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Bulletin of the American Physical Society

Electromagnetic radiation emanating from the molecular nanomagnet Fe$_{8}$

Amit Keren, Oren Shafir

Published Mar 20, 2009• 0 citations
OpenAlex

Abstract

Photons emitted by transition between the discrete levels of single molecular magnets might obey the elementary condition for Dicke’s super-radiance. We investigate this possibility in the Fe8 molecule where magnetization jumps are known to occur at discrete magnetic-field values. We found energy bursts each time the molecule undergoes a magnetization jump, confirming their quantum nature. A series of tests indicated that photons carry out the energy and that indeed these photons obey the elementary conditions for super-radiance.

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Electromagnetic radiation emanating from the molecular nanomagnet Fe8_{8}8​
Photons emitted by transition between the discrete levels of single molecular magnets might obey the elementary condition for Dicke’s super-radiance. We investigate this possibility in the Fe8 molecule where magnetization jumps are known to occur at discrete magnetic-field values. We found energy bursts each time the molecule undergoes a magnetization jump, confirming their quantum nature. A series of tests indicated that photons carry out the energy and that indeed these photons obey the elementary conditions for super-radiance.
Photons emitted by transition between the discrete levels of single molecular magnets might obey the elementary condition for Dicke's super-radiance. We investigate this possibility in the Fe8{\text{Fe}}_{8}Fe8​ molecule where magnetization jumps are known to occur at discrete magnetic-field values. We found energy bursts each time the molecule undergoes a magnetization jump, confirming their quantum nature. A series of tests indicated that photons carry out the energy and that indeed these photons obey the elementary conditions for super-radiance.
We study the dynamics of molecular nanomagnets through a fully quantum mechanical model describing high-spin and high-anisotropy magnetic molecules subjected to a time-dependent magnetic field along the quantization axis, which continuously inverts the population of spin states. Crystals of molecular nanomagnets placed inside a resonant cavity interact with a quantized electromagnetic field. Relaxation of excited states takes place by means of spin-photon interaction, allowing stimulated emission of radiation and creating a maser effect.
Abstract We study a superradiant quantum phase transition in the model of triangular molecular magnets coupled to the electric component of a microwave cavity field. The transition occurs when the coupling strength exceeds a critical value, d c , which, in sharp contrast to the standard two-level emitters, can be tuned by an external magnetic field. In addition to emitted radiation, the molecules develop an in-plane electric dipole moment at the transition. We estimate that the transition can be detected in state-of-the-art microwave cavities if their electric field couples to a crystal containing a sufficient number of oriented molecules.
Forbidden transitions between energy levels typically involve violation of selection rules imposed by symmetry and/or conservation laws. A nanomagnet tunneling between up and down states violates angular momentum conservation because of broken rotational symmetry. Here we report observations of highly forbidden transitions between spin states in a Ni_{4} single-molecule magnet in which a single photon can induce the spin to change by several times ℏ, nearly reversing the direction of the spin. These observations are understood as tunneling-assisted transitions that lift the standard Δm=±1 selection rule for single-photon transitions. These transitions are observed at low applied fields, where tunneling is dominated by the molecule's intrinsic anisotropy and the field acts as a perturbation. Such transitions can be exploited to create macroscopic superposition states that are not typically accessible through single-photon Δm=±1 transitions.
We present a microscopic model for the so-called quantum jumps in three-level atoms with one transition between two levels being strongly driven and the third level being metastable. Our model is based on calculating the elementary probability density P(0,t)(t1, … , t n ) which gives the probability density that exactly n photons are emitted at times t1, … , t n by the atom in the time interval (0, t) on the strong transition. This enables us to calculate the conditional probabilities c ˜ ( τ ) that given a photon has emitted at τ = 0 the next photon emission occurs at time τ. This quantity is shown to be the sum of two exponentials which for sufficient differetial in the time scales describe the periods of light and darkness. Using this conditional probability it is possible to numerically simulate the individual photon emissions.