Spin–lattice relaxation with non-linear couplings: Comparison between Fermi’s golden rule and extended dissipaton equation of motion DOI
Ruihao Bi, Yu Su, Yao Wang

et al.

The Journal of Chemical Physics, Journal Year: 2024, Volume and Issue: 161(2)

Published: July 10, 2024

Fermi’s golden rule (FGR) offers an empirical framework for understanding the dynamics of spin–lattice relaxation in magnetic molecules, encompassing mechanisms like direct (one-phonon) and Raman (two-phonon) processes. These principles effectively model experimental longitudinal rates, denoted as T1−1. However, under scenarios increased coupling strength nonlinear interactions, FGR’s applicability may diminish. This paper numerically evaluates exact rate kernels, employing extended dissipaton equation motion formalism. Our calculations reveal that when quadratic is considered, kernels exhibit a free induction decay-like feature, damping rates depend on interaction strength. We observe temperature dependence predicted by FGR significantly deviates from results since ignores higher order effects non-Markovian nature relaxation. methods can be easily to study other systems with interactions provide valuable insights into T1 molecular qubits strong.

Language: Английский

Tunable Charge Transport and Spin Dynamics in Two-Dimensional Conjugated Metal–Organic Frameworks DOI
Lu Yang, Ziqi Hu, Petko St. Petkov

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(4), P. 2574 - 2582

Published: Jan. 17, 2024

Two-dimensional conjugated metal–organic frameworks (2D c-MOFs) have attracted increasing interest in electronics due to their (semi)conducting properties. Charge-neutral 2D c-MOFs also possess persistent organic radicals that can be viewed as spin-concentrated arrays, affording new opportunities for spintronics. However, the strong π-interaction between neighboring layers of layer-stacked annihilates active spin centers and significantly accelerates relaxation, severely limiting potential qubits. Herein, we report precise tuning charge transport dynamics via control interlayer stacking. The introduction bulky side groups on ligands enables a significant dislocation from serrated stacking staggered stacking, thereby spatially weakening interactions. As consequence, electrical conductivity decreases by 6 orders magnitude, while density achieves more than 30-fold increase spin–lattice relaxation time (T1) is increased up ∼60 μs, hence being superior reference with compact stackings whose too fast detected. Spin results reveal spinless polaron pairs or bipolarons play critical roles these c-MOFs. Our strategy provides bottom-up approach enlarging c-MOFs, opening pathways developing MOF-based

Language: Английский

Citations

31
Stable organic radical qubits and their applications in quantum information science DOI Creative Commons
Ai-Mei Zhou,

Zhecheng Sun,

Lei Sun

et al.

The Innovation, Journal Year: 2024, Volume and Issue: 5(5), P. 100662 - 100662

Published: June 21, 2024

The past century has witnessed the flourishing of organic radical chemistry. Stable radicals are highly valuable for quantum technologies thanks to their inherent room temperature coherence, atomic-level designability, and fine tunability. In this comprehensive review, we highlight potential stable as high-temperature qubits explore applications in information science, which remain largely underexplored. Firstly, summarize known spin dynamic properties examine factors that influence electron relaxation decoherence times. This examination reveals design principles optimal operating conditions. We further discuss integration solid-state materials surface structures, present state-of-the-art computing, memory, sensing. Finally, analyze primary challenges associated with provide tentative insights future research directions.

Language: Английский

Citations

15
Photons, Excitons, and Electrons in Covalent Organic Frameworks DOI Creative Commons
Dominic Blätte, Frank Ortmann, Thomas Bein

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(47), P. 32161 - 32205

Published: Nov. 18, 2024

Covalent organic frameworks (COFs) are created by the condensation of molecular building blocks and nodes to form two-dimensional (2D) or three-dimensional (3D) crystalline frameworks. The diversity with different properties functionalities large number possible framework topologies open a vast space well-defined porous architectures. Besides more classical applications materials such as absorption, separation, catalytic conversions, interest in optoelectronic COFs has recently increased considerably. electronic both their linkage chemistry can be controlled tune photon absorption emission, create excitons charge carriers, use these carriers photocatalysis, luminescence, chemical sensing, photovoltaics. In this Perspective, we will discuss relationship between structural features properties, starting connectivity, layer stacking 2D COFs, control over defects morphology including thin film synthesis, exploring theoretical modeling structural, electronic, dynamic discussing recent intriguing focus on photocatalysis photoelectrochemistry. We conclude some remarks about present challenges future prospects powerful architectural paradigm.

Language: Английский

Citations

12
Rational Construction of Layered Two-Dimensional Conjugated Metal–Organic Frameworks with Room-Temperature Quantum Coherence DOI Creative Commons
Yang Lu, Yubin Fu, Ziqi Hu

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 27, 2025

Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) have emerged as an intriguing class of quantum materials due to their high crystallinity, persistent spin centers, and tunable structures topologies. However, it remains unclear how achieve long relaxation time at room temperature in 2D c-MOFs via a bottom-up design strategy. Herein, we hexahydroxytrithiatruxene ligand (HHTH) minimize the influence nuclear on electron while weakening d-π conjugation construct "spin docking" for preserving which enables resulting c-MOFs, Ni3HHTH2, exhibit coherence Rabi oscillations temperature. Spin dynamics studies not only reveal unusual temperature-dependent frequency Ni3HHTH2 but also indicate that coordination mode determines spin-lattice behavior spin-phonon coupling. These investigations provide general guideline development high-performance qubits based arrays.

Language: Английский

Citations

1
Rational Construction of Two-Dimensional Conjugated Metal–Organic Frameworks (2D c-MOFs) for Electronics and Beyond DOI Creative Commons
Yang Lu, Paolo Samorı́, Xinliang Feng

et al.

Accounts of Chemical Research, Journal Year: 2024, Volume and Issue: 57(14), P. 1985 - 1996

Published: July 4, 2024

ConspectusTwo-dimensional conjugated metal-organic frameworks (2D c-MOFs) have emerged as a novel class of multifunctional materials, attracting increasing attention due to their highly customizable chemistry yielding programmable and unprecedented structures properties. In particular, over the past decade, synergistic relationship between conductivity porosity 2D c-MOFs has paved way toward widespread applications. Despite promising potential, majority yet achieve atomically precise crystal structures, hindering full understanding control electronic structure intrinsic charge transport characteristics. When modulating properties two-dimensional layered framework decoupling processes within in layers is paramount importance, it represents significant challenge. Unfortunately, systems developed so far failed address such major research target, which can be achieved solely by manipulating c-MOFs. offer advantage organic radical molecules covalent frameworks: polymerization through oxidative coordination viable route form "spin-concentrated assemblies". However, role these spin centers still poorly understood, dynamics spins seldom been investigated. Consequently, overcoming challenges essential unlock potential electronics other related fields, new type quantum materials.In this Account, we summarize discuss our group's efforts at atomic level applications spintronics, thereby providing distinct evidence on platform for exploring phenomena. First, unravel key played rational design ligands decrease boundary defects, large single crystals, investigate The advantages disadvantages current structural elucidation strategies will discussed. Second, fundamental challenge c-MOF studies decouple in-plane interlayer pathways tuning To challenge, propose concept second-generation ligands, termed "programmable ligands", replace first-generation lack modifiability they mainly consist

Language: Английский

Citations

8
Electronic and quantum properties of organic two-dimensional crystals DOI
Zhiyong Wang, Mingchao Wang, Thomas Heine

et al.

Nature Reviews Materials, Journal Year: 2024, Volume and Issue: 10(2), P. 147 - 166

Published: Nov. 6, 2024

Language: Английский

Citations

8
Oriented Triplet Excitons as Long-Lived Electron Spin Qutrits in a Molecular Donor–Acceptor Single Cocrystal DOI
Jonathan R. Palmer, Malik L. Williams, Ryan M. Young

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 146(1), P. 1089 - 1099

Published: Dec. 29, 2023

The photogeneration of multiple unpaired electron spins within molecules is a promising route to applications in quantum information science because they can be initialized into well-defined, multilevel states (S > 1/2) and reproducibly fabricated by chemical synthesis. However, coherent manipulation these spin difficult realize typical molecular systems due the lack selective addressability short coherence times transitions. Here, challenges are addressed using donor–acceptor single cocrystals composed pyrene naphthalene dianhydride host spatially oriented triplet excitons, which exhibit photogenerated qutrit properties. Time-resolved paramagnetic resonance (TREPR) spectroscopy demonstrates that orienting excitons crystal platform imparts narrow, well-resolved, tunable resonances EPR spectrum, allowing sublevel Pulse-EPR reveals at temperatures above 30 K, decoherence driven exciton diffusion. limited electronic dipolar coupling below where T2 varies nonlinearly with optical excitation density annihilation. Overall, an optimized time = 7.1 μs 20 K achieved. These results provide important insights designing solid-state excitonic materials improved

Language: Английский

Citations

17
Enhancing Coherence Times of Chromophore-Radical Molecular Qubits and Qudits by Rational Design DOI
Yunfan Qiu, Hannah J. Eckvahl, Asif Equbal

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(47), P. 25903 - 25909

Published: Nov. 14, 2023

An important criterion for quantum operations is long qubit coherence times. To elucidate the influence of molecular structure on times spin qubits and qudits, a series molecules featuring perylenediimide (PDI) chromophores covalently linked to stable nitroxide radicals were synthesized investigated by pulse electron paramagnetic resonance spectroscopy. Photoexcitation PDI in these systems creates an excited quartet state (Q) followed spin-polarized doublet ground (D0), which hold promise as qudits qubits, respectively. By tailoring qudit/qubit candidates selective deuteration eliminating intramolecular motion, Tm = 9.1 ± 0.3 4.2 μs at 85 K D0 Q, respectively, are achieved. These represent nearly 3-fold enhancement compared those initial design. This approach offers rational structural design protocol effectively extending qudits/qubits.

Language: Английский

Citations

15
Metalloporphyrins as Building Blocks for Quantum Information Science DOI Creative Commons
Fabio Santanni, Alberto Privitera

Advanced Optical Materials, Journal Year: 2024, Volume and Issue: 12(18)

Published: May 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.

Language: Английский

Citations

6
A multifunctional pseudo-[6]oxocarbon molecule innate to six accessible oxidation states DOI Creative Commons
Paweł Pakulski, Michał Magott, Szymon Chorąży

et al.

Chem, Journal Year: 2024, Volume and Issue: 10(3), P. 971 - 997

Published: Jan. 22, 2024

Language: Английский

Citations

4