Chirality‐Induced Spin Selectivity: An Enabling Technology for Quantum Applications

Advanced Materials, Год журнала: 2023, Номер 35(28)

Опубликована: Май 12, 2023

Molecular spins are promising building blocks of future quantum technologies thanks to the unparalleled flexibility provided by chemistry, which allows design complex structures targeted for specific applications. However, their weak interaction with external stimuli makes it difficult access state at single-molecule level, a fundamental tool use, example, in computing and sensing. Here, an innovative solution exploiting interplay between chirality magnetism using chirality-induced spin selectivity effect on electron transfer processes is foreseen. It envisioned use spin-to-charge conversion mechanism that can be realized connecting molecular qubit dyad where donor acceptor linked chiral bridge. By numerical simulations based realistic parameters, shown could enable initialization, manipulation, single-spin readout qubits qudits even relatively high temperatures.

Язык: Английский

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Chiral lanthanide hexaazamacrocycles for circularly polarized luminescence, high relaxivity and magnetic resonance imaging

Inorganic Chemistry Frontiers, Год журнала: 2024, Номер 11(7), С. 2039 - 2048

Опубликована: Янв. 1, 2024

Mononuclear chiral lanthanide hexaazamacrocycles afford brilliant luminescence, strong CPL, high relaxivity and efficient MRI.

Язык: Английский

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Metalloporphyrins as Building Blocks for Quantum Information Science

Advanced Optical Materials, Год журнала: 2024, Номер 12(18)

Опубликована: Май 17, 2024

Abstract The intrinsic quantum nature of molecules opens exciting opportunities for developing the field information science. In this context, porphyrins stand out as ideal building blocks technologies thanks to their unique optical and electrical properties well capacity accommodate metal atoms ions. This review bridges chemistry physics porphyrins, providing an overview recent advances in porphyrin‐based molecular qubits. Starting from qubits, explores potential porphyrin units combine, leading formation logic gates hierarchical higher‐dimensional structures. Next, exploitation porphyrins' photophysical realizing long‐lived high spin states is examined. These are promising photogeneration multi‐level systems initialization control With a critical eye on current state‐of‐the‐art, elucidates future perspectives advancing technologies.

Язык: Английский

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Coherent Spin Manipulation in Mononuclear Gadolinium-Substituted Polyoxometalate–Organic Hybrids

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер unknown, С. 3072 - 3077

Опубликована: Март 18, 2025

While most research on molecule-based electron spin qubits has focused S = 1/2 ions for single-qubit gates, the need qubit interactions in quantum operations driven interest higher-spin molecules and multilevel states. Herein, we study dynamics of two mononuclear gadolinium-substituted polyoxometalate-organic hybrids with general formula K5[Gd(α-XW11O39)(H2L)]·14H2O (X Si, Ge; H2L N,N'-dimethyl-N,N'-bis(2-hydroxy-3-formyl-5-bromobenzyl)ethylenediamine), 1Si-Gd 1Ge-Gd. Pulsed EPR measurements reveal spin-lattice relaxation (T1) coherence (Tm) times up to 2315 2.6 μs at 3 K, respectively, diamagnetically diluted samples, as well Rabi oscillations 20 K. The obtained results make 1Ge-Gd few Gd-based complexes displaying such behavior, highlighting challenge coherently manipulating states Gd. Moreover, their hybrid organic-inorganic nature endows them chemical robustness solution stability, essential prerequisites surface immobilization future integration practical devices.

Язык: Английский

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Phosphonate Lanthanide Carbonate Cages: Remarkably Aggregated Lanthanide-Oxo Cores with Removable Cation Templates

Crystal Growth & Design, Год журнала: 2025, Номер unknown

Опубликована: Фев. 24, 2025

Язык: Английский

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Spin Qubit in a 2D Gd^IIINa^I‐Based Oxamato Supramolecular Coordination Framework

Chemistry - A European Journal, Год журнала: 2023, Номер 29(66)

Опубликована: Сен. 4, 2023

Qubits are the basic unit of quantum information and computation. To realize computing processing, decoherence times qubits must be long enough. Among studies molecule-based electron spin qubits, most work focused on ions with S=1/2, where only single-bit gates can constructed. However, operations require to interact each other, so people gradually carry out relevant research in or systems S>1/2 multilevel states. In this work, a two-dimensional (2D) oxygen-coordinated GdIII NaI -based oxamato supramolecular coordination framework, Na[Gd(4-HOpa)4 (H2 O)] ⋅ 2H2 O (1, 4-HOpa=N-4-hydroxyphenyloxamate), was selected as possible carrier qubit. The field-induced slow magnetic relaxation shows system has phonon bottleneck (PB) effect at low temperatures very weak anisotropy. pulse paramagnetic resonance show spin-lattice spin-spin T1 =1.66 ms 4 K Tm =4.25 μs 8 for its diamagnetically diluted sample (1Gd0.12 %). It suggested that relatively time is mainly ascribed near isotropic PB from trapped pure sample, while dilution further improves qubit performance.

Язык: Английский

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Enhanced coherence by coupling spins through a delocalized π-system: Vanadyl porphyrin dimers

Chem, Год журнала: 2023, Номер 10(1), С. 299 - 316

Опубликована: Окт. 11, 2023

Vanadium(IV) magnetic centers are prime candidates for molecular quantum units. One long-standing question is how to obtain a scaffold that connects multiple and allows two communication modalities: electronic. We have synthesized studied selection of vanadyl porphyrin dimers as models the most synthetically accessible linear arrays. show strongly π-conjugated backbone places system in an intermediate regime dominated by exchange coupling (J) protects coherence against electron pair flip-flop processes at low temperatures (<10 K). This result fundamental step toward design materials single-molecule devices controlled microwaves with electrical readout.

Язык: Английский

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Tunable spin and conductance in porphyrin-graphene nanoribbon hybrids

Communications Physics, Год журнала: 2023, Номер 6(1)

Опубликована: Май 23, 2023

Abstract Recently, porphyrin units have been attached to graphene nanoribbons (Por-GNR) enabling a multitude of structures. Here we report first-principles calculations two prototypical, experimentally feasible, Por-GNR hybrids, one which displays small band gap relevant as electrodes in devices. Embedding Fe atom the causes spin-polarized ground state ( S = 1). Using density functional theory and nonequilibrium Green’s function, examine 2-terminal setup involving Fe-Por-GNR between gap, electrodes. The coupling Fe- d GNR states results Fano anti-resonance feature spin transport, making conductance highly sensitive state. We demonstrate how mechanical strain or chemical adsorption on give rise spin-crossover 2 0, directly reflected transmission. Our provide deep understanding can open an avenue for carbon-based spintronics sensing.

Язык: Английский

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Conformation Governed Reactivity of Fused Thia-Sapphyrin Dimers Bearing Multiply Fused Heteroaromatic Rings

CCS Chemistry, Год журнала: 2023, Номер 5(6), С. 1332 - 1342

Опубликована: Март 7, 2023

Язык: Английский

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β-to-β Singly Linked Subphthalocyanine Dimers with Effective π-Conjugation

Organic Letters, Год журнала: 2024, Номер 26(44), С. 9471 - 9475

Опубликована: Окт. 31, 2024

In this work, a series of π-conjugated Subphthalocyanine dimers assembled by simple π-bridges were efficiently synthesized through metal-catalyzed reactions. Despite being singly linked, these readily accessible arrays exhibit excellent π-electron communication, significantly perturbing the orbital distribution conventional SubPcs and inducing notable alterations in their optical properties. The findings presented here demonstrate potential for constructing curved porphyrin with well-conjugated skeletons intriguing functionalities.

Язык: Английский

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