Terminal Ligand and Packing Effects on Slow Relaxation in an Isostructural Set of [Dy(H2dapp)X2]+ Single Molecule Magnets**

Pfleger, Rouven F.; Schlittenhardt, Sören; Merkel, Marcus; Rüben, Mario; Fink, Karin; Anson, Christopher E.; Bendix, Jesper; Powell, Annie K.

doi:10.1002/chem.202102918

Cited by 8 publications

(4 citation statements)

References 52 publications

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“…Restricting the sums in Eq. 14 to a few modes, whose energy and coupling are left as adjustable parameters, it was shown that additional insights on spin relaxation can be obtained with respect to a fitting done with simple power laws ( 23 , 48 – 50 ).…”

Section: Discussionmentioning

confidence: 99%

Toward exact predictions of spin-phonon relaxation times: An ab initio implementation of open quantum systems theory

Lunghi

2022

Sci. Adv.

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Spin-phonon coupling is the main driver of spin relaxation and decoherence in solid-state semiconductors at finite temperature. Controlling this interaction is a central problem for many disciplines, ranging from magnetic resonance to quantum technologies. Spin relaxation theories have been developed for almost a century but often use a phenomenological description of phonons and their coupling to spin, resulting in a nonpredictive tool and hindering our detailed understanding of spin dynamics. Here, we combine time-local master equations up to the fourth order with advanced electronic structure methods and perform predictions of spin-phonon relaxation time for a series of solid-state coordination compounds based on both transition metals and lanthanide Kramers ions. The agreement between experiments and simulations demonstrates that an accurate, universal, and fully ab initio implementation of spin relaxation theory is possible, thus paving the way to a systematic study of spin-phonon relaxation in solid-state materials.

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Section: Discussionmentioning

confidence: 99%

Toward exact predictions of spin-phonon relaxation times: An ab initio implementation of open quantum systems theory

Lunghi

2022

Sci. Adv.

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“…199 contains the frequency of the phonons contributing to relaxation and therefore is able to provide a clearer interpretation of relaxation experiments. Such approach has been successfully applied to a series of spin 1/2 systems [98,99,109,110].…”

Section: The Mechanism Of Spin-phonon Relaxation In Magnetic Moleculesmentioning

confidence: 99%

Spin-Phonon Relaxation in Magnetic Molecules: Theory, Predictions and Insights

Lunghi¹

2022

Preprint

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Magnetic molecules have played a central role in the development of magnetism and coordination chemistry and their study keeps leading innovation in cutting-edge scientific fields such as magnetic resonance, magnetism, spintronics, and quantum technologies. Crucially, a long spin lifetime well above cryogenic temperature is a stringent requirement for all these applications. In this chapter we review the foundations of spin relaxation theory and provide a detailed overview of first-principles strategies applied to the problem of spin-phonon relaxation in magnetic molecules. Firstly, we present a rigorous formalism of spin-phonon relaxation based on open quantum systems theory. These results are then used to derive classical phenomenological relations based on the Debye model. Finally, we provide a prescription of how to map the relaxation formalism onto existing electronic structure methods to obtain a quantitative picture of spin-phonon relaxation. Examples from the literature, including both transition metals and lanthanides compounds, will be discussed in order to illustrate how Direct, Orbach and Raman relaxation mechanisms can affect spin dynamics for this class of compounds.

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“…[5,7,12,13,15,22] There are two reviews: one is focused on elucidating the magnetic benefits and challenges of cooperativity within 3d-4f based coordination clusters of archetypical butterfly type, [21] and the other one highlights more generally the advancement of inorganic coordination chemistry by spectroscopy of isolated molecules in view of the applied methods and the achieved applications. [18] Three communications, [3,12,22] one concept article [8] and 17 full papers [1,2,[4][5][6][7][9][10][11][13][14][15][16][17]19,20,23] document and discuss particular 3MET species and their relevance for our understanding of the TM interactions within. A contribution on the development and application of a complete active space spin-orbit configuration interaction program designed for molecule magnets deserves special mention: this manuscript appears in a more specialized sister journal.…”

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confidence: 99%

“…The current special issue of Chemistry -a European Journal issue comprises 23 contributions in total, 17 of which stem from work that was conducted within the framework of the 3MET.de center, [1][2][3][4]6,[8][9][10][11]14,[16][17][18][19][20][21]23] and six from outside. [5,7,12,13,15,22] There are two reviews: one is focused on elucidating the magnetic benefits and challenges of cooperativity within 3d-4f based coordination clusters of archetypical butterfly type, [21] and the other one highlights more generally the advancement of inorganic coordination chemistry by spectroscopy of isolated molecules in view of the applied methods and the achieved applications.…”

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confidence: 99%

Cooperative Effects in Heterometallic Complexes

Prosenc

Kappes

Niedner‐Schatteburg

2021

Chemistry A European J

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This special issue on "Cooperative effects in heterometallic complexes" documents research focused on the synthesis, physicochemical characterization, and theoretical description of ligand-stabilized homo-and heterobimetallic complexes containing only a few metal atoms -typically three. We call them 3MET complexes in short -also to reflect the title of the transregional collaborative research center 3MET.de founded in 2009 and located at the TU Kaiserslautern (TUK) and at the Karlsruhe Institute of Technology (KIT).Both fully coordinated and coordinatively unsaturated species are of interest. In such 3MET complexes, the metal centers are often bound by way of bridging ligands, which facilitate controlled variation of metal-to-metal distances and relative orientations in order to characterize the corresponding structure/property relations at a fundamental level. This in turn allows us to elucidate how metal-metal interactions in multinuclear complexes and clusters comprising transition-metal and/or lanthanide atoms contribute to determining their properties. It also enables the identification of optimal systems and properties for future applications in the contexts of photoactive materials, optoelectronics, magnetic information storage, quantum computing, and selective catalysis.A central issue is to understand the transition between weak metal center coupling and stronger bonding, e. g., aurophilic or metallic, when separations between metal centers are varied by making use of appropriate ligands or macrocycles. New functionalities may thereby emerge.It is of interest to check for interactions, which give rise to cooperative effects, i. e. properties of the multinuclear complexes, which differ from those of the uncoupled metal centers. Notably, the magnetic, catalytic, and optical properties of such species can be strongly influenced by cooperative interactionsthemselves a manifestation of n-body intermetallic couplings, as determined by quantum chemistry. By changing metal center interaction and coupling, one can aim to tune and thus [a] Dr.

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Terminal Ligand and Packing Effects on Slow Relaxation in an Isostructural Set of [Dy(H₂dapp)X₂]⁺ Single Molecule Magnets**

Cited by 8 publications

References 52 publications

Toward exact predictions of spin-phonon relaxation times: An ab initio implementation of open quantum systems theory

Toward exact predictions of spin-phonon relaxation times: An ab initio implementation of open quantum systems theory

Spin-Phonon Relaxation in Magnetic Molecules: Theory, Predictions and Insights

Cooperative Effects in Heterometallic Complexes

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