Truncated forms of the second-rank orthorhombic Hamiltonians used in magnetism and electron magnetic resonance (EMR) studies are invalid—Why it went unnoticed for so long?

Abstract

This paper deals with the truncated forms of the second-rank orthorhombic Hamiltonians employed in magnetism and electron magnetic resonance (EMR) studies. Consideration of the intrinsic features of orthorhombic Hamiltonians reveals that the truncations, which consist in omission of one of three interdependent orthorhombic terms, are fundamentally invalid. Implications of the invalid truncations are: loss of generality of quantized spin models, misinterpretation of physical properties of systems studied (e.g. maximum rhombicity ratio and relative parameter values), and inconsistent notations for Hamiltonian parameters that hamper direct comparison of data from various sources. Truncated Hamiltonian forms identified in our survey are categorized and systematically reviewed. Examples are taken from studies of various magnetic systems, especially those involving transition ions, as well as model magnetic systems. The pertinent studies include magnetic ordering in three- and lower dimensions, e.g. [(CH 3) 4N]MnCl 3 (TMMC), canted ferromagnets, Haldane gap antiferromagnets, single molecule magnets exhibiting macroscopic quantum tunneling, e.g. Mn 12 complexes with spin S=10. Our study provides better insight into magnetic and spectroscopic properties of pertinent magnetic systems, which calls for reconsideration of the experimental and theoretical results based on invalid truncated Hamiltonians. The physical nature of Hamiltonians used in magnetism and EMR studies and other types of inappropriate terminology occurring, especially in model magnetism studies, require separate discussion.