Size-Dependent Ligand Quenching of Ferromagnetism in Co3(benzene)n+ Clusters Studied with X-ray Magnetic Circular Dichroism Spectroscopy

被引：28

作者：

Akin, Scott T. ^{[1
]}

Zamudio-Bayer, Vicente ^{[2
,3
]}

Duanmu, Kaining ^{[4
,5
]}

Leistner, Georg ^{[2
,6
]}

Hirsch, Konstantin ^{[2
,6
]}

Buelow, Christine ^{[2
,6
]}

Lawicki, Arkadiusz ^{[2
]}

Terasaki, Akira ^{[7
,8
]}

von Issendorff, Bernd ^{[3
]}

Truhlar, Donald G. ^{[4
,5
]}

Lau, J. Tobias ^{[2
]}

Duncan, Michael A. ^{[1
]}

机构：

[1] Univ Georgia, Dept Chem, Athens, GA 30602 USA

[2] Helmholtz Zentrum Berlin Mat & Energie, Inst Methoden & Instrumentierung Forsch Synchrotr, Albert Einstein Str 15, D-12489 Berlin, Germany

[3] Univ Freiburg, Inst Phys, Stefan Meier Str 21, D-79104 Freiburg, Germany

[4] Univ Minnesota, Chem Theory Ctr, Dept Chem, Minneapolis, MN 55455 USA

[5] Univ Minnesota, Supercomp Inst, Minneapolis, MN 55455 USA

[6] Tech Univ Berlin, Inst Opt & Atomare Phys, Hardenbergstr 36, D-10623 Berlin, Germany

[7] Genesis Res Inst Inc, East Tokyo Lab, 717-86 Futamata, Ichikawa, Chiba 2720001, Japan

[8] Kyushu Univ, Fac Sci, Dept Chem, Nishi Ku, 744 Motooka, Fukuoka 8190395, Japan

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2016年 / 7卷 / 22期

关键词：

INITIO MOLECULAR-DYNAMICS; DENSITY-FUNCTIONAL THEORY; TRANSITION-METAL ATOMS; SMALL FE CLUSTERS; NICKEL CLUSTERS; STERN-GERLACH; NI CLUSTERS; FREE COBALT; SPIN; ANISOTROPY;

D O I：

10.1021/acs.jpclett.6b01839

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Cobalt-benzene cluster ions of the form Co-3(bz)(n)(+) (n = 0-3) were produced in the gas phase, mass-selected, and cooled in a cryogenic ion trap held at 3-4 K. To explore ligand effects on cluster magnetic moments, these species were investigated with X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) spectroscopy. XMCD spectra yield both the spin and orbital angular momenta of these clusters. Co-3(+) has a spin magnetic moment of mu(S) = 6 mu(B) and an orbital magnetic moment of mu(L) = 3 mu(B). Co-3(bz)(+) and Co-3(bz)(2)(+) complexes were found to have spin and orbital magnetic moments identical to the values for ligand-free Co-3(+). However, coordination of the third benzene to form Co-3(bz)(3)(+) completely quenches the high spin state of the system. Density functional theory calculations elucidate the spin states of the Co-3(bz)(n)(+) species as a function of the number of attached benzene ligands, explaining the transition from septet to singlet for n = 0 -> 3.

引用

页码：4568 / 4575

页数：8

共 88 条

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