN | 0002-7863 1520-5126 1520-5126 |
| DOI | 10.1021/ja5043116 |
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| Abstract | Cyclic alkyl(amino) carbene stabilized two- and three-coordinate Fe(I) complexes, (cAAC)2FeCl (2) and [(cAAC)2Fe][B(C6F5)4] (3), respectively, were prepared and thoroughly studied by a bouquet of analytical techniques as well as theoretical calculations. Magnetic susceptibility and Mössbauer spectroscopy reveal the +1 oxidation state and S = 3/2 spin ground state of iron in both compounds. 2 and 3 show slow magnetic relaxation typical for single molecule magnets under an applied direct current magnetic field. The high-frequency EPR measurements confirm the S = 3/2 ground state with a large, positive zero-field splitting (∼20.4 cm–1) and reveal easy plane anisotropy for compound 2. CASSCF/CASPT2/RASSI-SO ab initio calculations using the MOLCAS program package support the experimental results. |
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| AbstractList | Cyclic alkyl(amino) carbene stabilized two- and three-coordinate Fe(I) complexes, (cAAC)2FeCl (2) and [(cAAC)2Fe][B(C6F5)4] (3), respectively, were prepared and thoroughly studied by a bouquet of analytical techniques as well as theoretical calculations. Magnetic susceptibility and Mössbauer spectroscopy reveal the +1 oxidation state and S = 3/2 spin ground state of iron in both compounds. 2 and 3 show slow magnetic relaxation typical for single molecule magnets under an applied direct current magnetic field. The high-frequency EPR measurements confirm the S = 3/2 ground state with a large, positive zero-field splitting (∼20.4 cm–1) and reveal easy plane anisotropy for compound 2. CASSCF/CASPT2/RASSI-SO ab initio calculations using the MOLCAS program package support the experimental results. Cyclic alkyl(amino) carbene stabilized two- and three-coordinate Fe(I) complexes, (cAAC)2FeCl (2) and [(cAAC)2Fe][B(C6F5)4] (3), respectively, were prepared and thoroughly studied by a bouquet of analytical techniques as well as theoretical calculations. Magnetic susceptibility and Mössbauer spectroscopy reveal the +1 oxidation state and S = 3/2 spin ground state of iron in both compounds. 2 and 3 show slow magnetic relaxation typical for single molecule magnets under an applied direct current magnetic field. The high-frequency EPR measurements confirm the S = 3/2 ground state with a large, positive zero-field splitting (∼20.4 cm(-1)) and reveal easy plane anisotropy for compound 2. CASSCF/CASPT2/RASSI-SO ab initio calculations using the MOLCAS program package support the experimental results.Cyclic alkyl(amino) carbene stabilized two- and three-coordinate Fe(I) complexes, (cAAC)2FeCl (2) and [(cAAC)2Fe][B(C6F5)4] (3), respectively, were prepared and thoroughly studied by a bouquet of analytical techniques as well as theoretical calculations. Magnetic susceptibility and Mössbauer spectroscopy reveal the +1 oxidation state and S = 3/2 spin ground state of iron in both compounds. 2 and 3 show slow magnetic relaxation typical for single molecule magnets under an applied direct current magnetic field. The high-frequency EPR measurements confirm the S = 3/2 ground state with a large, positive zero-field splitting (∼20.4 cm(-1)) and reveal easy plane anisotropy for compound 2. CASSCF/CASPT2/RASSI-SO ab initio calculations using the MOLCAS program package support the experimental results. Cyclic alkyl(amino) carbene stabilized two- and three-coordinate Fe(I) complexes, (cAAC)2FeCl (2) and [(cAAC)2Fe][B(C6F5)4] (3), respectively, were prepared and thoroughly studied by a bouquet of analytical techniques as well as theoretical calculations. Magnetic susceptibility and Mössbauer spectroscopy reveal the +1 oxidation state and S = 3/2 spin ground state of iron in both compounds. 2 and 3 show slow magnetic relaxation typical for single molecule magnets under an applied direct current magnetic field. The high-frequency EPR measurements confirm the S = 3/2 ground state with a large, positive zero-field splitting (∼20.4 cm(-1)) and reveal easy plane anisotropy for compound 2. CASSCF/CASPT2/RASSI-SO ab initio calculations using the MOLCAS program package support the experimental results. Cyclic alkyl(amino) carbene stabilized two- and three-coordinate Fe(I) complexes, (cAAC)₂FeCl (2) and [(cAAC)₂Fe][B(C₆F₅)₄] (3), respectively, were prepared and thoroughly studied by a bouquet of analytical techniques as well as theoretical calculations. Magnetic susceptibility and Mössbauer spectroscopy reveal the +1 oxidation state and S = 3/2 spin ground state of iron in both compounds. 2 and 3 show slow magnetic relaxation typical for single molecule magnets under an applied direct current magnetic field. The high-frequency EPR measurements confirm the S = 3/2 ground state with a large, positive zero-field splitting (∼20.4 cm–¹) and reveal easy plane anisotropy for compound 2. CASSCF/CASPT2/RASSI-SO ab initio calculations using the MOLCAS program package support the experimental results. |
| Author | Mondal, Kartik Chandra Amin Sk, Nurul Ungur, Liviu Roesky, Herbert W Meyer, Franc Ramachandran, Vasanth Dalal, Naresh S van Tol, Johan Neufeld, Roman Chibotaru, Liviu F Carl, Elena Christian, Jonathan Demeshko, Serhiy Samuel, Prinson P Stalke, Dietmar |
| AuthorAffiliation | Institut für Anorganische Chemie Georg-August-Universität Florida State University National High Magnetic Field Laboratory Departments of Chemistry and Biochemistry KU Leuven |
| AuthorAffiliation_xml | – name: Departments of Chemistry and Biochemistry – name: Georg-August-Universität – name: KU Leuven – name: National High Magnetic Field Laboratory – name: Florida State University – name: Institut für Anorganische Chemie |
| Author_xml | – sequence: 1 givenname: Prinson P surname: Samuel fullname: Samuel, Prinson P – sequence: 2 givenname: Kartik Chandra surname: Mondal fullname: Mondal, Kartik Chandra – sequence: 3 givenname: Nurul surname: Amin Sk fullname: Amin Sk, Nurul – sequence: 4 givenname: Herbert W surname: Roesky fullname: Roesky, Herbert W email: hroesky@gwdg.de – sequence: 5 givenname: Elena surname: Carl fullname: Carl, Elena – sequence: 6 givenname: Roman surname: Neufeld fullname: Neufeld, Roman – sequence: 7 givenname: Dietmar surname: Stalke fullname: Stalke, Dietmar email: dstalke@chemie.uni-goettingen.de – sequence: 8 givenname: Serhiy surname: Demeshko fullname: Demeshko, Serhiy – sequence: 9 givenname: Franc surname: Meyer fullname: Meyer, Franc email: franc.meyer@chemie.uni-goettingen.de – sequence: 10 givenname: Liviu surname: Ungur fullname: Ungur, Liviu email: liviu.ungur@chem.kuleuven.be – sequence: 11 givenname: Liviu F surname: Chibotaru fullname: Chibotaru, Liviu F – sequence: 12 givenname: Jonathan surname: Christian fullname: Christian, Jonathan – sequence: 13 givenname: Vasanth surname: Ramachandran fullname: Ramachandran, Vasanth – sequence: 14 givenname: Johan surname: van Tol fullname: van Tol, Johan – sequence: 15 givenname: Naresh S surname: Dalal fullname: Dalal, Naresh S email: dalal@chem.fsu.edu |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/25072104$$D View this record in MEDLINE/PubMed |
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| Snippet | Cyclic alkyl(amino) carbene stabilized two- and three-coordinate Fe(I) complexes, (cAAC)2FeCl (2) and [(cAAC)2Fe][B(C6F5)4] (3), respectively, were prepared... Cyclic alkyl(amino) carbene stabilized two- and three-coordinate Fe(I) complexes, (cAAC)₂FeCl (2) and [(cAAC)₂Fe][B(C₆F₅)₄] (3), respectively, were prepared... |
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| SubjectTerms | iron magnetic fields magnetic materials oxidation spectroscopy |
| Title | Electronic Structure and Slow Magnetic Relaxation of Low-Coordinate Cyclic Alkyl(amino) Carbene Stabilized Iron(I) Complexes |
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