Influence of Electron Correlation on the Electronic Structure and Magnetism of Transition-Metal Phthalocyanines

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• 作者：Iulia Emilia Brumboiu ; Soumyajyoti Haldar ; Johann Lüder ; Olle Eriksson ; Heike C. Herper ; Barbara Brena ; Biplab Sanyal
• 刊名：Journal of Chemical Theory and Computation
• 出版年：2016
• 出版时间：April 12, 2016
• 年：2016
• 卷：12
• 期：4
• 页码：1772-1785
• 全文大小：983K
• 年卷期：0
• ISSN：1549-9626

文摘

There exists an extensive literature on the electronic structure of transition-metal phthalocyanines (TMPcs), either as single molecules or adsorbed on surfaces, where explicit intra-atomic Coulomb interactions of the strongly correlated orbitals are included in the form of a Hubbard U term. The choice of U is, to a large extent, based solely on previous values reported in the literature for similar systems. Here, we provide a systematic analysis of the influence of electron correlation on the electronic structure and magnetism of several TMPcs (MnPc, FePc, CoPc, NiPc, and CuPc). By comparing calculated results to valence-band photoelectron spectroscopy measurements, and by determining the Hubbard term from linear response, we show that the choice of U is not as straightforward and can be different for each different TMPc. This, in turn, highlights the importance of individually estimating the value of U for each system before performing any further analysis and shows how this value can influence the final results.