A molecular perspective on quantum information

Scholes, Gregory D.

doi:10.1098/rspa.2023.0599

Cited by 12 publications

(11 citation statements)

References 84 publications

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“…The three spin sublevels are completely degenerate at the nonrelativistic level, and the degeneracy is, albeit often very slightly, lifted by the relativistic effect, i.e., spin–spin coupling (SSC) and spin–orbit coupling (SOC). This is called zero-field splitting (ZFS) and is not only a factor in determining the spectrum of magnetic spectroscopy for paramagnetic species but also an important character for utilizing molecules in quantum information science. − In fact, photoinduced spin polarization to one of the three spin sublevels is efficiently realized for many planar aromatic hydrocarbons and nitrogen-vacancy centers (NV-center) of synthetic diamond . This non-Boltzmann distributed polarization can be exploited in dynamic nuclear polarization (DNP) − and MASER − operating under mild conditions.…”

Section: Introductionmentioning

confidence: 99%

Zero-Field Splitting Tensor of the Triplet Excited States of Aromatic Molecules: A Valence Full-π Complete Active Space Self-Consistent Field Study

Miyokawa,

Kurashige

2024

J. Phys. Chem. A

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A method to predict the D tensor in the molecular frame with multiconfigurational wave functions in large active space was proposed, and the spin properties of the lowest triplets of aromatic molecules were examined with full-π active space; such calculations were challenging because the size of active space grows exponentially with the number of π electrons. In this method, the exponential growth of complexity is resolved by the density matrix renormalization group (DMRG) algorithm. From the D tensor, we can directly determine the direction of the magnetic axes and the ZFS parameters, D- and E-values, of the phenomenological spin Hamiltonian with their signs, which are not usually obtained in ESR experiments. The method using the DMRG-CASSCF wave function can give correct results even when the sign of D- and E-values is sensitive to the accuracy of the prediction of the D tensor and existing methods fail to predict the correct magnetic axes.

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Section: Introductionmentioning

confidence: 99%

Zero-Field Splitting Tensor of the Triplet Excited States of Aromatic Molecules: A Valence Full-π Complete Active Space Self-Consistent Field Study

Miyokawa,

Kurashige

2024

J. Phys. Chem. A

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“…In other papers, we provide a more detailed tutorial review. 106 Quantum systems considered model qubits are typically two-level systems. The classical analogy is a switch that can take values of 0 or 1, just like the binary basis for digital communication and computation, which are based on two-state systems.…”

Section: Introductionmentioning

confidence: 99%

“…Here we include a very brief overview of some key points about quantum information science. In other papers, we provide a more detailed tutorial review . Quantum systems considered model qubits are typically two-level systems.…”

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confidence: 99%

Molecular and Supramolecular Materials: From Light-Harvesting to Quantum Information Science and Technology

Zhang,

Oberg,

et al. 2024

J. Phys. Chem. Lett.

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Figure 2. Molecular quantum materials and technologies. (a) Synthetic electron spin systems, M1: (2,2,6,6-tetramethylpiperidin-N-oxyl-4-yl) 3,5dimethylbenzoate-4-yl tetrephthalate diradicals; 32 M2: magnesium phthalocyanine with three nitroxyl radicals; 32 M3: Hexamethoxyphenalenyl radical; 32 M4: side-functionalized graphene nanoribbon radicals; 123 M5: topological stabilized magnetic centers. 123 (b) Schematic representation of the grafting procedure leading to immobilized BTR radicals inside the pores of SBA-15 host phase. 34 Adapted with permission from ref 34. Copyright 2021 Wiley-VCH. (c) Molecular structure of two GdIII trapped in a C79N fullerene. 95 Adapted with permission from ref 95. Copyright 2017 American Chemical Society. (d) TM radicals doped with their corresponding diamagnetic hydrogenated products to increase Tm. 132 (e) Schematic presentation of the impact of polymer rigidity on the luminescence and electron spin dynamics of the radical polymers. 35

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“…The quantum mechanical properties of nuclear and electron spins, namely, superposition and entanglement, result in their being ideal candidates for quantum bits (qubits) used in quantum information science (QIS) applications. − However, the small energy differences between their quantum states mean that fundamental structure–function studies related to the generation of spin polarization and further preparation of the spin system are important. Stable radical-elaborated chromophores are ideal in this context, and they have been used as qubit candidates in novel studies of coherence, logic gate operations, qubit candidates, spin teleportation, and photoinduced dynamic nuclear (hyper)polarization. ,,− …”

Section: Introductionmentioning

confidence: 99%

Photoinduced Magnetic Exchange-Jump Promotes Ground State Biradical Electron Spin Polarization

Kirk,

Shultz,

Marri

et al. 2024

J. Am. Chem. Soc.

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Photoinduced electron spin polarization (ESP) is reported in the electronic ground states of three Pt(II) complexes comprised of two S = 1/2 nitronyl nitroxide (NN) radicals attached through different length paraphenylethynyl bridges to the 3,6 positions of a catecholate (CAT, donor) and 4,4′-di-tert-butyl-2,2′-bipyridine (bpy, acceptor). Complexes 1−3 have from 17 to 41 bonds separating NN radicals and display cw-EPR spectra consistent withrespectively, where J NN-NN is the magnetic exchange coupling between NN radicals in the electronic ground state, and a N is the isotropic 14 N hyperfine coupling constant. Light-induced transient EPR spectra characterized as enhanced ground-state absorption were observed for all three complexes using 532 nm pulsed laser excitation into the ligand-to-ligand charge transfer (LL'CT) band of the (CAT)Pt(bpy) chromophore. The magnitude of the observed ESP increases in the order 1 < 2 < 3 and is inversely correlated with the magnitude of ground-state J NN-NN . In addition to the experimental observation of net absorptive polarization in 1−3, light excitation also produces multiplet polarization in 2. Since the weak dipolar coupling leads to a strong spectral overlap of the absorptive and emissive components, the multiplet polarization is not observed in 1 and 3 and is very weak in 2. The ability to spin-polarize multiple radical spins with a single photon is anticipated to advance new photoinduced multi qubit/qudit ESP protocols for quantum information science applications.

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A molecular perspective on quantum information

Cited by 12 publications

References 84 publications

Zero-Field Splitting Tensor of the Triplet Excited States of Aromatic Molecules: A Valence Full-π Complete Active Space Self-Consistent Field Study

Zero-Field Splitting Tensor of the Triplet Excited States of Aromatic Molecules: A Valence Full-π Complete Active Space Self-Consistent Field Study

Molecular and Supramolecular Materials: From Light-Harvesting to Quantum Information Science and Technology

Photoinduced Magnetic Exchange-Jump Promotes Ground State Biradical Electron Spin Polarization

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