Air‑stable High Performance Macrocyclic Dysprosium（Ⅲ） Single‑Ion Magnet

doi:10.19894/j.issn.1000-0518.220008

Chinese Journal of Applied Chemistry ›› 2022, Vol. 39 ›› Issue (10): 1586-1592.DOI: 10.19894/j.issn.1000-0518.220008

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Air‑stable High Performance Macrocyclic Dysprosium（Ⅲ） Single‑Ion Magnet

Hui LI¹^,², Zhen-Hua ZHU¹, Chen ZHAO¹^,², Jin-Kui TANG¹^,²()

^1.State Key Laboratory of Rare Earth Resource Utilization，Changchun Institute of Applied Chemistry，Chinese Academy of Sciences，Changchun 130022，China
^2.University of Science and Technology of China，Hefei 230026，China
^3.University of Chinese Academy of Sciences，Beijing 100049，China

Received:2022-01-10 Accepted:2022-03-19 Published:2022-10-01 Online:2022-10-05
Contact: Jin-Kui TANG
About author:tang@ciac.ac.cn
Supported by:
the Key Research Program of Frontier Sciences, CAS(ZDBS?LY?SLH023);the Key Research Program of the Chinese Academy of Sciences(ZDRW?CN?2021?3?3);the National Natural Science Foundation of China(21871247);the Royal Society?Newton Advanced Fellowship(NA160075)

1. Air stable High Performance Macrocyclic Dysprosium(III) Single Ion Magnet.pdf(487KB)

Abstract

Abstract:

Designing and preparing air-stable high-performance single-molecule magnets （SMMs） is of great significance toward the implementation of SMMs in high-density information storage， quantum computation and molecular-based spintronics devices. Herein， an air-stable macrocyclic Dy（III） single-ion magnet with pentagonal bipyramidal local symmetry is obtained by the reaction between N，N'-bis（2-aminoethyl）-1，3-propanediamine and 2，6-diacetylpyridine with the dysprosium ion as template. Single crystal X-ray diffraction reveals that the dysprosium ion is encapsulated in the equatorial plane with BPh₄^- as counter anion and the axial position is occupied by two Ph₃SiO^-. The state magnetic measurements gives the χ_MT value of 13.96 cm³·K/mol at room temperature， close to the theoretical value of 14.17 cm³·K/mol for one isolated Dy（III） ion. The dynamic magnetic measurements confirm its typical SMM behavior under a zero dc field with the effective magnetic reversal barrier up to 1008 K. Magneto-structural investigations show that the excellent SMM properties are attributed to the D_5h local symmetry and the strongly axial crystal field created by two Ph₃SiO^- for the dysprosium ion. Thermogravimetric analysis indicates that the compound is extremely air stable and the decomposition temperature reaches up to 297 ℃， which provides a promising avenue for depositing high performance SMMs on conductive substrate surfaces.

Key words: Single-ion magnet, Dysprosium ion, Crystal field, Anisotropy barrier

CLC Number:

O646.8

Hui LI, Zhen-Hua ZHU, Chen ZHAO, Jin-Kui TANG. Air‑stable High Performance Macrocyclic Dysprosium（Ⅲ） Single‑Ion Magnet[J]. Chinese Journal of Applied Chemistry, 2022, 39(10): 1586-1592.

Figures/Tables 6

Fig.1 Cationic structure （A） and equatorial plane （B） of ［Dy1（LN5）（Ph3SiO）2］（BPh4）·CH2Cl2. Dy， yellow green； O， red； N， blue； Si， orange； C， gray. Hydrogen atoms， solvent molecules and BPh4- are omitted for clarity

Fig.2 Temperature dependence of χMT values for compound ［Dy（LN5）（Ph3SiO）2］（BPh4）·CH2Cl2 under a DC field of 1000 Oe

Fig.3 Field dependence of magnetization for compound ［Dy（LN5）（Ph3SiO）2］（BPh4）·CH2Cl2 at temperatures of 5.0， 3.0 and 1.9 K

Fig.4 Frequency dependence of the out-of-phase χ″ ac susceptibility data for ［Dy（LN5）（Ph3SiO）2］（BPh4）·CH2Cl2 in temperature range of 2.0~66 K under a zero dc field

Fig.5 Temperature dependence of the relaxation time in the form of natural logarithm for compound ［Dy（LN5）（Ph3SiO）2］（BPh4）·CH2Cl2， the solid line represents the best fit to the overall magnetic relaxation process

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Air‑stable High Performance Macrocyclic Dysprosium（Ⅲ） Single‑Ion Magnet

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