Spin decontamination for magnetic dipolar coupling calculations: Application to high-spin molecules and solid-state spin qubits
An accurate description of the two-electron density, crucial for magnetic coupling in spin systems, provides in general a major challenge for density functional theory calculations. It affects, e.g., the calculated zero-field splitting (ZFS) energies of spin qubits in semiconductors that frequently...
| Main Authors: | , , |
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| Format: | Article |
| Language: | English |
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American Physical Society
2020-04-01
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| Series: | Physical Review Research |
| Online Access: | http://doi.org/10.1103/PhysRevResearch.2.022024 |
| _version_ | 1827286159397486592 |
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| author | Timur Biktagirov Wolf Gero Schmidt Uwe Gerstmann |
| author_facet | Timur Biktagirov Wolf Gero Schmidt Uwe Gerstmann |
| author_sort | Timur Biktagirov |
| collection | DOAJ |
| description | An accurate description of the two-electron density, crucial for magnetic coupling in spin systems, provides in general a major challenge for density functional theory calculations. It affects, e.g., the calculated zero-field splitting (ZFS) energies of spin qubits in semiconductors that frequently deviate significantly from experiment. In the present work, (i) we propose an efficient and robust strategy to correct for spin contamination in both extended periodic and finite-size systems, (ii) verify its accuracy using model high-spin molecules, and finally, (iii) apply the methodology to calculate accurate ZFS of spin qubits (NV^{−} centers, divacancies) in diamond and silicon carbide. The approach is shown to reduce the dependence on the used exchange-correlation functional to a minimum. |
| first_indexed | 2024-04-24T10:26:45Z |
| format | Article |
| id | doaj.art-2479b7d348cd425bb991068db4e98d24 |
| institution | Directory Open Access Journal |
| issn | 2643-1564 |
| language | English |
| last_indexed | 2024-04-24T10:26:45Z |
| publishDate | 2020-04-01 |
| publisher | American Physical Society |
| record_format | Article |
| series | Physical Review Research |
| spelling | doaj.art-2479b7d348cd425bb991068db4e98d242024-04-12T16:53:18ZengAmerican Physical SocietyPhysical Review Research2643-15642020-04-012202202410.1103/PhysRevResearch.2.022024Spin decontamination for magnetic dipolar coupling calculations: Application to high-spin molecules and solid-state spin qubitsTimur BiktagirovWolf Gero SchmidtUwe GerstmannAn accurate description of the two-electron density, crucial for magnetic coupling in spin systems, provides in general a major challenge for density functional theory calculations. It affects, e.g., the calculated zero-field splitting (ZFS) energies of spin qubits in semiconductors that frequently deviate significantly from experiment. In the present work, (i) we propose an efficient and robust strategy to correct for spin contamination in both extended periodic and finite-size systems, (ii) verify its accuracy using model high-spin molecules, and finally, (iii) apply the methodology to calculate accurate ZFS of spin qubits (NV^{−} centers, divacancies) in diamond and silicon carbide. The approach is shown to reduce the dependence on the used exchange-correlation functional to a minimum.http://doi.org/10.1103/PhysRevResearch.2.022024 |
| spellingShingle | Timur Biktagirov Wolf Gero Schmidt Uwe Gerstmann Spin decontamination for magnetic dipolar coupling calculations: Application to high-spin molecules and solid-state spin qubits Physical Review Research |
| title | Spin decontamination for magnetic dipolar coupling calculations: Application to high-spin molecules and solid-state spin qubits |
| title_full | Spin decontamination for magnetic dipolar coupling calculations: Application to high-spin molecules and solid-state spin qubits |
| title_fullStr | Spin decontamination for magnetic dipolar coupling calculations: Application to high-spin molecules and solid-state spin qubits |
| title_full_unstemmed | Spin decontamination for magnetic dipolar coupling calculations: Application to high-spin molecules and solid-state spin qubits |
| title_short | Spin decontamination for magnetic dipolar coupling calculations: Application to high-spin molecules and solid-state spin qubits |
| title_sort | spin decontamination for magnetic dipolar coupling calculations application to high spin molecules and solid state spin qubits |
| url | http://doi.org/10.1103/PhysRevResearch.2.022024 |
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