The spin-phonon relaxation mechanism of single-molecule magnets in the presence of strong exchange coupling
Fuente:
arXiv
Saved in:
| Main Authors: | , , , , , , , |
|---|---|
| Format: | Preprint |
| Published: |
2024
|
| Subjects: | |
| Online Access: | |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1866929616962191360 |
|---|---|
| author | Mondal, Sourav Netz, Julia Hunger, David Suhr, Simon Sarkar, Biprajit van Slageren, Joris Köhn, Andreas Lunghi, Alessandro |
| author_facet | Mondal, Sourav Netz, Julia Hunger, David Suhr, Simon Sarkar, Biprajit van Slageren, Joris Köhn, Andreas Lunghi, Alessandro |
| contents | Magnetic relaxation in coordination compounds is largely dominated by the interaction of the spin with phonons. Large zero-field splitting and exchange coupling values have been empirically found to strongly suppress spin relaxation and have been used as the main guideline for designing new molecular compounds. Although a comprehensive understanding of spin-phonon relaxation has been achieved for mononuclear complexes, only a qualitative picture is available for polynuclear compounds. Here we fill this critical knowledge gap by providing a full first-principle description of spin-phonon relaxation in an air-stable Co(II) dimer with both large single-ion anisotropy and exchange coupling. Simulations reproduce the experimental relaxation data with excellent accuracy and provide a microscopic understanding of Orbach and Raman relaxation pathways and their dependency on exchange coupling, zero-field splitting, and molecular vibrations. Theory and numerical simulations show that increasing cluster nuclearity to just four cobalt units would lead to a complete suppression of Raman relaxation. These results hold a general validity for single-molecule magnets, providing a deeper understanding of their relaxation and revised strategies for their improvement. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2412_04362 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | The spin-phonon relaxation mechanism of single-molecule magnets in the presence of strong exchange coupling Mondal, Sourav Netz, Julia Hunger, David Suhr, Simon Sarkar, Biprajit van Slageren, Joris Köhn, Andreas Lunghi, Alessandro Materials Science Magnetic relaxation in coordination compounds is largely dominated by the interaction of the spin with phonons. Large zero-field splitting and exchange coupling values have been empirically found to strongly suppress spin relaxation and have been used as the main guideline for designing new molecular compounds. Although a comprehensive understanding of spin-phonon relaxation has been achieved for mononuclear complexes, only a qualitative picture is available for polynuclear compounds. Here we fill this critical knowledge gap by providing a full first-principle description of spin-phonon relaxation in an air-stable Co(II) dimer with both large single-ion anisotropy and exchange coupling. Simulations reproduce the experimental relaxation data with excellent accuracy and provide a microscopic understanding of Orbach and Raman relaxation pathways and their dependency on exchange coupling, zero-field splitting, and molecular vibrations. Theory and numerical simulations show that increasing cluster nuclearity to just four cobalt units would lead to a complete suppression of Raman relaxation. These results hold a general validity for single-molecule magnets, providing a deeper understanding of their relaxation and revised strategies for their improvement. |
| title | The spin-phonon relaxation mechanism of single-molecule magnets in the presence of strong exchange coupling |
| topic | Materials Science |
| url | https://arxiv.org/abs/2412.04362 |