Category: Research Highlight

Behaviour of DFT-based approaches to the spin– orbit term of zero-field splitting tensors: a case study of metallocomplexes, MIII(acac)3 (M = V, Cr, Mn, Fe and Mo)

Phys. Chem. Chem. Phys., accepted (2017). DOI: 10.1039/C7CP05533a Spin–orbit contributions to the zero-field splitting (ZFS) tensor (DSO tensor) of MIII(acac)3 complexes (M = V, Cr, Mn, Fe and Mo; acac = acetylacetonate anion) are evaluated by means of ab initio (a hybrid CASSCF/MRMP2) and DFT (Pederson–Khanna (PK) and natural orbital-based Pederson–Khanna (NOB-PK)) methods, focusing on the behaviour of […]

Analyses of sizable ZFS and magnetic tensors of high spin metallocomplexes

Phys. Chem. Chem. Phys., accepted (2017). DOI: 10.1039/C7CP03850J The fictitious spin-1/2 Hamiltonian approach is the putative method to analyze the fine-structure/hyperfine ESR spectra of high spin metallocomplexes having sizable zerofield splitting (ZFS), thus giving salient principal g-values far from around g = 2 without explicitly providing their ZFS parameters in most cases. Indeed, the significant departure of the g-values […]

Quantum Chemistry on Quantum Computers: A Polynomial-Time Quantum Algorithm for Constructing the Wave Functions of Open-Shell Molecules

J. Phys. Chem. A 120, pp.6459-6466 (2016). DOI: 10.1021/acs.jpca.6b04932 Quantum computers are capable to efficiently perform full configuration interaction (FCI) calculations of atoms and molecules by using the quantum phase estimation (QPE) algorithm. Because the success probability of the QPE depends on the overlap between approximate and exact wave functions, efficient methods to prepare accurate initial […]

Adiabatic Quantum Computing with Spin Qubits Hosted by Molecules

Phys. Chem. Chem. Phys., accepted. DOI:10.1039/C4CP04744C  A molecular spin quantum computer (MSQC) requires electron spin qubits which pulse-based electron spin/magnetic resonance (ESR/MR) techniques can afford to manipulate for implementing quantum gate operations in open shell molecular entities. Importantly, nuclear spins which are topologically connected, particularly in organic molecular spin systems are client qubits, while electron spins […]

An ab initio MO study of heavy atom effects on the zero-field splitting tensors of high-spin nitrenes: how the spin–orbit contributions are affecte

Phys. Chem. Chem. Phys., 16, pp.9171-9181 (2014). DOI:10.1039/c4cp00822g    The CASSCF and the hybrid CASSCF–MRMP2 methods are applied to the calculations of spin–spin and spin–orbit contributions to the zero-field splitting tensors (D tensors) of the halogen-substituted spin- septet 2,4,6-trinitrenopyridines, focusing on the heavy atom effects on the spin–orbit term of the D ten- sors (DSO tensors). […]

Pulsed electron spin nutation spectroscopy for weakly exchange-coupled multi-spin molecular systems with nuclear hyperfine couplings: a general approach to bi- and triradicals and determination of their spin dipolar and exchange interactions

Molecular Physics, 111, published on the web on July 4, 2013 DOI:10.1080/00268976.2013.811304   Weakly exchange-coupled biradicals have attracted much attention in terms of their dynamic nuclear polarisation application in NMR spectroscopy for biological systems or the use of synthetic electron-spin qubits in quantum information processing/quantum-computing technology. Analogues multi-partite molecular systems are important in entering a […]

Hexamethoxyphenalenyl as a Possible Quantum Spin Simulator: An Electronically Stabilized Neutral π Radical with Novel Quantum Coherence Owing to Extremely High Nuclear Spin Degeneracy

Angew. Chem. Int. Ed., 52, published on the web on April 2, 2013 DOI:10.1002/anie.201301435 A phenalenyl radical with six methoxy groups, which were introduced symmetrically, has been synthesized. The extensively delocalized and highly symmetric lectronic-spin system was studied with advanced cw-/pulsed-ESR techniques, thereby giving an experimental model to explore molecular quantum spin simulators with novel […]

A Synthetic Two-Spin Quantum Bit: g-Engineered Exchange-Coupled Biradical Designed for Controlled-NOT Gate Operations

Angew. Chem. Int. Ed., 51, pp.9860-9864 (2012)DOI:10.1002/anie.201204489 A quantum gate: A system of two coupled electron spins that is useful for simple quantum computing operations has been prepared by synthesis of a biradical 1 and co-crystallization with an isomorphous host molecule. The two weakly exchange-coupled quantum bits (target qubit blue and control qubit red) span four […]

Pulsed electron spin nutation spectroscopy of weakly exchange-coupled biradicals: a general theoretical approach and determination of the spin dipolar interaction

Phys. Chem. Chem. Phys., 14, pp.9137-9148 (2012)DOI:10.1039/c2cp40778g Weakly exchange-coupled biradicals have attracted much attention in terms of their DNP application in NMR spectroscopy for biological systems or the use of synthetic electron-spin qubits. Pulse-ESR based electron spin nutation (ESN) spectroscopy applied to biradicals is generally treated as transition moment spectroscopy from the theoretical side, illustrating […]

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