A multireference picture of electronic excited states in vanadyl and copper tetraphenyl porphyrin molecular qubits
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arXiv
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| Format: | Preprint |
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2025
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| _version_ | 1866918004331118592 |
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| author | Sarkar, Arup Lunghi, Alessandro |
| author_facet | Sarkar, Arup Lunghi, Alessandro |
| contents | The nature of electronic excited states has a deep impact on the dynamics of molecular spins, but remains poorly understood and characterized. Here we carry out a thorough multiconfigurational investigation for two prototypical molecular qubits based on vanadyl and copper tetra-phenyl porphyrins. State-average CASSCF and NEVPT2 calculations have been employed with four different active spaces of growing complexity to account for the d-d, second d-shell, ligand-to-metal charge transfer states and $π-π^*$ excited states, revealing an in-depth picture of low-lying excited states in agreement with experimental observations. The largest active spaces attempted, (13,14) for the vanadyl and (17,12) for the copper compounds, reveal that the lowest-lying excited states originate from $π-π^*$ quartet excitations. These findings shed light on the nature of the excited states of molecular qubits, taking an important step toward elucidating their role in molecular spin dynamics. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2504_20778 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | A multireference picture of electronic excited states in vanadyl and copper tetraphenyl porphyrin molecular qubits Sarkar, Arup Lunghi, Alessandro Quantum Physics Materials Science The nature of electronic excited states has a deep impact on the dynamics of molecular spins, but remains poorly understood and characterized. Here we carry out a thorough multiconfigurational investigation for two prototypical molecular qubits based on vanadyl and copper tetra-phenyl porphyrins. State-average CASSCF and NEVPT2 calculations have been employed with four different active spaces of growing complexity to account for the d-d, second d-shell, ligand-to-metal charge transfer states and $π-π^*$ excited states, revealing an in-depth picture of low-lying excited states in agreement with experimental observations. The largest active spaces attempted, (13,14) for the vanadyl and (17,12) for the copper compounds, reveal that the lowest-lying excited states originate from $π-π^*$ quartet excitations. These findings shed light on the nature of the excited states of molecular qubits, taking an important step toward elucidating their role in molecular spin dynamics. |
| title | A multireference picture of electronic excited states in vanadyl and copper tetraphenyl porphyrin molecular qubits |
| topic | Quantum Physics Materials Science |
| url | https://arxiv.org/abs/2504.20778 |