Magnetic Ordering in Gold Nanoclusters

Agrachev, Mikhail; Antonello, Sabrina; Dainese, Tiziano; Ruzzi, Marco; Zoleo, Alfonso; Apra, Edoardo; Govind, Niranjan; Fortunelli, Alessandro; Sementa, Luca; Maran, Flavio

doi:10.1021/acsomega.7b00472

Title: Magnetic Ordering in Gold Nanoclusters

Journal Article · Mon Jun 12 00:00:00 EDT 2017 · ACS Omega

DOI:https://doi.org/10.1021/acsomega.7b00472· OSTI ID:1363986

Agrachev, Mikhail ^[1]; Antonello, Sabrina ^[1]; Dainese, Tiziano ^[1]; Ruzzi, Marco ^[1]; Zoleo, Alfonso ^[1];

^[2]; Govind, Niranjan ^[2];

^[3]; Sementa, Luca ^[3];

^[4]

Univ. of Padova, Padova (Italy)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
CNR-ICCOM & IPCF, Pisa (Italy)
Univ. of Padova, Padova (Italy); Univ. of Connecticut, Storrs, CT (United States)

Here, several research groups have observed magnetism in monolayer-protected gold-cluster samples, but the results were often contradictory and thus a clear understanding of this phenomenon is still missing. We used Au₂₅(SCH₂CH₂Ph)₁₈⁰, which is a paramagnetic cluster that can be prepared with atomic precision and whose structure is known precisely. Previous magnetometry studies only detected paramagnetism. We used samples representing a range of crystallographic orders and studied their magnetic behaviors by electron paramagnetic resonance (EPR). As a film, Au₂₅(SCH₂CH₂Ph)₁₈⁰ displays paramagnetic behavior but, at low temperature, ferromagnetic interactions are detectable. One or few single crystals undergo physical reorientation with the applied field and display ferromagnetism, as detected through hysteresis experiments. A large collection of microcrystals is magnetic even at room temperature and shows distinct paramagnetic, superparamagnetic, and ferromagnetic behaviors. Simulation of the EPR spectra shows that both spin-orbit coupling and crystal distortion are important to determine the observed magnetic behaviors. DFT calculations carried out on single cluster and periodic models predict values of spin6orbit coupling and crystal6splitting effects in agreement with the EPR derived quantities. Magnetism in gold nanoclusters is thus demonstrated to be the outcome of a very delicate balance of factors. To obtain reproducible results, the samples must be (i) controlled for composition and thus be monodispersed with atomic precision, (ii) of known charge state, and (iii) well defined also in terms of crystallinity and experimental conditions. This study highlights the efficacy of EPR spectroscopy to provide a molecular understanding of these phenomena

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1363986

Report Number(s):: PNNL-SA-125554; 49645; KP1704020

Journal Information:: ACS Omega, Vol. 2, Issue 6; ISSN 2470-1343

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 53 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Magnetic Ordering in Gold Nanoclusters

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