Control and Transferability of Magnetic Interactions in Supramolecular Structures: Trimers of {Cr Ni} Antiferromagnetic Rings

Overview

Journal Chemistry

Specialty Chemistry

Date 2023 Sep 22

PMID 37737455

Authors

Selena J Lockyer

Deepak Asthana

George F S Whitehead

Inigo J Vitorica-Yrezabal

Grigore A Timco

Eric J L McInnes

Richard E P Winpenny

Affiliations

Soon will be listed here.

Abstract

A synthetic strategy is demonstrated to prepare two distinct trimers of antiferromagnetically coupled {Cr Ni} rings, substantially varying the magnetic interactions between the spin centres. The interactions were studied using multi-frequency cw EPR: in a trimer linked via non-covalent H-bonding interactions no measurable interaction between rings was seen, while in a trimer linked via iso-nicotinate groups isotropic and anisotropic exchange interactions of +0.42 and -0.8 GHz, respectively, were observed. The latter are the same as those for a simpler hetero-dimer system, showing how the spin-spin interactions can be built in a predictable and modular manner in these systems.

Citing Articles

Control and Transferability of Magnetic Interactions in Supramolecular Structures: Trimers of {Cr Ni} Antiferromagnetic Rings.

Lockyer S, Asthana D, Whitehead G, Vitorica-Yrezabal I, Timco G, McInnes E Chemistry. 2023; 29(69):e202302360.

PMID: 37737455 PMC: 10947047. DOI: 10.1002/chem.202302360.

References

Vignesh K, Langley S, Moubaraki B, Murray K, Rajaraman G . Large Hexadecametallic {Mn(III) -Ln(III) } Wheels: Synthesis, Structural, Magnetic, and Theoretical Characterization. Chemistry. 2015; 21(46):16364-9. DOI: 10.1002/chem.201503424. View

Timco G, Marocchi S, Garlatti E, Barker C, Albring M, Bellini V . Heterodimers of heterometallic rings. Dalton Trans. 2016; 45(42):16610-16615. DOI: 10.1039/c6dt01941b. View

Larsen F, McInnes E, El Mkami H, Overgaard J, Piligkos S, Rajaraman G . Synthesis and characterization of heterometallic {Cr7M} wheels. Angew Chem Int Ed Engl. 2009; 42(1):101-5. DOI: 10.1002/anie.200390034. View

Nakazawa S, Nishida S, Ise T, Yoshino T, Mori N, Rahimi R . A synthetic two-spin quantum bit: g-engineered exchange-coupled biradical designed for controlled-NOT gate operations. Angew Chem Int Ed Engl. 2012; 51(39):9860-4. DOI: 10.1002/anie.201204489. View

de Camargo L, Briganti M, Santana F, Stinghen D, Ribeiro R, Nunes G . Exploring the Organometallic Route to Molecular Spin Qubits: The [CpTi(cot)] Case. Angew Chem Int Ed Engl. 2020; 60(5):2588-2593. DOI: 10.1002/anie.202009634. View

Troiani F, Ghirri A, Affronte M, Carretta S, Santini P, Amoretti G . Molecular engineering of antiferromagnetic rings for quantum computation. Phys Rev Lett. 2005; 94(20):207208. DOI: 10.1103/PhysRevLett.94.207208. View

Kundu K, White J, Moehring S, Yu J, Ziller J, Furche F . A 9.2-GHz clock transition in a Lu(II) molecular spin qubit arising from a 3,467-MHz hyperfine interaction. Nat Chem. 2022; 14(4):392-397. DOI: 10.1038/s41557-022-00894-4. View

Candini A, Lorusso G, Troiani F, Ghirri A, Carretta S, Santini P . Entanglement in supramolecular spin systems of two weakly coupled antiferromagnetic rings (purple-Cr7Ni). Phys Rev Lett. 2010; 104(3):037203. DOI: 10.1103/PhysRevLett.104.037203. View

Whitehead G, Cross B, Carthy L, Milway V, Rath H, Fernandez A . Rings and threads as linkers in metal-organic frameworks and poly-rotaxanes. Chem Commun (Camb). 2013; 49(65):7195-7. DOI: 10.1039/c3cc42300j. View

10.

Faust T, Bellini V, Candini A, Carretta S, Lorusso G, Allan D . Chemical control of spin propagation between heterometallic rings. Chemistry. 2011; 17(50):14020-30. DOI: 10.1002/chem.201101785. View

11.

McInnes E, Timco G, Whitehead G, Winpenny R . Heterometallic Rings: Their Physics and use as Supramolecular Building Blocks. Angew Chem Int Ed Engl. 2015; 54(48):14244-69. DOI: 10.1002/anie.201502730. View

12.

Saalfrank R, Prakash R, Maid H, Hampel F, Heinemann F, Trautwein A . Synthesis and characterization of metal-centered, six-membered, mixed-valent, heterometallic wheels of iron, manganese, and indium. Chemistry. 2006; 12(9):2428-33. DOI: 10.1002/chem.200501497. View

13.

Lee C, Leigh D, Pritchard R, Schultz D, Teat S, Timco G . Hybrid organic-inorganic rotaxanes and molecular shuttles. Nature. 2009; 458(7236):314-8. DOI: 10.1038/nature07847. View

14.

Bader K, Dengler D, Lenz S, Endeward B, Jiang S, Neugebauer P . Room temperature quantum coherence in a potential molecular qubit. Nat Commun. 2014; 5:5304. DOI: 10.1038/ncomms6304. View

15.

Timco G, McInnes E, Pritchard R, Tuna F, Winpenny R . Heterometallic rings made from chromium stick together easily. Angew Chem Int Ed Engl. 2008; 47(50):9681-4. DOI: 10.1002/anie.200803637. View

16.

Timco G, Carretta S, Troiani F, Tuna F, Pritchard R, Muryn C . Engineering the coupling between molecular spin qubits by coordination chemistry. Nat Nanotechnol. 2009; 4(3):173-8. DOI: 10.1038/nnano.2008.404. View

17.

Pedersen K, Ariciu A, McAdams S, Weihe H, Bendix J, Tuna F . Toward Molecular 4f Single-Ion Magnet Qubits. J Am Chem Soc. 2016; 138(18):5801-4. DOI: 10.1021/jacs.6b02702. View

18.

Ariciu A, Woen D, Huh D, Nodaraki L, Kostopoulos A, Goodwin C . Engineering electronic structure to prolong relaxation times in molecular qubits by minimising orbital angular momentum. Nat Commun. 2019; 10(1):3330. PMC: 6659626. DOI: 10.1038/s41467-019-11309-3. View

19.

Lockyer S, Fielding A, Whitehead G, Timco G, Winpenny R, McInnes E . Close Encounters of the Weak Kind: Investigations of Electron-Electron Interactions between Dissimilar Spins in Hybrid Rotaxanes. J Am Chem Soc. 2019; 141(37):14633-14642. PMC: 6814243. DOI: 10.1021/jacs.9b05590. View

20.

Lockyer S, Asthana D, Whitehead G, Vitorica-Yrezabal I, Timco G, McInnes E . Control and Transferability of Magnetic Interactions in Supramolecular Structures: Trimers of {Cr Ni} Antiferromagnetic Rings. Chemistry. 2023; 29(69):e202302360. PMC: 10947047. DOI: 10.1002/chem.202302360. View