Rigidifying Qubit Candidates in a Cu‐Porphyrin Nanohoop: Dipolar Coupling in Spin Pairs and Spin‐Polarized Ground State

Abstract Assembling molecular qubit candidates with precise control over the position and orientation of spin centers is an important contemporary challenge for synthesis. In this work, we show that the rigidity of highly strained macrocycles from the cycloparaphenylene family gives rise to distinct spin‐spin and light‐spin interactions that make such few‐qubit systems a promising testing ground for future quantum technologies. We synthesized conjugated nanohoop Cu[3]CPTA that comprises three Cu(II)porphyrin centers ( S = ½) with a Cu–Cu distance of ca. 18 Å (by single‐crystal X‐ray diffraction). Continuous‐wave (cw) and pulse electron‐paramagnetic resonance (EPR) studies revealed that dipolar coupling in spin pairs is so well defined in this nanohoop that the Cu–Cu distance can be determined accurately via double electron–electron resonance (DEER). By transient cwEPR, we observed a rare case of a light‐induced polarization of a doublet ground state in frozen solution. The fact that ground state polarization was significantly less pronounced in a comparable, but more flexible macrocycle will inspire future efforts to better understand and harness this effect.

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Publication Details

Journal
Angewandte Chemie International Edition
Published
2025-12-09
DOI
https://doi.org/10.1002/anie.202522950
Primary Topic
Magnetism in coordination complexes
Type
article
Field-Weighted Citation Impact
0.00

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article

Rigidifying Qubit Candidates in a Cu‐Porphyrin Nanohoop: Dipolar Coupling in Spin Pairs and Spin‐Polarized Ground State

Inhar Imaz, Linda Zedler, Xavi Ribas, Louis Blechschmidt et al.
Angewandte Chemie International Edition
Magnetism in coordination complexes
article

Rigidifying Qubit Candidates in a Cu‐Porphyrin Nanohoop: Dipolar Coupling in Spin Pairs and Spin‐Polarized Ground State

Inhar Imaz, Linda Zedler, Xavi Ribas, Louis Blechschmidt, Adriana Sacristán‐Martín, Ashley J. Redman, Max von Delius, Xingmao Chang, Fabian Schwer, Daniel Maspoch, Sabine Richert, Benjamin Dietzek‐Ivanšić, Markus P. B. Wiedmaier
article en

Abstract

Abstract Assembling molecular qubit candidates with precise control over the position and orientation of spin centers is an important contemporary challenge for synthesis. In this work, we show that the rigidity of highly strained macrocycles from the cycloparaphenylene family gives rise to distinct spin‐spin and light‐spin interactions that make such few‐qubit systems a promising testing ground for future quantum technologies. We synthesized conjugated nanohoop Cu[3]CPTA that comprises three Cu(II)porphyrin centers ( S = ½) with a Cu–Cu distance of ca. 18 Å (by single‐crystal X‐ray diffraction). Continuous‐wave (cw) and pulse electron‐paramagnetic resonance (EPR) studies revealed that dipolar coupling in spin pairs is so well defined in this nanohoop that the Cu–Cu distance can be determined accurately via double electron–electron resonance (DEER). By transient cwEPR, we observed a rare case of a light‐induced polarization of a doublet ground state in frozen solution. The fact that ground state polarization was significantly less pronounced in a comparable, but more flexible macrocycle will inspire future efforts to better understand and harness this effect.

Angewandte Chemie International EditionVol. 65(4)
Institució Catalana de Recerca i Estudis Avançats (ES), Helmholtz Institute Jena (DE), Universität Ulm (DE), Universitat de Girona (ES), Leibniz Institute of Photonic Technology (DE), Institut Català de Nanociència i Nanotecnologia (ES), Center for Integrated Quantum Science and Technology (DE)
Alexander von Humboldt-Stiftung, Deutsche Forschungsgemeinschaft, Institució Catalana de Recerca i Estudis Avançats, Universität Ulm, Center for Integrated Quantum Science and Technology
Openalex Percentile: Top 71%
Magnetism in coordination complexes
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