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Title: Meta-Atom Behavior in Clusters Revealing Large Spin Ground States

Abstract

The field of single molecule magnetism remains predicated on super- and double exchange mechanisms to engender large spin ground states. An alternative approach to achieving high-spin architectures involves synthesizing weak-field clusters featuring close M–M interactions to produce a single valence orbital manifold. Population of this orbital manifold in accordance with Hund’s rules could potentially yield thermally persistent high-spin ground states under which the valence electrons remain coupled. We now demonstrate this effect with a reduced hexanuclear iron cluster that achieves an S = 19/2 (χMT ≈ 53 cm3 K/mol) ground state that persists to 300 K, representing the largest spin ground state persistent to room temperature reported to date. The reduced cluster displays single molecule magnet behavior manifest in both variable-temperature zero-field 57Fe Mössbauer and magnetometry with a spin reversal barrier of 42.5(8) cm -1 and a magnetic blocking temperature of 2.9 K (0.059 K/min).

Authors:
 [1];  [1]
  1. Harvard Univ., Cambridge, MA (United States)
Publication Date:
Research Org.:
Harvard Univ., Cambridge, MA (United States)
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
OSTI Identifier:
1467660
Grant/Contract Number:  
SC0008313
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 137; Journal Issue: 43; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Hernández Sánchez, Raúl, and Betley, Theodore A. Meta-Atom Behavior in Clusters Revealing Large Spin Ground States. United States: N. p., 2015. Web. doi:10.1021/jacs.5b08962.
Hernández Sánchez, Raúl, & Betley, Theodore A. Meta-Atom Behavior in Clusters Revealing Large Spin Ground States. United States. doi:10.1021/jacs.5b08962.
Hernández Sánchez, Raúl, and Betley, Theodore A. Tue . "Meta-Atom Behavior in Clusters Revealing Large Spin Ground States". United States. doi:10.1021/jacs.5b08962. https://www.osti.gov/servlets/purl/1467660.
@article{osti_1467660,
title = {Meta-Atom Behavior in Clusters Revealing Large Spin Ground States},
author = {Hernández Sánchez, Raúl and Betley, Theodore A.},
abstractNote = {The field of single molecule magnetism remains predicated on super- and double exchange mechanisms to engender large spin ground states. An alternative approach to achieving high-spin architectures involves synthesizing weak-field clusters featuring close M–M interactions to produce a single valence orbital manifold. Population of this orbital manifold in accordance with Hund’s rules could potentially yield thermally persistent high-spin ground states under which the valence electrons remain coupled. We now demonstrate this effect with a reduced hexanuclear iron cluster that achieves an S = 19/2 (χMT ≈ 53 cm3 K/mol) ground state that persists to 300 K, representing the largest spin ground state persistent to room temperature reported to date. The reduced cluster displays single molecule magnet behavior manifest in both variable-temperature zero-field 57Fe Mössbauer and magnetometry with a spin reversal barrier of 42.5(8) cm-1 and a magnetic blocking temperature of 2.9 K (0.059 K/min).},
doi = {10.1021/jacs.5b08962},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 43,
volume = 137,
place = {United States},
year = {2015},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 6 works
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