Strangely attractive: Collaboration and feedback in the field of molecular magnetism

Abstract

The fluid synergy between experimentalists and theoreticians has, for decades, led to a deeper understanding of the processes that govern single-molecule magnets. This approach has allowed for the establishment of proven design criteria for the control of magnetic properties through molecular architecture and the development of new magnetic measurement techniques and innovative computational methodologies.Here, we give an account of the experimental and theoretical joint endeavor carried out as part of the synthesis group led by David Mills and the computational/theoretical team led by Nicholas Chilton, together with colleagues in synthetic f-element chemistry and magnetism at the University of Manchester. In addition, we provide a personal perspective on collaborative work in molecular magnetism and how such collaborations are essential for advancing the field further. K E Y W O R D S collaboration between theoreticians and experimentalists, dysprosium, f-element, lanthanide, molecular magnetism, SMM

Spin–phonon coupling and magnetic relaxation in single-molecule magnets

“…However, as the phonon DoS (eqn ( 7)) must go to zero at zero energy (i.e. g(0) = 0), the anti-Lorentzian lineshape should be used instead (eqn (11)). In practice, however, there is little difference if Lorentzian or even Gaussian lineshapes are used.…”

Magnetic anisotropy and structural flexibility in the field-induced single ion magnets [Co{(OPPh2)(EPPh2)N}2], E = S, Se, explored by experimental and computational methods

“…[9][10][11] Thus, currently there is an increased interest in exploring slow relaxing mononuclear metal complexes, which are referred to either as mononuclear SMMs or as single ion magnets (SIMs). [12][13][14][15] Along these lines, intense research efforts have been devoted to mononuclear complexes of lanthanides [16][17][18][19][20][21] and actinides, 22 exhibiting large magnetic anisotropy. Potential applications of these materials include information-storage or molecular devices that could be employed for the design of quantum computers.…”

“…Potential applications of these materials include information-storage or molecular devices that could be employed for the design of quantum computers. [23][24][25] However, it should be stressed that the slow magnetization relaxation of SMMs and SIMs is limited to temperatures lower than the corresponding blocking temperature (T B ), 20 setting a target of increasing this limit to technologically manageable values. To that end, major breakthroughs have been reported during the last five years concerning lanthanide complexes, the T B value of which approaches, [26][27][28] or even surpasses, 29,30 that of liquid nitrogen (77 K).…”

Magnetic Properties and Electronic Structure of the S = 2 Complex [MnIII{(OPPh2)2N}3] Showing Field-Induced Slow Magnetization Relaxation

“…In an alternative approach, research efforts have been directed toward mononuclear complexes of lanthanides and actinides exhibiting large magnetic anisotropy, as well as blocking temperatures ( T B ) approaching, − or even surpassing, that of liquid nitrogen (77 K). There has also been an increased interest in exploring mononuclear transition-metal-based complexes, by both experimental − and computational methods. , Collectively, the above complexes are referred to as either mononuclear SMMs or single-ion magnets (SIMs) …”

“…9 However, such multinuclear systems usually exhibit only small magnetic anisotropies, 10−12 counteracting the favorable effect of a high S value on the magnitude of the effective energy barrier due to which SMMs exhibit slow relaxation of magnetization. 13 In an alternative approach, research efforts have been directed toward mononuclear complexes of lanthanides and actinides exhibiting large magnetic anisotropy, as well as blocking temperatures (T B ) 14 approaching, 15−17 or even surpassing, 18 that of liquid nitrogen (77 K). There has also been an increased interest in exploring mononuclear transitionmetal-based complexes, by both experimental 19−22 and computational methods.…”