Ab Initio Prediction of Tunneling Relaxation Times and Effective Demagnetization Barriers in Kramers Lanthanide Single-Molecule Magnets

The Journal of Physical Chemistry Letters
Daniel Aravena

Abstract

Single-molecule magnets (SMMs) are promising candidates for molecule-based quantum information devices. Their main limitation is their cryogenic operative temperature. To achieve devices performing at higher temperatures, demagnetization mechanisms must be suppressed by chemical tuning. Electronic structure calculations can provide useful information to rationalize SMM behavior, but they do not provide a direct prediction for the key experimental parameters describing magnetic relaxation (i.e., tunneling relaxation time (τQT) and effective demagnetization barrier ( Ueff)). In this Letter, a first-principles model is proposed to predict τQT and Ueff for mononuclear, half-integer spin SMMs, allowing direct comparison with experiment. Model accuracy was assessed against experimental data for 18 mononuclear LnIII complexes (15 DyIII and 3 ErIII) and applied to 3 of the current best-performing SMMs, correctly predicting nontrivial relaxation pathways. The model shows that the combination of single-ion anisotropy and spin-spin dipolar coupling can account for the major part of tunneling demagnetization for the studied systems.

References

Aug 31, 2010·Angewandte Chemie·Shang-Da JiangSong Gao
Aug 16, 2011·Journal of the American Chemical Society·Jeffrey D RinehartJeffrey R Long
Sep 22, 2011·Chemistry : a European Journal·Ye BiSong Gao
Oct 29, 2011·Journal of the American Chemical Society·Matthew JeleticMuralee Murugesu
Feb 7, 2012·Chemistry : a European Journal·Gong-Jun ChenDai-Zheng Liao
Jul 25, 2013·Nature Chemistry·Robin J BlaggRichard E P Winpenny
Nov 19, 2013·Inorganic Chemistry·Daniel Aravena, Eliseo Ruiz
Jul 2, 2014·Nature Communications·Silvia Gómez-CocaFernando Luis
Jul 15, 2015·Chemical Society Reviews·Stephen T Liddle, Joris van Slageren
Feb 18, 2016·Journal of the American Chemical Society·Yan-Cong ChenMing-Liang Tong
Mar 11, 2016·Chemistry : a European Journal·Eva LucacciniLorenzo Sorace
Apr 8, 2016·Journal of the American Chemical Society·Jiang LiuMing-Liang Tong
Jan 12, 2017·Journal of the American Chemical Society·Katie L M HarrimanMuralee Murugesu
Jan 31, 2017·Chemistry : a European Journal·Yan-Cong ChenMing-Liang Tong
Mar 7, 2017·Nature Communications·Alessandro LunghiStefano Sanvito
Mar 14, 2017·Chemical Communications : Chem Comm·Y KishiL Ouahab
Jun 7, 2017·Angewandte Chemie·Fu-Sheng GuoRichard A Layfield
Aug 25, 2017·Nature·Conrad A P GoodwinDavid P Mills
Oct 11, 2017·Chemical Science·Alessandro LunghiRoberta Sessoli
Nov 4, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Lei ChenYou Song
Dec 8, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Sandeep K GuptaRamaswamy Murugavel
Mar 2, 2018·Chemical Society Reviews·Jun-Liang LiuMing-Liang Tong
Aug 1, 2016·Chemical Science·Sandeep K GuptaRamaswamy Murugavel

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Citations

May 9, 2019·Chemistry : a European Journal·Mei DingJeremy M Smith
Jun 11, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Matilde FondoJesús Sanmartín-Matalobos
Jun 27, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Daniel Aravena, Eliseo Ruiz
Oct 21, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Sourav Dey, Gopalan Rajaraman
Oct 21, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Ming KongYou Song
Oct 28, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Fang LuYi-Quan Zhang
Nov 26, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Yolimar GilDaniel Aravena
Dec 16, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Sheng ZhangSanping Chen
Jan 19, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·E PilichosJ Mayans
Jul 22, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Matteo Briganti, Federico Totti
Jul 22, 2021·Chemistry, an Asian Journal·Guo-Guo WengLi-Min Zheng
Jul 25, 2019·The Journal of Physical Chemistry. a·Ryan PedersonKyungwha Park
Sep 29, 2021·Chemistry : a European Journal·Martín AmozaEliseo Ruiz
Nov 18, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Yubao DongDongfeng Li
Dec 3, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Lena SpilleckeRüdiger Klingeler
Jan 7, 2022·Dalton Transactions : an International Journal of Inorganic Chemistry·Arpan Mondal, Sanjit Konar

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