曹東波 董梅

摘 要：采用九種DFT方法搭配七種基組對(duì)FeS0/-、FeS20/-、Fe2S20/-、Fe3S40/-和Fe4S40/- 進(jìn)行了系統(tǒng)的研究。通過對(duì)比，發(fā)現(xiàn)B3LYP和B3PW91搭配6-311+G*和QZVP基組計(jì)算的絕熱電子親和能（AEA）與實(shí)驗(yàn)值吻合的很好。采用B3LYP/6-311+G*計(jì)算了，確定了以上各團(tuán)簇結(jié)構(gòu)的基態(tài)電子態(tài)；發(fā)現(xiàn)其中，F(xiàn)e2S2、Fe3S4、Fe3S4-、Fe4S4和Fe4S4-具有反鐵磁性。同時(shí)用自然價(jià)鍵軌道理論（NBO）對(duì)團(tuán)簇的磁性進(jìn)行了分析。

關(guān)鍵詞：鐵硫團(tuán)簇；密度泛函理論；磁性

Abstract：The structures and energies of the electronic ground states of the FeS0/-， FeS20/-， Fe2S20/-， Fe3S40/- and Fe4S40/- neutral and anionic clusters have been computed systematically with nine computational methods in combination with seven basis sets in this thesis. The computed adiabatic electronic affinities （AEA） have been compared with the available experimental data. Most reasonable agreements between theory and experiment have been found for both hybrid B3LYP and B3PW91 functional in conjugation with the 6-311+G* and QZVP basis sets. Detailed comparisons between the available experimental and computed AEA data at B3LYP/6-311+G* identify the electronic ground state for the clusters involved. In addition， Fe2S2， Fe3S4， Fe3S4-， Fe4S4， and Fe4S4- are found to be antiferromagnetic at B3LYP/6-311+G* level. The magnetic properties have been discussed on the basis of natural bond orbital analysis.

Key word：Iron-sulfur Clusters；DFT；Magnetism

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