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Singly and triply linked magnetic porphyrin lanthanide arrays

Abstract:
The introduction of paramagnetic metal centers into a conjugated π-system is a promising approach toward engineering spintronic materials. Here, we report an investigation of two types of spin-bearing dysprosium(III) and gadolinium(III) porphyrin dimers: singly meso–meso-linked dimers with twisted conformations and planar edge-fused β,meso,β-linked tapes. The rare-earth spin centers sit out of the plane of the porphyrin, so that the singly linked dimers are chiral, and their enantiomers can be resolved, whereas the edge-fused tape complexes can be separated into syn and anti stereoisomers. We compare the crystal structures, UV–vis–NIR absorption spectra, electrochemistry, EPR spectroscopy, and magnetic behavior of these complexes. Low-temperature SQUID magnetometry measurements reveal intramolecular antiferromagnetic exchange coupling between the GdIII centers in the edge-fused dimers (syn isomer: J = −51 ± 2 MHz; anti isomer: J = −19 ± 3 MHz), whereas no exchange coupling is detected in the singly linked twisted complex. The phase-memory times, Tm, are in the range of 8–10 μs at 3 K, which is long enough to test quantum computational schemes using microwave pulses. Both the syn and anti Dy2 edge-fused tapes exhibit single-molecule magnetic hysteresis cycles at temperatures below 0.5 K with slow magnetization dynamics.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1021/jacs.2c02084

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Role:
Author
ORCID:
0000-0003-2979-5698
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Role:
Author
ORCID:
0000-0002-1200-7686



Publisher:
American Chemical Society
Journal:
Journal of the American Chemical Society More from this journal
Volume:
144
Issue:
19
Pages:
8693–8706
Publication date:
2022-05-03
Acceptance date:
2022-04-20
DOI:
EISSN:
1520-5126
ISSN:
0002-7863


Language:
English
Keywords:
Pubs id:
1256217
Local pid:
pubs:1256217
Deposit date:
2022-05-04
ARK identifier:

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