227 citations · 456 across the 33 of their papers we have counts for
35 papers
Multireference Density Matrix Embedding for Spin-Phonon Relaxation
Shreya Verma, Antonio L. Mariano, Matthew R. Hermes +3
Spin-phonon coupling governs magnetic relaxation in numerous systems including single-molecule magnets and molecular spin qubits. In most cases, the accurate prediction of spin rel…
Triangulene-based diradicals as a blueprint for molecular quantum platforms with optical addressability and long spin coherence times
Arup Sarkar, Cathal Hogan, Conor Ryan +2
The identification of molecules that combine long spin coherence times and efficient spin-optical interfaces, ideally at room temperature, is pivotal towards the development of mol…
Maximizing the magnetic anisotropy of Dy complexes by fine tuning organic ligands: A systematic multireference high-throughput exploration of over 30k molecules
Lion Frangoulis, Lorenzo A. Mariano. Vu Ha Anh Nguyen, Zahra Khatibi +1
The design of the coordination environment of magnetic ions is key to achieving properties such as large magnetic anisotropy and slow magnetic relaxation, but a systematic explorat…
A first-principles linear response theory for open quantum systems and its application to Orbach and direct magnetic relaxation in Ln-based coordination polymers
Mikolaj Żychowicz, Jakub J. Zakrzewski, Szymon Chorazy +1
Single-Molecule Magnets (SMMs) exhibit slow magnetic relaxation as a result of axial magnetic anisotropy inhibiting spin-phonon transitions. In order to establish a direct link bet…
Raman relaxation in Yb(III) molecular qubits: non-trivial correlations between spin-phonon coupling and molecular structure
Giacomo Sansone, Lorenzo A. Mariano, Stefano Carretta +2
The coordination complexes of Yb(III) exhibit some of the longest spin coherence times among 4f compounds, making them a promising platform for molecular quantum technologies. Whil…
Extending spin-lattice relaxation theory to three-phonon processes
Nilanjana Chanda, Alessandro Lunghi
Spin-lattice relaxation theory has been developed over almost a century, but some cardinal assumptions on the nature of the interactions involved have never been fully verified. Th…
Efficient training of generative models from multireference simulations and its application to the design of Dy complexes with large magnetic anisotropy
Zahra Khatibi, Lorenzo A. Mariano, Lion Frangoulis +1
Generative machine learning models can potentially provide direct access to novel and relevant portions of the full chemical space, overcoming the cost of systematic sampling. Howe…
On the challenge of simulating dipolar contributions to spin relaxation with generalized cluster correlation expansion methods
Conor Ryan, Alessandro Lunghi
The study of spin decoherence is often performed by assuming that spin-phonon interactions lead to relaxation at high temperatures, and spin-spin dipolar interactions instead contr…
Fourth-order quantum master equations reveal that spin-phonon decoherence undercuts long magnetization relaxation times in single-molecule magnets
Alessandro Lunghi
Spin-phonon interaction is known to drive magnetic relaxation in solid-state systems, but little evidence is available on how it affects coherence time. Here we extend fourth-order…
A multireference picture of electronic excited states in vanadyl and copper tetraphenyl porphyrin molecular qubits
Arup Sarkar, Alessandro Lunghi
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 multicon…
Spin decoherence in molecular crystals: nuclear v.s. electronic spin baths
Conor Ryan, Valerio Briganti, Cathal Hogan +2
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…
Generating new coordination compounds via multireference simulations, genetic algorithms and machine learning: the case of Co(II) molecular magnets
Lion Frangoulis, Zahra Khatibi, Lorenzo A. Mariano +1
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 mo…
The spin-phonon relaxation mechanism of single-molecule magnets in the presence of strong exchange coupling
Sourav Mondal, Julia Netz, David Hunger +5
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 em…
The Mechanism of Spin-Phonon Relaxation in Endohedral Metallofullene Single Molecule Magnets
Tanu Sharma, Rupesh Kumar Tiwari, Sourav Dey +3
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 calcu…
A machine-learning framework for accelerating spin-lattice relaxation simulations
Valerio Briganti, Alessandro Lunghi
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 s…
Charting new regions of Cobalt's chemical space with maximally large magnetic anisotropy: A computational high-throughput study
Lorenzo A. Mariano, Vu Ha Anh Nguyen, Valerio Briganti +1
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 magne…
The role of electronic excited states in the spin-lattice relaxation of spin-1/2 molecules
Lorenzo A. Mariano, Vu Ha Anh Nguyen, Jonatan B. Petersen +5
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 considerin…
Spin-vibronic dynamics in open-shell systems beyond the spin Hamiltonian formalism
Lorenzo A. Mariano, Sourav Mondal, Alessandro Lunghi
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…
Efficient Generation of Stable Linear Machine-Learning Force Fields with Uncertainty-Aware Active Learning
Valerio Briganti, Alessandro Lunghi
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 da…
A self-consistent field approach for the variational quantum eigensolver: orbital optimization goes adaptive
Aaron Fitzpatrick, Anton Nykänen, N. Walter Talarico +4
We present a self consistent field approach (SCF) within the Adaptive Derivative-Assembled Problem-Tailored Ansatz Variational Quantum Eigensolver (ADAPT-VQE) framework for efficie…
Spin-phonon decoherence in solid-state paramagnetic defects from first principles
Sourav Mondal, Alessandro Lunghi
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…
Unravelling the contributions to spin-lattice relaxation in Kramers single-molecule magnets
Sourav Mondal, Alessandro Lunghi
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 structur…
Spin-Phonon Relaxation in Magnetic Molecules: Theory, Predictions and Insights
Alessandro Lunghi
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…
Predicting tensorial molecular properties with equivariant machine-learning models
Vu Ha Anh Nguyen, Alessandro Lunghi
Embedding molecular symmetries into machine-learning models is key for efficient learning of chemico-physical scalar properties, but little evidence on how to extend the same strat…