| Autor: |
Privitera, Alberto, Chiesa, Alessandro, Santanni, Fabio, Carella, Angelo, Ranieri, Davide, Caneschi, Andrea, Krzyaniak, Matthew D., Young, Ryan M., Wasielewski, Michael R., Carretta, Stefano, Sessoli, Roberta |
| Rok vydání: |
2024 |
| Předmět: |
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| Druh dokumentu: |
Working Paper |
| Popis: |
Photoexcited organic chromophores appended to molecular qubits can serve as a source of spin initialization or multi-level qudit generation for quantum information applications. So far, this approach has been primarily investigated in chromophore/stable radical systems. Here, we extend this concept to a meso-meso linked oxovanadium(IV) porphyrin - free base porphyrin dimer. Femtosecond transient absorption experiments reveal that photoexcitation of the free base porphyrin leads to picosecond triplet state formation via enhanced intersystem crossing. Time-resolved electron paramagnetic resonance (TREPR) experiments carried out at both 85 K and room temperature reveal the formation of a long-lived spin-polarized quartet state through triplet-doublet spin mixing. Notably, a distinct hyperfine structure arising from the interaction between the electron spin quartet state and the vanadyl nucleus (51V, I=7/2) is evident, with the quartet state exhibiting long-lived spin polarization even at room temperature. Theoretical simulations of the TREPR spectra confirm the photogenerated quartet state and provide insights into the non-Boltzmann spin populations. Exploit-ing this phenomenon affords the possibility of using photoinduced triplet states in porphyrins for quantum information as a resource to polarize and magnetically couple molecular electronic or nuclear spin qubits and qudits. |
| Databáze: |
arXiv |
| Externí odkaz: |
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