Room-temperature optical spin polarization of an electron spin qudit in a vanadyl -- free base porphyrin dimer

• URL: http://arxiv.org/abs/2408.02104v1
• Date: Sun, 4 Aug 2024 18:08:20 GMT
• Title: Room-temperature optical spin polarization of an electron spin qudit in a vanadyl -- free base porphyrin dimer
• Authors: Alberto Privitera, Alessandro Chiesa, Fabio Santanni, Angelo Carella, Davide Ranieri, Andrea Caneschi, Matthew D. Krzyaniak, Ryan M. Young, Michael R. Wasielewski, Stefano Carretta, Roberta Sessoli,
• Abstract summary: Photoexcited organic chromophores appended to molecular qubits can serve as a source of spin initialization or multi-level qudit generation for quantum information applications. 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. Exploiting 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.
• Score: 35.34500698545813
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: 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.

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