Coexistence of Spin–Lattice Relaxation and Phonon-Bottleneck Processes in GdIII–Phthlocyaninato Triple-Decker Complexes under Highly Diluted Conditions

Yoji Horii; Keiichi Katoh; Yuji Miyazaki; Marko Damjanović; Tetsu Sato; Liviu Ungur; Liviu F. Chibotaru; Brian K. Breedlove; Motohiro Nakano; Wolfgang Wernsdorfer; Masahiro Yamashita

doi:10.1002/chem.201905796

Coexistence of Spin–Lattice Relaxation and Phonon-Bottleneck Processes in Gd^III–Phthlocyaninato Triple-Decker Complexes under Highly Diluted Conditions

Yoji Horii, Keiichi Katoh, Yuji Miyazaki, Marko Damjanović, Tetsu Sato, Liviu Ungur, Liviu F. Chibotaru, Brian K. Breedlove, Motohiro Nakano, Wolfgang Wernsdorfer, Masahiro Yamashita

SCI - Chemistry

Research output: Contribution to journal › Article › peer-review

8 Citations (Scopus)

Abstract

Gd³⁺ complexes have been shown to undergo unusual slow magnetic relaxation processes similar to those of single-molecule magnets (SMMs), even though Gd³⁺ does not exhibit strong magnetic anisotropy. To reveal the origin of the slow magnetic relaxation of Gd³⁺ complexes, we have investigated the magnetic properties and heat capacities of two Gd³⁺-phthalocyaninato triple-decker complexes, one of which has intramolecular Gd³⁺–Gd³⁺ interactions and the other does not. It was found that the Gd³⁺–Gd³⁺ interactions accelerate the magnetic relaxation processes. In addition, magnetically diluted samples, prepared by doping a small amount of the Gd³⁺ complexes into a large amount of diamagnetic Y³⁺ complexes, underwent dual magnetic relaxation processes. A detailed dynamic magnetic analysis revealed that the coexistence of spin–lattice relaxation and phonon-bottleneck processes is the origin of the dual magnetic relaxation processes.

Original language	English
Pages (from-to)	8076-8082
Number of pages	7
Journal	Chemistry - A European Journal
Volume	26
Issue number	36
DOIs	https://doi.org/10.1002/chem.201905796
Publication status	Published - 2020 Jun 26

Keywords

gadolinium
magnetic properties
phonon-bottleneck effect
porphyrinoids
spin–lattice relaxation

ASJC Scopus subject areas

Catalysis
Organic Chemistry

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10.1002/chem.201905796

Cite this

Horii, Y., Katoh, K., Miyazaki, Y., Damjanović, M., Sato, T., Ungur, L., Chibotaru, L. F., Breedlove, B. K., Nakano, M., Wernsdorfer, W., & Yamashita, M. (2020). Coexistence of Spin–Lattice Relaxation and Phonon-Bottleneck Processes in Gd^III–Phthlocyaninato Triple-Decker Complexes under Highly Diluted Conditions. Chemistry - A European Journal, 26(36), 8076-8082. https://doi.org/10.1002/chem.201905796

Horii, Y, Katoh, K, Miyazaki, Y, Damjanović, M, Sato, T, Ungur, L, Chibotaru, LF, Breedlove, BK, Nakano, M, Wernsdorfer, W & Yamashita, M 2020, 'Coexistence of Spin–Lattice Relaxation and Phonon-Bottleneck Processes in Gd^III–Phthlocyaninato Triple-Decker Complexes under Highly Diluted Conditions', Chemistry - A European Journal, vol. 26, no. 36, pp. 8076-8082. https://doi.org/10.1002/chem.201905796

@article{042527e12b2348efa77ab81ae8528859,

title = "Coexistence of Spin–Lattice Relaxation and Phonon-Bottleneck Processes in GdIII–Phthlocyaninato Triple-Decker Complexes under Highly Diluted Conditions",

abstract = "Gd3+ complexes have been shown to undergo unusual slow magnetic relaxation processes similar to those of single-molecule magnets (SMMs), even though Gd3+ does not exhibit strong magnetic anisotropy. To reveal the origin of the slow magnetic relaxation of Gd3+ complexes, we have investigated the magnetic properties and heat capacities of two Gd3+-phthalocyaninato triple-decker complexes, one of which has intramolecular Gd3+–Gd3+ interactions and the other does not. It was found that the Gd3+–Gd3+ interactions accelerate the magnetic relaxation processes. In addition, magnetically diluted samples, prepared by doping a small amount of the Gd3+ complexes into a large amount of diamagnetic Y3+ complexes, underwent dual magnetic relaxation processes. A detailed dynamic magnetic analysis revealed that the coexistence of spin–lattice relaxation and phonon-bottleneck processes is the origin of the dual magnetic relaxation processes.",

keywords = "gadolinium, magnetic properties, phonon-bottleneck effect, porphyrinoids, spin–lattice relaxation",

author = "Yoji Horii and Keiichi Katoh and Yuji Miyazaki and Marko Damjanovi{\'c} and Tetsu Sato and Liviu Ungur and Chibotaru, {Liviu F.} and Breedlove, {Brian K.} and Motohiro Nakano and Wolfgang Wernsdorfer and Masahiro Yamashita",

note = "Funding Information: This work was financially supported by the JSPS KAKENHI (Grant nos. JP20225003, JP15K05467, JP24750119, JP14J02656, JP17K19102, and JP18K14242), Tohoku University Molecule and Material Synthesis Platform in the Nanotechnology Platform Project, and CREST, JST (Grant No. JPMJCR12L3). M.Y. thanks the support by the 111 project (B18030) of China. We thank Dr. Y. Nakano for ICP‐AES measurements. The scientific grants R‐143‐000‐A80‐114 and R‐143‐ 000‐A65‐133 from the National University of Singapore are gratefully acknowledged. Computational resources from NSCC are gratefully acknowledged. This paper is Contribution No. 61 from the Research Center for Thermal and Entropic Science. Funding Information: This work was financially supported by the JSPS KAKENHI (Grant nos. JP20225003, JP15K05467, JP24750119, JP14J02656, JP17K19102, and JP18K14242), Tohoku University Molecule and Material Synthesis Platform in the Nanotechnology Platform Project, and CREST, JST (Grant No. JPMJCR12L3). M.Y. thanks the support by the 111 project (B18030) of China. We thank Dr. Y. Nakano for ICP-AES measurements. The scientific grants R-143-000-A80-114 and R-143- 000-A65-133 from the National University of Singapore are gratefully acknowledged. Computational resources from NSCC are gratefully acknowledged. This paper is Contribution No. 61 from the Research Center for Thermal and Entropic Science. Publisher Copyright: {\textcopyright} 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim",

year = "2020",

month = jun,

day = "26",

doi = "10.1002/chem.201905796",

language = "English",

volume = "26",

pages = "8076--8082",

journal = "Chemistry - A European Journal",

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publisher = "Wiley-VCH Verlag",

number = "36",

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TY - JOUR

T1 - Coexistence of Spin–Lattice Relaxation and Phonon-Bottleneck Processes in GdIII–Phthlocyaninato Triple-Decker Complexes under Highly Diluted Conditions

AU - Horii, Yoji

AU - Katoh, Keiichi

AU - Miyazaki, Yuji

AU - Damjanović, Marko

AU - Sato, Tetsu

AU - Ungur, Liviu

AU - Chibotaru, Liviu F.

AU - Breedlove, Brian K.

AU - Nakano, Motohiro

AU - Wernsdorfer, Wolfgang

AU - Yamashita, Masahiro

N1 - Funding Information: This work was financially supported by the JSPS KAKENHI (Grant nos. JP20225003, JP15K05467, JP24750119, JP14J02656, JP17K19102, and JP18K14242), Tohoku University Molecule and Material Synthesis Platform in the Nanotechnology Platform Project, and CREST, JST (Grant No. JPMJCR12L3). M.Y. thanks the support by the 111 project (B18030) of China. We thank Dr. Y. Nakano for ICP‐AES measurements. The scientific grants R‐143‐000‐A80‐114 and R‐143‐ 000‐A65‐133 from the National University of Singapore are gratefully acknowledged. Computational resources from NSCC are gratefully acknowledged. This paper is Contribution No. 61 from the Research Center for Thermal and Entropic Science. Funding Information: This work was financially supported by the JSPS KAKENHI (Grant nos. JP20225003, JP15K05467, JP24750119, JP14J02656, JP17K19102, and JP18K14242), Tohoku University Molecule and Material Synthesis Platform in the Nanotechnology Platform Project, and CREST, JST (Grant No. JPMJCR12L3). M.Y. thanks the support by the 111 project (B18030) of China. We thank Dr. Y. Nakano for ICP-AES measurements. The scientific grants R-143-000-A80-114 and R-143- 000-A65-133 from the National University of Singapore are gratefully acknowledged. Computational resources from NSCC are gratefully acknowledged. This paper is Contribution No. 61 from the Research Center for Thermal and Entropic Science. Publisher Copyright: © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

PY - 2020/6/26

Y1 - 2020/6/26

N2 - Gd3+ complexes have been shown to undergo unusual slow magnetic relaxation processes similar to those of single-molecule magnets (SMMs), even though Gd3+ does not exhibit strong magnetic anisotropy. To reveal the origin of the slow magnetic relaxation of Gd3+ complexes, we have investigated the magnetic properties and heat capacities of two Gd3+-phthalocyaninato triple-decker complexes, one of which has intramolecular Gd3+–Gd3+ interactions and the other does not. It was found that the Gd3+–Gd3+ interactions accelerate the magnetic relaxation processes. In addition, magnetically diluted samples, prepared by doping a small amount of the Gd3+ complexes into a large amount of diamagnetic Y3+ complexes, underwent dual magnetic relaxation processes. A detailed dynamic magnetic analysis revealed that the coexistence of spin–lattice relaxation and phonon-bottleneck processes is the origin of the dual magnetic relaxation processes.

AB - Gd3+ complexes have been shown to undergo unusual slow magnetic relaxation processes similar to those of single-molecule magnets (SMMs), even though Gd3+ does not exhibit strong magnetic anisotropy. To reveal the origin of the slow magnetic relaxation of Gd3+ complexes, we have investigated the magnetic properties and heat capacities of two Gd3+-phthalocyaninato triple-decker complexes, one of which has intramolecular Gd3+–Gd3+ interactions and the other does not. It was found that the Gd3+–Gd3+ interactions accelerate the magnetic relaxation processes. In addition, magnetically diluted samples, prepared by doping a small amount of the Gd3+ complexes into a large amount of diamagnetic Y3+ complexes, underwent dual magnetic relaxation processes. A detailed dynamic magnetic analysis revealed that the coexistence of spin–lattice relaxation and phonon-bottleneck processes is the origin of the dual magnetic relaxation processes.

KW - gadolinium

KW - magnetic properties

KW - phonon-bottleneck effect

KW - porphyrinoids

KW - spin–lattice relaxation

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JO - Chemistry - A European Journal

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