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arXiv:cond-mat/9906375 · Physical Review Letters

Mechanisms of Decoherence in Weakly Anisotropic Molecular Magnets

V. V. Dobrovitski, Mikhail I. Katsnelson, B. N. Harmon

Published Apr 10, 2000• 54 citations
arXivHTMLPDF

Abstract

Decoherence mechanisms in crystals of weakly anisotropic magnetic molecules, such as V15, are studied. We show that an important decohering factor is the rapid thermal fluctuation of dipolar interactions between magnetic molecules. A model is proposed to describe the influence of this source of decoherence. Based on the exact solution of this model, we show that at relatively high temperatures, about 0.5 K, the quantum coherence in a V15 molecule is not suppressed and, in principle, can be detected experimentally. Therefore, these molecules may be suitable prototype systems for study of physical processes taking place in quantum computers.

DOI
10.1103/physrevlett.84.3458

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Decoherence mechanisms in crystals of weakly anisotropic magnetic molecules, such as V15, are studied. We show that an important decohering factor is the rapid thermal fluctuation of dipolar interactions between magnetic molecules. A model is proposed to describe the influence of this source of decoherence. Based on the exact solution of this model, we show that at relatively high temperatures, about 0.5 K, the quantum coherence in a V15 molecule is not suppressed and, in principle, can be detected experimentally. Therefore, these molecules may be suitable prototype systems for study of physical processes taking place in quantum computers.
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 measured Rabi oscillations of an ensemble of spins (here the spins 3/2 of the V15 single molecular magnet) are strongly damped by the excitation ac-field. The corresponding decoherence mechanism is attributed to an electromagnetic noise created by the dipolar spin-bath, inhomogeneously driven by the microwave field. Decoherence by electronic and nuclear spin-baths express themselves very differently vs microwave power. This decoherence mechanism should apply to all types of weakly interacting ensembles of qubits, beyond magnetism.
Abstract : With the production of polar molecules in the quantum regime, long-range dipolar interactions are expected to facilitate understanding of strongly interacting many-body quantum systems and to realize lattice spin models for exploring quantum magnetism. In ordinary atomic systems, where contact interactions require wavefunction overlap, effective spin interactions on a lattice can be mediated by tunnelling, through a process referred to as superexchange; however, the coupling is relatively weak and is limited to nearest-neighbour interactions. In contrast, dipolar interactions exist even in the absence of tunnelling and extend beyond nearest neighbours. This allows coherent spin dynamics to persist even for gases with relatively high entropy and low lattice filling. Measured effects of dipolar interactions in ultracold molecular gases have been limited to the modification of inelastic collisions and chemical reactions. Here we use dipolar interactions of polar molecules pinned in a three-dimensional optical lattice to realize a lattice spin model. Spin is encoded in rotational states of molecules that are prepared and probed by microwaves. Resonant exchange of rotational angular momentum between two molecules realizes a spin-exchange interaction. The dipolar interactions are apparent in the evolution of the spin coherence, which shows oscillations in addition to an overall decay of the coherence. The frequency of these oscillations, the strong dependence of the spin coherence time on the lattice filling factor and the effect of a multipulse sequence designed to reverse dynamics due to two-body exchange interactions all provide evidence of dipolar interactions. Furthermore, we demonstrate the suppression of loss in weak lattices due to a continuous quantum Zeno mechanism. Measurements of these tunnelling-induced losses allow us to determine the lattice filling factor independently.
Single molecule magnets are novel mesoscopic materials exhibiting both classical and quantum properties. Revealing the decoherence and entanglement mechanisms in these systems is crucial for the applications in quantum information technologies. In this thesis, quantum tunneling of magnetization is studied in single molecule magnet dimer [Mn4]2. Motivated by the recent experiments demanding the modification of the current theories, phonon mediated spin bath decoherence model is proposed. In the first part of the thesis, the magnetization of the [Mn4]2 dimer under external magnetic field is investigated. Alternative entangled spin states involved in quantum tunnelings are identified by means of the exact solution of the Schrödinger equation and the Landau-Zener-Stückelberg method. Later, a decoherence model is introduced in which the interaction between the single molecule magnet (central spin) and spin bath is mediated by phonons in a coherent state or thermal distribution. It is observed that the decoherence factor decays in a Gaussian fashion and it becomes independent of the phonon frequencies at short times for coherent states and low temperature thermal distribution. In the former case, if the phonon energies are much larger than spin-phonon coupling or bath spins are fully polarized, decoherence time becomes independent of the initial phonon state. For the thermal state case, phonons play more important role in decoherence with increasing temperature. Possible effects of the temperature on spin bath contribution to decoherence is discussed. Then, the effect of entangled environment on decoherence is analyzed. Entanglement within environment is shown to reduce the decoherence of central spin. Also, the entanglement dynamics of the central bipartite spin system is studied. Classification of the Bell states is examined for common spin bath, and separate spin baths. Last part of the thesis is the analysis of dephasing in entangled qutrits (three level quantum systems) under the classical noise, and quantum decoherence. Density matrix formalism is shown to give equivalent results for both cases. For common and separate baths, robust and fragile Bell-like qutrit states were determined, and Horodecki's bound entangled state is shown to be more robust to decoherence in the latter case.
Spin-phonon interactions are known to drive magnetic relaxation in solid-state systems but are generally overlooked as a contribution to spin decoherence through dephasing. Here, we extend quantum master equations to account for coherence terms and describe the full effect of up to two-phonon processes on spin dynamics. We implement this method fully ab initio for a molecule with large magnetization blocking temperature and show that, although strong axial magnetic anisotropy ensures slow magnetic relaxation approaching seconds at 77 kelvins, the superposition of Kramers doublets is coherent for less than 10 nanoseconds due to a two-phonon pure dephasing mechanism. This process, in principle, applies to any quantum system interacting with a thermal bath of phonons, advancing our understanding of quantum decoherence in solid-state systems.
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.