Alessandro Lunghi
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View article: Chiral Dysprosium-[7]Helicene Macrocycles Showing Record Single-Molecule Magnet Properties in the Lanthanide–Helicene Family
Chiral Dysprosium-[7]Helicene Macrocycles Showing Record Single-Molecule Magnet Properties in the Lanthanide–Helicene Family Open
Chiral helicene-based metal complexes have emerged as an extremely promising class of multifunctional molecules for a wide range of applications. Despite significant progress in the synthesis of helicene-based transition-metal complexes in…
View article: Spin decoherence in molecular crystals: Nuclear vs electronic spin baths
Spin decoherence in molecular crystals: Nuclear vs electronic spin baths Open
The loss of information about the relative phase between two quantum states, known as decoherence, strongly limits resolution in electron paramagnetic spectroscopy and hampers the use of molecules for quantum information processing. At low…
View article: Supramolecular Interactions Modulate Raman Relaxation in D5h Symmetric Dy(III) Single-Molecule Magnets Opening the Magnetic Hysteresis up to 50 K
Supramolecular Interactions Modulate Raman Relaxation in D5h Symmetric Dy(III) Single-Molecule Magnets Opening the Magnetic Hysteresis up to 50 K Open
Dysprosium-based single-molecule magnets (SMMs) exhibit large values of magnetic anisotropy and large coercive fields, offering the potential to support magnetic information storage at the molecular level. Owning to the molecular nature of…
View article: Generating New Coordination Compounds via Multireference Simulations, Genetic Algorithms, and Machine Learning: The Case of Co(II) and Dy(III) Molecular Magnets
Generating New Coordination Compounds via Multireference Simulations, Genetic Algorithms, and Machine Learning: The Case of Co(II) and Dy(III) Molecular Magnets Open
The design of coordination compounds with target properties often requires years of continuous feedback loop between theory, simulations, and experiments. In the case of magnetic molecules, this conventional strategy has indeed led to the …
View article: A Multireference Picture of Electronic Excited States in Vanadyl and Copper Tetraphenyl Porphyrin Molecular Qubits
A Multireference Picture of Electronic Excited States in Vanadyl and Copper Tetraphenyl Porphyrin Molecular Qubits Open
The nature of electronic excited states has a deep impact on the dynamics of molecular spins but remains poorly understood and characterized. Here we carry out a thorough multiconfigurational investigation for two prototypical molecular qu…
View article: The Spin-Phonon Relaxation Mechanism of Single-Molecule Magnets in the Presence of Strong Exchange Coupling
The Spin-Phonon Relaxation Mechanism of Single-Molecule Magnets in the Presence of Strong Exchange Coupling Open
Magnetic relaxation in coordination compounds is largely dominated by the interaction of the spin with phonons. Although a comprehensive understanding of spin-phonon relaxation has been achieved for mononuclear complexes, only a qualitativ…
View article: Role of Electron Correlation beyond the Active Space in Achieving Quantitative Predictions of Spin-Phonon Relaxation
Role of Electron Correlation beyond the Active Space in Achieving Quantitative Predictions of Spin-Phonon Relaxation Open
Single-molecule magnets (SMMs) are promising candidates for molecular-scale data storage and processing due to their strong magnetic anisotropy and long spin relaxation times. However, as the temperature rises, interactions between electro…
View article: The role of electronic excited states in the spin-lattice relaxation of spin-1/2 molecules
The role of electronic excited states in the spin-lattice relaxation of spin-1/2 molecules Open
Magnetic resonance is a prime method for the study of chemical and biological structures and their dynamical processes. The interpretation of many of these experiments relies on understanding how the spin of unpaired electrons exchanges en…
View article: The mechanism of spin-phonon relaxation in endohedral metallofullerene single molecule magnets
The mechanism of spin-phonon relaxation in endohedral metallofullerene single molecule magnets Open
Low-lying phonons associated with the specific bending motion of cluster atoms with high spin-phonon coupling play a crucial role in the system's relaxation dynamics.
View article: The Role of Electron Correlation Beyond the Active Space in Achieving Quantitative Predictions of Spin-Phonon Relaxation
The Role of Electron Correlation Beyond the Active Space in Achieving Quantitative Predictions of Spin-Phonon Relaxation Open
Single-molecule magnets (SMMs) are promising candidates for molecular-scale data storage and processing due to their strong magnetic anisotropy and long spin relaxation times. However, as temperature rises, interactions between electronic …
View article: The spin-phonon relaxation mechanism of single-molecule magnets in the presence of strong exchange coupling
The spin-phonon relaxation mechanism of single-molecule magnets in the presence of strong exchange coupling Open
Magnetic relaxation in coordination compounds is largely dominated by the interaction of the spin with phonons. Large zero-field splitting and exchange coupling values have been empirically found to strongly suppress spin relaxation and ha…
View article: Charting Regions of Cobalt’s Chemical Space with Maximally Large Magnetic Anisotropy: A Computational High-Throughput Study
Charting Regions of Cobalt’s Chemical Space with Maximally Large Magnetic Anisotropy: A Computational High-Throughput Study Open
Magnetic anisotropy slows down magnetic relaxation and plays a prominent role in the design of permanent magnets. Coordination compounds of Co(II) in particular exhibit large magnetic anisotropy in the presence of low-coordination environm…
View article: The Mechanism of Spin-Phonon Relaxation in Endohedral Metallofullene Single Molecule Magnets
The Mechanism of Spin-Phonon Relaxation in Endohedral Metallofullene Single Molecule Magnets Open
This study presents the first-ever investigation of spin-phonon coupling mechanisms in fullerene-based single-molecule magnets (SMMs) using ab initio CASSCF combined with DFT calculations. While lanthanide-based SMMs, particularly those wi…
View article: A machine-learning framework for accelerating spin-lattice relaxation simulations
A machine-learning framework for accelerating spin-lattice relaxation simulations Open
Molecular and lattice vibrations are able to couple to the spin of electrons and lead to their relaxation and decoherence. Ab initio simulations have played a fundamental role in shaping our understanding of this process but further progre…
View article: Charting new regions of Cobalt's chemical space with maximally large magnetic anisotropy: A computational high-throughput study
Charting new regions of Cobalt's chemical space with maximally large magnetic anisotropy: A computational high-throughput study Open
Magnetic anisotropy slows down magnetic relaxation and plays a prominent role in the design of permanent magnets. Coordination compounds of Co(II) in particular exhibit large magnetic anisotropy in the presence of low-coordination environm…
View article: The role of electronic excited states in the spin-lattice relaxation of spin-1/2 molecules
The role of electronic excited states in the spin-lattice relaxation of spin-1/2 molecules Open
Magnetic resonance is a prime method for the study of chemical and biological structures and their dynamical processes. The interpretation of these experiments relies on considering the spin of electrons as the sole relevant degree of free…
View article: Spin-Vibronic Dynamics in Open-Shell Systems beyond the Spin Hamiltonian Formalism
Spin-Vibronic Dynamics in Open-Shell Systems beyond the Spin Hamiltonian Formalism Open
Vibronic coupling has a dramatic influence over a large number of molecular processes, ranging from photochemistry to spin relaxation and electronic transport. The simulation of vibronic coupling with multireference wave function methods h…
View article: Spin-vibronic dynamics in open-shell systems beyond the spin Hamiltonian formalism
Spin-vibronic dynamics in open-shell systems beyond the spin Hamiltonian formalism Open
Vibronic coupling has a dramatic influence over a large number of molecular processes, ranging from photo-chemistry, to spin relaxation and electronic transport. The simulation of vibronic coupling with multi-reference wavefunction methods…
View article: Spin-phonon decoherence in solid-state paramagnetic defects from first principles
Spin-phonon decoherence in solid-state paramagnetic defects from first principles Open
Paramagnetic defects in diamond and hexagonal boron nitride possess a combination of spin and optical properties that make them prototypical solid-state qubits. Despite the coherence of these spin qubits being critically limited by spin-ph…
View article: Efficient generation of stable linear machine-learning force fields with uncertainty-aware active learning
Efficient generation of stable linear machine-learning force fields with uncertainty-aware active learning Open
Machine-learning (ML) force fields (FFs) enable an accurate and universal description of the potential energy surface of molecules and materials on the basis of a training set of ab initio data. However, large-scale applications of these m…
View article: Stiffness and Atomic-Scale Friction in Superlubricant MoS<sub>2</sub> Bilayers
Stiffness and Atomic-Scale Friction in Superlubricant MoS<sub>2</sub> Bilayers Open
Molecular dynamics simulations, performed with chemically accurate ab initio machine-learning force fields, are used to demonstrate that layer stiffness has profound effects on the superlubricant state of two-dimensional van der Waals hete…
View article: Efficient Generation of Stable Linear Machine-Learning Force Fields with Uncertainty-Aware Active Learning
Efficient Generation of Stable Linear Machine-Learning Force Fields with Uncertainty-Aware Active Learning Open
Machine-learning force fields enable an accurate and universal description of the potential energy surface of molecules and materials on the basis of a training set of ab initio data. However, large-scale applications of these methods rest…
View article: The critical role of ultra-low-energy vibrations in the relaxation dynamics of molecular qubits
The critical role of ultra-low-energy vibrations in the relaxation dynamics of molecular qubits Open
Improving the performance of molecular qubits is a fundamental milestone towards unleashing the power of molecular magnetism in the second quantum revolution. Taming spin relaxation and decoherence due to vibrations is crucial to reach thi…
View article: Spin-Phonon Relaxation in Magnetic Molecules: Theory, Predictions and Insights
Spin-Phonon Relaxation in Magnetic Molecules: Theory, Predictions and Insights Open
Magnetic molecules have played a central role in the development of magnetism and coordination chemistry, and their study keeps leading innovation in cutting-edge scientific fields such as magnetic resonance, magnetism, spintronics, and qu…
View article: Spin-phonon decoherence in solid-state paramagnetic defects from first principles
Spin-phonon decoherence in solid-state paramagnetic defects from first principles Open
Paramagnetic defects in diamond and hexagonal boron nitride possess a unique combination of spin and optical properties that make them prototypical solid-state qubits. Despite the coherence of these spin qubits being critically limited by …
View article: A self-consistent field approach for the variational quantum eigensolver: orbital optimization goes adaptive
A self-consistent field approach for the variational quantum eigensolver: orbital optimization goes adaptive Open
We present a self consistent field approach (SCF) within the Adaptive Derivative-Assembled Problem-Tailored Ansatz Variational Quantum Eigensolver (ADAPT-VQE) framework for efficient quantum simulations of chemical systems on near-term qua…
View article: Unraveling the Contributions to Spin–Lattice Relaxation in Kramers Single-Molecule Magnets
Unraveling the Contributions to Spin–Lattice Relaxation in Kramers Single-Molecule Magnets Open
The study of how spin interacts with lattice vibrations and relaxes to equilibrium provides unique insights into its chemical environment and the relation between electronic structure and molecular composition. Despite its importance for s…
View article: Unravelling the contributions to spin-lattice relaxation in Kramers single-molecule magnets
Unravelling the contributions to spin-lattice relaxation in Kramers single-molecule magnets Open
The study of how spin interacts with lattice vibrations and relaxes to equilibrium provides unique insights on its chemical environment and the relation between electronic structure and molecular composition. Despite its importance for sev…