Quantum coherent spin–electric control in a molecular nanomagnet at clock transitions

Liu, Junjie; Mrozek, Jakub; Ullah, Aman; Duan, Yan; Baldoví, José J.; Coronado, Eugenio; Gaita‐Ariño, Alejandro; Ardavan, Arzhang

doi:10.1038/s41567-021-01355-4

Cited by 46 publications

(47 citation statements)

References 30 publications

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“…Nanotechnologies building on the development of synthetic DNA 122 may offer the toolkit for these new construction paradigms. Integration of molecular qubits into such devices and electric field control 61,123 of the qubits are key challenges. Atomic spin qubits on surfaces have the advantage that they can be arranged into arbitrary nanostructures with atomic-scale precision 124 .…”

Section: Discussionmentioning

confidence: 99%

“…This motivated the design of magnetic molecules with coherence times of tens or hundreds 59 of microseconds at low temperatures and coherent spin dynamics persisting at room temperature 60 . Light 34 and electric fields 32,61 offer rapid manipulation of functional units and interconnects and may provide controls for implementing conditional classical or quantum information operations 62 .…”

Section: Self-assembled Nanostructuresmentioning

confidence: 99%

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Quantum-coherent nanoscience

et al. 2021

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For the past three decades, nanoscience has widely affected many areas in physics, chemistry, and engineering, and has led to numerous fundamental discoveries as well as applications and products.Concurrently, quantum science and technology has developed into a cross-disciplinary research endeavour connecting these same areas and holds a burgeoning commercial promise. Although quantum physics dictates the behaviour of nanoscale objects, quantum coherence, which is central to quantum information, communication and sensing has not played an explicit role in much of nanoscience. This Review describes fundamental principles and practical applications of quantum coherence in nanoscale systems, a research area we call quantum-coherent nanoscience. We structure this manuscript according to specific degrees of freedom that can be quantum-coherently controlled in a given nanoscale system such as charge, spin, mechanical motion, and photons. We review the current state of the art and focus

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Section: Discussionmentioning

confidence: 99%

Section: Self-assembled Nanostructuresmentioning

confidence: 99%

Quantum-coherent nanoscience

et al. 2021

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“…Atoms [33] and atom-like defects [34] in SiC possess significant electrical tunability of their electronic states, which may be exploited for flip-flop transitions in the presence of hyperfine-coupled nuclei. Molecular systems could permit even more tailored electrical responses, as already observed in recent ensemble experiments [9].…”

Section: D)mentioning

confidence: 67%

“…The longer coherence time of natural atoms and atomlike systems is accompanied by a reduced sensitivity to electric fields, making EDSR more challenging. EDSR was demonstrated in ensembles of color centers in silicon carbide [8] and molecular magnets [9] for electron spins, and ensembles of donors in silicon for nuclear spins [10]. At the single-atom level, coherent electrical control was demonstrated in scanning tunneling microscope experiments, [11], single-atom molecular magnets [12] and high-spin donor nuclei [13].…”

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confidence: 99%

An electrically-driven single-atom `flip-flop' qubit

Savytskyy¹,

Botzem²,

Fuentes³

et al. 2022

Preprint

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The spins of atoms and atom-like systems are among the most coherent objects in which to store quantum information. However, the need to address them using oscillating magnetic fields hinders their integration with quantum electronic devices. Here we circumvent this hurdle by operating a single-atom 'flip-flop' qubit in silicon, where quantum information is encoded in the electronnuclear states of a phosphorus donor. The qubit is controlled using local electric fields at microwave frequencies, produced within a metal-oxide-semiconductor device. The electrical drive is mediated by the modulation of the electron-nuclear hyperfine coupling, a method that can be extended to many other atomic and molecular systems. These results pave the way to the construction of solidstate quantum processors where dense arrays of atoms can be controlled using only local electric fields.

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“…[1][2][3][6][7][8][9][10] Inspired by this great success, organic radicals and transition-metal-based (TM) and lanthanide-based (Ln) magnetic molecules have been tailored to have desirable properties for quantum information science applications by utilizing the versatility of chemical environment. [15][16][17][18][19][20][21][22][23][24] Either molecular electronic spin states or electronic-nuclear spin states can be considered as quantum bits (qubits) or quantum d-levels (qudits) which may be initialized, read-out, or controlled by an external magnetic field and/or electric field, or optical means. For organic donor-acceptor-radical molecules, the electronic spin states were shown to be entangled and teleported with high fidelity by using microwave pulses and photoexcitation.…”

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confidence: 99%

Computational Insights into Electronic Excitations, Spin-Orbit Coupling Effects, and Spin Decoherence in Cr(IV)-based Molecular Qubits

Janicka¹,

Wysocki²,

Park³

2022

Preprint

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The great success of point defects and dopants in semiconductors for quantum information processing has invigorated a search for molecules with analogous properties.Flexibility and tunability of desired properties in a large chemical space have great advantages over solid-state systems. The properties analogous to point defects were demonstrated in Cr(IV)-based molecular family, Cr(IV)(aryl) 4 , where the electronic spin states were optically initialized, read out, and controlled. Despite this kick-start, there is still a large room for enhancing properties crucial for molecular qubits. Here we provide computational insights into key properties of the Cr(IV)-based molecules aimed at assisting chemical design of efficient molecular qubits. Using the multireference ab-initio methods, we investigate the electronic states of Cr(IV)(aryl) 4 molecules with slightly different ligands, showing that the zero-phonon line energies agree with the experiment, and that the excited spin-triplet and spin-singlet states are highly sensitive to small chemical perturbations. By adding spin-orbit interaction, we find that the

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Quantum coherent spin–electric control in a molecular nanomagnet at clock transitions

Cited by 46 publications

References 30 publications

Quantum-coherent nanoscience

Quantum-coherent nanoscience

An electrically-driven single-atom `flip-flop' qubit

Computational Insights into Electronic Excitations, Spin-Orbit Coupling Effects, and Spin Decoherence in Cr(IV)-based Molecular Qubits

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