Exploiting chemistry and molecular systems for quantum information science

Wasielewski, Michael R.; Forbes, Malcolm D. E.; Frank, Natia L.; Kowalski, Karol; Scholes, Gregory D.; Yuen-Zhou, Joel; Baldo, Marc A.; Freedman, Danna E.; Goldsmith, Randall H.; Goodson, Theodore; Kirk, Martin L.; McCusker, James K.; Ogilvie, Jennifer P.; Shultz, David A.; Stoll, Stefan; Whaley, K. Birgitta

doi:10.1038/s41570-020-0200-5

Cited by 291 publications

(296 citation statements)

References 206 publications

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“… 24 In addition, a great advantage is represented by the availability of a set of addressable and accessible electronic and nuclear energy levels that can be probed by electromagnetic pulses. 25 , 26 …”

Section: Introductionmentioning

confidence: 99%

Probing Vibrational Symmetry Effects and Nuclear Spin Economy Principles in Molecular Spin Qubits

et al. 2020

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The selection of molecular spin qubits with a long coherence time, T m , is a central task for implementing molecule-based quantum technologies. Even if a sufficiently long T m can be achieved through an efficient synthetic strategy and ad hoc experimental measurement procedures, many factors contributing to the loss of coherence still need to be thoroughly investigated and understood. Vibrational properties and nuclear spins of hydrogens are two of them. The former plays a paramount role, but a detailed theoretical investigation aimed at studying their effects on the spin dynamics of molecular complexes such as the benchmark phthalocyanine (Pc) is still missing, whereas the effect of the latter deserves to be examined in detail for such a class of compounds. In this work, we adopted a combined theoretical and experimental approach to investigate the relaxation properties of classical [Cu(Pc)] and a Cu II complex based on the ligand tetrakis(thiadiazole)porphyrazine (H 2 TTDPz), characterized by a hydrogen-free molecular structure. Systematic calculations of molecular vibrations exemplify the effect of normal modes on the spin–lattice relaxation process, unveiling a different contribution to T 1 depending on the symmetry of normal modes. Moreover, we observed that an appreciable T m enhancement could be achieved by removing hydrogens from the ligand.

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Section: Introductionmentioning

confidence: 99%

Probing Vibrational Symmetry Effects and Nuclear Spin Economy Principles in Molecular Spin Qubits

et al. 2020

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“…[94] Elucidating the interplay of spin states, heavy atom effects and inherentr eaction (rather than emission quenching) efficienciess hould therefore be very important for the photochemistry of the future. [95][96][97][98][99] Novel molecular dyads with av isible-light-harvesting metal complexa nd ar edoxactive heavy-atom free chromophore provide ap romising alternative to conventionalm etal complexes, as has emerged from this work. triplets by Asc 2À as af unction of the donor( Asc 2À )concentration.P arameters used for the kinetic simulations( values for the dyad shown in brackets): unquenched triplet lifetime,0 .6 ms( 150 ms);quenching rate constant, 6.4 10 9 m À1 s À1 [29,30] (3.6 10 8 m À1 s À1 ); inherent cage escape yield,0.43 (0.58).…”

Section: Discussionmentioning

confidence: 94%

Controlling Spin‐Correlated Radical Pairs with Donor–Acceptor Dyads: A New Concept to Generate Reduced Metal Complexes for More Efficient Photocatalysis

Neumann

Wenger

Kerzig

2021

Chemistry A European J

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One-electron reduced metal complexes derived from photoactive ruthenium or iridium complexes are important intermediates for substrate activation steps in photoredox catalysis and for the photocatalytic generation of solar fuels. However,o wing to the heavy atom effect, direct photochemical pathways to these key intermediates suffer from intrinsic efficiency problems resulting from rapid geminate recombination of radical pairs within the so-called solvent cage. In this study,w ep repared and investigated molecular dyads capable of producing reduced metal complexes via an indirect pathway relyingo nas equence of energy and electron transfer processes between aR uc omplex and ac ovalently connected anthracene moiety.O ur test reaction to establish the proof-of-concept is the photochem-ical reduction of ruthenium(tris)bipyridine by the ascorbate dianion as sacrificial donor in aqueous solution. The photochemicalk ey step in the Ru-anthracene dyads is the reduction of ap urely organic (anthracene) triplet exciteds tate by the ascorbate dianion, yielding as pin-correlated radical pair whose (unproductive) recombination is strongly spin-forbidden. By carrying out detailed laser flash photolysis investigations, we provide clear evidence for the indirect reduced metal complex generation mechanism and show that this pathway can outperform the conventionald irect metal complex photoreduction. The furthero ptimization of our approach involving relativelys imple molecular dyads might result in novel photocatalysts that convert substrates with unprecedented quantum yields.

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“…The controlled entanglement through a very weak (but non-negligible) switchable magnetic interaction between a pair of highly coherent spin carriers acting as individual quantum bits (qubits) is crucial for the physical implementation of quantum information processing (QIP) through quantum gates. In contrast to current computational methodology based on classical bits, QIP may offer a new paradigm for performing quantum logic operations that exploits the quantum coherence properties of electron spin-based qubits in forming part of a quantum gate in future quantum computers [29][30][31][32][33][34][35][36][37][38][39][40][41][42][43][44][45].…”

Section: Conclusion and Outlook: Metallosupramolecular Chemistry Actmentioning

confidence: 99%

“…The metallosupramolecular chemistry term was coined by Constable in 1994 to describe an emerging research area in the field of supramolecular chemistry [1,2], where the advantage of coordination chemistry is taken to control the metal-directed assembly of supramolecular systems [3][4][5][6][7][8][9][10]. Metallosupramolecular chemistry provides convenient tools for the current evolution from molecular magnetism [11][12][13][14][15][16][17][18] toward single-molecule spintronics [19][20][21][22][23][24][25][26][27][28] and quantum computing [29][30][31][32][33][34][35][36][37][38][39][40][41][42][43][44][45]. The internal (steric and electronic modulation) and external control (chemo-, electro-and photostimulation) of the magnetic coupling through ligand ...…”

Section: Introduction and Background: Molecular Magnetism Meets Metalmentioning

confidence: 99%

When Molecular Magnetism Meets Supramolecular Chemistry: Multifunctional and Multiresponsive Dicopper(II) Metallacyclophanes as Proof-of-Concept for Single-Molecule Spintronics and Quantum Computing Technologies?

et al. 2020

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Molecular magnetism has made a long journey, from the fundamental studies on through-ligand electron exchange magnetic interactions in dinuclear metal complexes with extended organic bridges to the more recent exploration of their electron spin transport and quantum coherence properties. Such a field has witnessed a renaissance of dinuclear metallacyclic systems as new experimental and theoretical models for single-molecule spintronics and quantum computing, due to the intercrossing between molecular magnetism and metallosupramolecular chemistry. The present review reports a state-of-the-art overview as well as future perspectives on the use of oxamato-based dicopper(II) metallacyclophanes as promising candidates to make multifunctional and multiresponsive, single-molecule magnetic (nano)devices for the physical implementation of quantum information processing (QIP). They incorporate molecular magnetic couplers, transformers, and wires, controlling and facilitating the spin communication, as well as molecular magnetic rectifiers, transistors, and switches, exhibiting a bistable (ON/OFF) spin behavior under external stimuli (chemical, electronic, or photonic). Special focus is placed on the extensive research work done by Professor Francesc Lloret, an outstanding chemist, excellent teacher, best friend, and colleague, in recognition of his invaluable contributions to molecular magnetism on the occasion of his 65th birthday.

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Exploiting chemistry and molecular systems for quantum information science

Cited by 291 publications

References 206 publications

Probing Vibrational Symmetry Effects and Nuclear Spin Economy Principles in Molecular Spin Qubits

Probing Vibrational Symmetry Effects and Nuclear Spin Economy Principles in Molecular Spin Qubits

Controlling Spin‐Correlated Radical Pairs with Donor–Acceptor Dyads: A New Concept to Generate Reduced Metal Complexes for More Efficient Photocatalysis

When Molecular Magnetism Meets Supramolecular Chemistry: Multifunctional and Multiresponsive Dicopper(II) Metallacyclophanes as Proof-of-Concept for Single-Molecule Spintronics and Quantum Computing Technologies?

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