Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Insights in Magnetodynamics from a Simple Two-Level Model

Stanislav M. Avdoshenko, Rajyavardhan Ray

Published May 7, 2020• 1 citation
Publisher

Abstract

With single-molecule magnets research on the rise as a result of recent advantages in the field, like remarkable high blocking temperatures up to 60 Kelvin [Nature, 548, 439, 2017], gigantic coercivity up to 80 Tesla [Nat Commun., 10, 571, 2019], magnetization stability in the thin films, further applications are seriously in the scope. The possible venue here is to develop a theory of magnetic moment manipulation and control at the microscopic level. Theory of optimal control in quantum dynamics in complex systems is well-developed. For example, the uses of density matrix techniques have been well summarized already in the early ‘60s by Fano, Haar, and many others. Thus, in many respects, the task is to reframe that research into the language of the problem at hand, and into familiar terms for the community. Recently, it was already proven the Redfield reduced density matrix techniques are applicable for slow-relaxing single-molecule magnets [Nat Commun., 8, 14620, 2017]. In our recent contribution[PCCP,20, 11656, 2018], we have outlined the use of Lindblad dynamics in combination with a few axioms in the rationalization of the relaxation behavior of single-molecule magnets. In this report we put this approach in the context of the magentodynamics theory, showing the close connection to the Landau-Lifshitz-Gilbert model and presenting further elaboration for the proposed method.

DOI
10.26434/chemrxiv.12246194

Related papers

Insights in Magnetodynamics from a Simple Two-Level Model

Stanislav M. Avdoshenko, Rajyavardhan Ray

With single-molecule magnets research on the rise as a result of recent advantages in the field, like remarkable high blocking temperatures up to 60 Kelvin [Nature, 548, 439, 2017], gigantic coercivity up to 80 Tesla [Nat Commun., 10, 571, 2019], magnetization stability in the thin films, further applications are seriously in the scope. The possible venue here is to develop a theory of magnetic moment manipulation and control at the microscopic level. Theory of optimal control in quantum dynamics in complex systems is well-developed. For example, the uses of density matrix techniques have been well summarized already in the early ‘60s by Fano, Haar, and many others. Thus, in many respects, the task is to reframe that research into the language of the problem at hand, and into familiar terms for the community. Recently, it was already proven the Redfield reduced density matrix techniques are applicable for slow-relaxing single-molecule magnets [Nat Commun., 8, 14620, 2017]. In our recent contribution[PCCP,20, 11656, 2018], we have outlined the use of Lindblad dynamics in combination with a few axioms in the rationalization of the relaxation behavior of single-molecule magnets. In this report we put this approach in the context of the magentodynamics theory, showing the close connection to the Landau-Lifshitz-Gilbert model and presenting further elaboration for the proposed method.

•May 7, 2020•1 citation

Quantum Magnetism and Frustration

George Mathew

A number of many-body problems that are highly complex in three dimensions can be solved in a low-dimensional system. Simple one-dimensional Hamiltonians that describe such systems have yielded exact, closed-form solutions for their dynamic and static properties. Low-dimensional magnets have gained significant attention for their distinct characteristics that facilitate the analysis of quantum model ground and excited states, the examination of potential new phases of matter, and exploration of the interplay between thermal and quantum fluctuations. The chapter’s main topic is theoretical ideas and outcomes concerning one-dimensional magnetism, and their relevance to real materials and experiments.

River Publishers eBooks•Sep 30, 2025•0 citations

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 more

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 between physical observables and the microscopic theory of magnetic relaxation, we here develop and numerically implement a first-principles linear-response theory for open quantum systems that provides access to the complex a.c. magnetic susceptibility in the presence of an oscillating a.c. magnetic field. Once combined with density functional theory and multiconfigurational electronic structure simulations, this formalism is applied in a fully first-principles fashion to three cyanido-bridged Ln/Y-based coordination polymers with general formula {Ln$^{III}_x$ Y$^{III}_{1-x}$ [Co(CN)$_6$]}, where Ln = Yb (1), Tb (2), and Dy (3). The method is able to reproduce the low-temperature direct relaxation process and its field dependence, as well as the high-temperature Orbach relaxation regime for all the investigated compounds. These results demonstrate the feasibility of ab initio simulations of magnetic a.c.susceptibility in lanthanide-based SMMs and support the potential of further development of ab initio open quantum systems methods towards the completion of a magnetization dynamics theory.

cond-mat.mtrl-sciCross-listedarXiv:2603.18725•Mar 20, 2026

Quantum control of nuclear magnetic resonance spin systems

Jun Li, Jiangyu Cui, Xiaodong Yang +6 more

With the development of quantum information science, the active manipulation of quantum systems is becoming an important research frontier. To build realistic quantum information processors, one of the challenges is to implement arbitrary desired operations with high precision on quantum systems. A large number of quantum control methods and relevant numerical techniques have been put forward in recent years, such as quantum optimal control and quantum feedback control. Nuclear magnetic resonance (NMR) spin systems offer an excellent testbed to develop benchmark tools and techniques for controlling quantum systems. In this review paper, we briefly introduce some of the basic control ideas developed for NMR systems in recent years. We first explain, for the liquid spin systems, the physics of various couplings and the causes of relaxation effects. These mechanisms govern the system dynamics, and thus are crucial for constructing rigorous and efficient control models. We also identify three types of available control means: 1) raido-frequency fields as coherent controls; 2) phase cycling, gradient fields and relaxation effects as non-unitary controls; 3) radiation damping effect as feedback control mechanism. Then, we elucidate some important control tasks, which may arise from the conventional NMR spectroscopy (e.g., pulse design and polarization transfer) or from quantum information science (e.g., algorithmic cooling and pseudo-pure state preparation). In the last part, we review some of the most important control methods that are applicable to NMR control tasks. For systems with a relatively small number of spins, it is possible to use analytic optimal control theory to realize the target unitary operations. However, for larger systems, numerical methods are necessary. The gradient ascent pulse engineering algorithm and pulse compiler techniques are the most successful techniques for implementing complicated quantum networks currently. There are some interesting topics of utilizing radiation damping and relaxation effects to achieve more powerful controls. Finally, we give an outline of the possible future work.

Acta Physica Sinica•Jan 1, 2015•4 citations

Spin quantum dynamics in molecular magnets

John J. Henderson

Molecular magnets are ideal systems to probe the realm that borders quantum and classical physics, as well as to study decoherence phenomena in nanoscale systems. The control of the quantum behavior of these materials and their structural characteristics requires synthesis of new complexes with desirable properties which will allow probing of the fundamental aspects of nanoscale physics and quantum information processing. Of particular interest among the magnetic molecular materials are single-molecule magnets (SMMs) and antiferromagnetic (AFM) molecular wheels in which the spin state of the molecule is known to behave quantum mechanically at low temperatures. In previous experiments the dynamics of the magnetic moment of the molecules is governed by incoherent quantum tunneling. Short decoherence times are mainly due to interactions between molecular magnets within the crystal and interactions of the electronic spin with the nuclear spin of neighboring ions within the molecule. This decoherence problem has imposed a limit to the understanding of the molecular spin dynamics and the sources of decoherence in condensed matter systems. Particularly, intermolecular dipolar interactions within the crystal, which shorten the coherence times in concentrated samples, have stymied progress in this direction. Several recent works have reported a direct measurement of the decoherence time in molecular magnets. This has been done by eliminating the dephasing created by dipolar interactions between neighboring molecules. This has been achieved by a) a dilution of the molecules in a liquid solution to decrease the dipolar interaction by separating the molecules, and b) by polarizing the spin bath by applying a high magnetic field at low temperatures. Unfortunately, both approaches restrict the experimental studies of quantum dynamics. For example, the dilution of molecular magnets in liquid solution causes a dispersion of the molecular spin orientation and anisotropy axes, while the large fields required to polarize the spin bath overcome the anisotropy of the molecular spin. In this thesis I have explored two methods to overcome dipolar interactions in molecular magnets: a) studying the dynamics of molecular magnets in single crystals where the separation between magnetic molecules is obtained by chemical doping or where the high crystalline quality allows observations intrinsic to the quantum mechanical nature of the tunneling of the spin, and b) studying the electronic transport through an individual magnetic molecule which has been carefully placed in a single-electron transistor device. I have used EPR microstrip resonators to measure Fe17Ga molecular wheels within single crystals of Fe18 AFM wheels, as well as demonstrating, for the first time in a Single Molecule Magnet, the complete suppression of a Quantum Tunneling of the Magnetization transition forbidden by molecular symmetry.

Journal of International Crisis and Risk Communication Research•Jan 1, 2009•0 citations

Numerical solution of quantum Landau-Lifshitz-Gilbert equation

Vahid Azimi Mousolou, Davoud Mirzaei

The classical Landau–Lifshitz–Gilbert (LLG) equation has long served as a cornerstone for modeling magnetization dynamics in magnetic systems, yet its classical nature limits its applicability to inherently quantum phenomena such as entanglement and nonlocal correlations. Inspired by the need to incorporate quantum effects into spin dynamics, recently a quantum generalization of the LLG equation is proposed [Phys. Rev. Lett. 133, 266704 (2024)] which captures essential quantum behavior in many-body systems. In this work, we develop a robust numerical methodology tailored to this quantum LLG framework that not only handles the complexity of quantum many-body systems but also preserves the intrinsic mathematical structures and physical properties dictated by the equation. We apply the proposed method to a class of quantum systems with a moderate number of spins that host host topological states of matter, and demonstrate rich quantum behavior, including the emergence of long-time entangled states. This approach opens a pathway toward reliable simulations of quantum magnetism beyond classical approximations, potentially leading to new discoveries.

arXiv:2506.19594•Computer Physics Communications•Oct 28, 2025•1 citation
With single-molecule magnets research on the rise as a result of recent advantages in the field, like remarkable high blocking temperatures up to 60 Kelvin [Nature, 548, 439, 2017], gigantic coercivity up to 80 Tesla [Nat Commun., 10, 571, 2019], magnetization stability in the thin films, further applications are seriously in the scope. The possible venue here is to develop a theory of magnetic moment manipulation and control at the microscopic level. Theory of optimal control in quantum dynamics in complex systems is well-developed. For example, the uses of density matrix techniques have been well summarized already in the early ‘60s by Fano, Haar, and many others. Thus, in many respects, the task is to reframe that research into the language of the problem at hand, and into familiar terms for the community. Recently, it was already proven the Redfield reduced density matrix techniques are applicable for slow-relaxing single-molecule magnets [Nat Commun., 8, 14620, 2017]. In our recent contribution[PCCP,20, 11656, 2018], we have outlined the use of Lindblad dynamics in combination with a few axioms in the rationalization of the relaxation behavior of single-molecule magnets. In this report we put this approach in the context of the magentodynamics theory, showing the close connection to the Landau-Lifshitz-Gilbert model and presenting further elaboration for the proposed method.
With single-molecule magnets research on the rise as a result of recent advantages in the field, like remarkable high blocking temperatures up to 60 Kelvin [Nature, 548, 439, 2017], gigantic coercivity up to 80 Tesla [Nat Commun., 10, 571, 2019], magnetization stability in the thin films, further applications are seriously in the scope. The possible venue here is to develop a theory of magnetic moment manipulation and control at the microscopic level. Theory of optimal control in quantum dynamics in complex systems is well-developed. For example, the uses of density matrix techniques have been well summarized already in the early ‘60s by Fano, Haar, and many others. Thus, in many respects, the task is to reframe that research into the language of the problem at hand, and into familiar terms for the community. Recently, it was already proven the Redfield reduced density matrix techniques are applicable for slow-relaxing single-molecule magnets [Nat Commun., 8, 14620, 2017]. In our recent contribution[PCCP,20, 11656, 2018], we have outlined the use of Lindblad dynamics in combination with a few axioms in the rationalization of the relaxation behavior of single-molecule magnets. In this report we put this approach in the context of the magentodynamics theory, showing the close connection to the Landau-Lifshitz-Gilbert model and presenting further elaboration for the proposed method.
A number of many-body problems that are highly complex in three dimensions can be solved in a low-dimensional system. Simple one-dimensional Hamiltonians that describe such systems have yielded exact, closed-form solutions for their dynamic and static properties. Low-dimensional magnets have gained significant attention for their distinct characteristics that facilitate the analysis of quantum model ground and excited states, the examination of potential new phases of matter, and exploration of the interplay between thermal and quantum fluctuations. The chapter’s main topic is theoretical ideas and outcomes concerning one-dimensional magnetism, and their relevance to real materials and experiments.
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 between physical observables and the microscopic theory of magnetic relaxation, we here develop and numerically implement a first-principles linear-response theory for open quantum systems that provides access to the complex a.c. magnetic susceptibility in the presence of an oscillating a.c. magnetic field. Once combined with density functional theory and multiconfigurational electronic structure simulations, this formalism is applied in a fully first-principles fashion to three cyanido-bridged Ln/Y-based coordination polymers with general formula {LnxIII^{III}_xxIII​ Y1−xIII^{III}_{1-x}1−xIII​ [Co(CN)6_66​]}, where Ln = Yb (1), Tb (2), and Dy (3). The method is able to reproduce the low-temperature direct relaxation process and its field dependence, as well as the high-temperature Orbach relaxation regime for all the investigated compounds. These results demonstrate the feasibility of ab initio simulations of magnetic a.c.susceptibility in lanthanide-based SMMs and support the potential of further development of ab initio open quantum systems methods towards the completion of a magnetization dynamics theory.
With the development of quantum information science, the active manipulation of quantum systems is becoming an important research frontier. To build realistic quantum information processors, one of the challenges is to implement arbitrary desired operations with high precision on quantum systems. A large number of quantum control methods and relevant numerical techniques have been put forward in recent years, such as quantum optimal control and quantum feedback control. Nuclear magnetic resonance (NMR) spin systems offer an excellent testbed to develop benchmark tools and techniques for controlling quantum systems. In this review paper, we briefly introduce some of the basic control ideas developed for NMR systems in recent years. We first explain, for the liquid spin systems, the physics of various couplings and the causes of relaxation effects. These mechanisms govern the system dynamics, and thus are crucial for constructing rigorous and efficient control models. We also identify three types of available control means: 1) raido-frequency fields as coherent controls; 2) phase cycling, gradient fields and relaxation effects as non-unitary controls; 3) radiation damping effect as feedback control mechanism. Then, we elucidate some important control tasks, which may arise from the conventional NMR spectroscopy (e.g., pulse design and polarization transfer) or from quantum information science (e.g., algorithmic cooling and pseudo-pure state preparation). In the last part, we review some of the most important control methods that are applicable to NMR control tasks. For systems with a relatively small number of spins, it is possible to use analytic optimal control theory to realize the target unitary operations. However, for larger systems, numerical methods are necessary. The gradient ascent pulse engineering algorithm and pulse compiler techniques are the most successful techniques for implementing complicated quantum networks currently. There are some interesting topics of utilizing radiation damping and relaxation effects to achieve more powerful controls. Finally, we give an outline of the possible future work.
Molecular magnets are ideal systems to probe the realm that borders quantum and classical physics, as well as to study decoherence phenomena in nanoscale systems. The control of the quantum behavior of these materials and their structural characteristics requires synthesis of new complexes with desirable properties which will allow probing of the fundamental aspects of nanoscale physics and quantum information processing. Of particular interest among the magnetic molecular materials are single-molecule magnets (SMMs) and antiferromagnetic (AFM) molecular wheels in which the spin state of the molecule is known to behave quantum mechanically at low temperatures. In previous experiments the dynamics of the magnetic moment of the molecules is governed by incoherent quantum tunneling. Short decoherence times are mainly due to interactions between molecular magnets within the crystal and interactions of the electronic spin with the nuclear spin of neighboring ions within the molecule. This decoherence problem has imposed a limit to the understanding of the molecular spin dynamics and the sources of decoherence in condensed matter systems. Particularly, intermolecular dipolar interactions within the crystal, which shorten the coherence times in concentrated samples, have stymied progress in this direction. Several recent works have reported a direct measurement of the decoherence time in molecular magnets. This has been done by eliminating the dephasing created by dipolar interactions between neighboring molecules. This has been achieved by a) a dilution of the molecules in a liquid solution to decrease the dipolar interaction by separating the molecules, and b) by polarizing the spin bath by applying a high magnetic field at low temperatures. Unfortunately, both approaches restrict the experimental studies of quantum dynamics. For example, the dilution of molecular magnets in liquid solution causes a dispersion of the molecular spin orientation and anisotropy axes, while the large fields required to polarize the spin bath overcome the anisotropy of the molecular spin. In this thesis I have explored two methods to overcome dipolar interactions in molecular magnets: a) studying the dynamics of molecular magnets in single crystals where the separation between magnetic molecules is obtained by chemical doping or where the high crystalline quality allows observations intrinsic to the quantum mechanical nature of the tunneling of the spin, and b) studying the electronic transport through an individual magnetic molecule which has been carefully placed in a single-electron transistor device. I have used EPR microstrip resonators to measure Fe17Ga molecular wheels within single crystals of Fe18 AFM wheels, as well as demonstrating, for the first time in a Single Molecule Magnet, the complete suppression of a Quantum Tunneling of the Magnetization transition forbidden by molecular symmetry.
The classical Landau–Lifshitz–Gilbert (LLG) equation has long served as a cornerstone for modeling magnetization dynamics in magnetic systems, yet its classical nature limits its applicability to inherently quantum phenomena such as entanglement and nonlocal correlations. Inspired by the need to incorporate quantum effects into spin dynamics, recently a quantum generalization of the LLG equation is proposed [Phys. Rev. Lett. 133, 266704 (2024)] which captures essential quantum behavior in many-body systems. In this work, we develop a robust numerical methodology tailored to this quantum LLG framework that not only handles the complexity of quantum many-body systems but also preserves the intrinsic mathematical structures and physical properties dictated by the equation. We apply the proposed method to a class of quantum systems with a moderate number of spins that host host topological states of matter, and demonstrate rich quantum behavior, including the emergence of long-time entangled states. This approach opens a pathway toward reliable simulations of quantum magnetism beyond classical approximations, potentially leading to new discoveries.