Accurate crystal field Hamiltonians of single-ion magnets at mean-field cost
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arXiv
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| Autori principali: | , , , , , , |
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| Natura: | Preprint |
| Pubblicazione: |
2025
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| _version_ | 1866916966377193472 |
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| author | Peng, Linqing Liu, Shuanglong Zhang, Xing Chen, Xiao Li, Chenghan Cheng, Hai-Ping Chan, Garnet Kin-Lic |
| author_facet | Peng, Linqing Liu, Shuanglong Zhang, Xing Chen, Xiao Li, Chenghan Cheng, Hai-Ping Chan, Garnet Kin-Lic |
| contents | The effective crystal field Hamiltonian provides the key description of the electronic properties of single-ion magnets, but obtaining its parameters from ab initio computation is challenging. We introduce a simple approach to derive the effective crystal field Hamiltonian through density functional calculations of randomly rotated mean-field states within the low-energy manifold. In benchmarks on five lanthanide-based complexes, we find that we compute with mean-field cost an effective crystal field Hamiltonian that matches the state-of-the-art from much more expensive multi-configurational quantum chemistry methods. In addition, we are able to reproduce the experimental low-energy spectrum and magnetic properties with an accuracy exceeding prior attempts. Due to its low cost, our approach provides a crucial ingredient in the computational design of single-ion magnets with tailored physical properties and low-energy spectra. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2505_16905 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Accurate crystal field Hamiltonians of single-ion magnets at mean-field cost Peng, Linqing Liu, Shuanglong Zhang, Xing Chen, Xiao Li, Chenghan Cheng, Hai-Ping Chan, Garnet Kin-Lic Chemical Physics Materials Science Strongly Correlated Electrons Computational Physics Quantum Physics The effective crystal field Hamiltonian provides the key description of the electronic properties of single-ion magnets, but obtaining its parameters from ab initio computation is challenging. We introduce a simple approach to derive the effective crystal field Hamiltonian through density functional calculations of randomly rotated mean-field states within the low-energy manifold. In benchmarks on five lanthanide-based complexes, we find that we compute with mean-field cost an effective crystal field Hamiltonian that matches the state-of-the-art from much more expensive multi-configurational quantum chemistry methods. In addition, we are able to reproduce the experimental low-energy spectrum and magnetic properties with an accuracy exceeding prior attempts. Due to its low cost, our approach provides a crucial ingredient in the computational design of single-ion magnets with tailored physical properties and low-energy spectra. |
| title | Accurate crystal field Hamiltonians of single-ion magnets at mean-field cost |
| topic | Chemical Physics Materials Science Strongly Correlated Electrons Computational Physics Quantum Physics |
| url | https://arxiv.org/abs/2505.16905 |