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arXiv:0810.4822 · Laser Physics Letters

Coherent spin radiation by magnetic nanomolecules and nanoclusters

Vyacheslav I. Yukalov, Victor K. Henner, П.В. Харебов, Elizaveta P. Yukalova

Published Aug 4, 2008• 23 citations
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Abstract

The peculiarities of coherent spin radiation by magnetic nanomolecules is investigated by means of numerical simulation. The consideration is based on a microscopic Hamiltonian taking into account realistic dipole interactions. Superradiance can be realized only when the molecular sample is coupled to a resonant electric circuit. The feedback mechanism allows for the achievement of a fast spin reversal time and large radiation intensity. The influence on the level of radiation, caused by sample shape and orientation, is analysed. The most powerful coherent radiation is found to occur for an elongated sample directed along the resonator magnetic field.

DOI
10.1002/lapl.200810077

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The peculiarities of coherent spin radiation by magnetic nanomolecules is investigated by means of numerical simulation. The consideration is based on a microscopic Hamiltonian taking into account realistic dipole interactions. Superradiance can be realized only when the molecular sample is coupled to a resonant electric circuit. The feedback mechanism allows for the achievement of a fast spin reversal time and large radiation intensity. The influence on the level of radiation, caused by sample shape and orientation, is analysed. The most powerful coherent radiation is found to occur for an elongated sample directed along the resonator magnetic field.
A spin system is considered with a Hamiltonian typical of molecular magnets, having dipole-dipole interactions and a single-site magnetic anisotropy. In addition, spin interactions through the common radiation field are included. A fully quantum-mechanical derivation of the collective radiation rate is presented. An effective narrowing of the dipole-dipole attenuation, due to high spin polarization is taken into account. The influence of the radiation rate on spin dynamics is carefully analysed. It is shown that this influence is completely negligible. No noticeable collective effects, such as superradiance, can appear in molecular magnets, being caused by electromagnetic spin radiation. Spin superradiance can arise in molecular magnets only when these are coupled to a resonant electric circuit, as has been suggested earlier by one of the authors in Laser Phys. 12, 1089 (2002).
The assemblies of either quantum dots or magnetic nanoclusters are studied. It is shown that such assemblies can produce coherent radiation. A method is developed for solving the systems of nonlinear equations describing the dynamics of such assemblies. The method is shown to be general and applicable to systems of different physical nature. Despite mathematical similarities of dynamical equations, the physics of the processes for quantum dots and magnetic nanoclusters is rather different. In a quantum dot assembly, coherence develops due to the Dicke effect of dot interactions through the common radiation field. For a system of magnetic clusters, coherence in the spin motion appears due to the Purcell effect caused by the feedback action of a resonator. Self-organized coherent spin radiation cannot arise without a resonator. This principal difference is connected with the different physical nature of dipole forces between the objects. Effective dipole interactions between the radiating quantum dots, appearing due to photon exchange, collectivize the dot radiation. While the dipolar spin interactions exist from the beginning, yet before radiation, and on the contrary, they dephase spin motion, thus destroying the coherence of moving spins. In addition, quantum dot radiation exhibits turbulent photon filamentation that is absent for radiating spins.
A comparative analysis is given of spin superradiance and atomic superradiance. Their similarities and distinctions are emphasized. It is shown that, despite a close analogy, these phenomena are fundamentally different. In atomic systems, superradiance is a self-organized process, in which both the initial cause, being spontaneous emission, as well as the collectivizing mechanism of their interactions through the common radiation field, are of the same physical nature. Contrary to this, in actual spin systems with dipole interactions, the latter are the major reason for spin motion. Electromagnetic spin interactions through radiation are negligible and can never produce collective effects. The possibility of realizing superradiance in molecular magnets by coupling them to a resonant circuit is discussed.
The phenomenon of superradiation due to a resonant circuit and the backward influence of the radiation field in a standard magnetic resonance experiment is investigated. It is shown that although the effect of this phenomenon in the radio-frequency region is small, it leads to a change in the shape of the absorption line, which may be possible to observe in an appropriately designed experiment. The predicted shape of the wings of the absorption curve is unusual in magnetic resonance. This analysis, using a traditional magnetic resonance approach, compares favorably with the results of a numerical simulation of superradiation from a system of spins.
We discuss the coherent behavior of a polarized, nuclear or electron, spin system for which the magnetic dipole radiation emitted in the radio-frequency region, has approximately quadratic dependence on the number of spins. An effective method of describing these phenomena is provided by computer simulation of a microscopic model of the spin system. Important aspects of this numeric simulation are described, together with a comparison with the theoretical predictions. The behavior of the transverse component of the magnetic moment, M+(t){M}^{+}(t)M+(t), in super-radiant conditions is studied. In addition, the role of dipole-dipole interactions in super-radiation phenomena is investigated in detail. It is shown that some important features of super-radiation cannot be described with the Bloch equations.