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.
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.
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.
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.
The quantum dynamics of mesoscopic or macroscopic systems is always complicated by their coupling to many `environmental' modes. At low T these environmental effects are dominated by localized modes, such as nuclear and paramagnetic spins, and defects (which also dominate the entropy and specific heat). This environment, at low energies, maps onto a `spin bath' model. This contrasts with `oscillator bath' models (originated by Feynman and Vernon) which describe delocalized environmental modes such as electrons, phonons, photons, magnons, etc. The couplings to N spin bath modes are independent of N (rather than the ~O(1/( N ) 1/2 ) dependence typical of oscillator baths), and often strong. One cannot in general map a spin bath to an oscillator bath (or vice versa); they constitute distinct `universality classes' of quantum environment. We show how the mapping to spin bath models is made, and then discuss several examples in detail, including moving particles, magnetic solitons, nanomagnets, and SQUIDs, coupled to nuclear and paramagnetic spin environments. We then focus on the `central spin' model, which couples a central two-level system to a background spin bath. It is the spin bath analogue of the famous `spin-boson' oscillator model, and describes, e.g., the tunnelling dynamics of nanoscopic and mesoscopic magnets and superconductors. We show how to average over (or `integrate out') spin bath modes, using an operator instanton technique, to find the central spin dynamics. The formal manouevres involve four separate averages - each average corresponds physically to a different `decoherence' mechanism acting on the central spin dynamics. Each environmental spin has its own topological `spin phase', which by interacting with the phase of the central system, decoheres it - this can happen even without dissipation. We give analytic results for the central spin correlation functions, under various conditions. We then describe the application of this theory to magnetic and superconducting systems. Particular attention is given to recent work on tunnelling magnetic macromolecules, where the role of the nuclear spin bath in controlling the tunnelling is very clear; we also discuss other magnetic systems in the quantum regime, and the influence of nuclear and paramagnetic spins on flux dynamics in SQUIDs. Finally, we discuss decoherence mechanisms and coherence experiments in superconductors and magnets. We show that a spin bath environment causes decoherence even in the T 0 limit. Control of this decoherence will be essential in the effort to construct `qubits' for quantum computers.
We study decoherence induced on a two-level system coupled to a one-dimensional quantum spin chain. We consider the cases where the dynamics of the chain is determined by the Ising, XY, or Heisenberg exchange Hamiltonian. This model of quantum baths can be of fundamental importance for the understanding of decoherence in open quantum systems, since it can be experimentally engineered by using atoms in optical lattices. As an example, here we show how to implement a pure dephasing model for a qubit system coupled to an interacting spin bath. We provide results that go beyond the case of a central spin coupled uniformly to all the spins of the bath, in particular showing what happens when the bath enters different phases, or becomes critical; we also study the dependence of the coherence loss on the number of bath spins to which the system is coupled and we describe a coupling-independent regime in which decoherence exhibits universal features, irrespective of the system-environment coupling strength. Finally, we establish a relation between decoherence and entanglement inside the bath. For the Ising and the XY models we are able to give an exact expression for the decay of coherences, while for the Heisenberg bath we resort to the numerical time-dependent density matrix renormalization group.
We consider here the problem of a "central spin", with spin quantum number S≫1, interacting with a set of microscopic spins. Interactions between the microscopic spins are ignored. This model describes magnetic grains or magnetic macromolecules (ferromagnetically or antiferromagnetically ordered) interacting with nuclear spins and with any surrounding paramagnetic electronic spins. It has also been used to describe Si:P near the metal-insulator transition, and quantum spin glasses. In this paper we consider the possible coherent motion of the central spin. We reduce the model to an effective low-energy Hamiltonian, and then calculate the correlation function using instanton methods. The general solution is given for the unbiased case, for all relevant values of the couplings. Under certain conditions, nuclear spin diffusion also plays a role. The results are then used to calculate the spectral absorption for 2 experimental systems, viz., TbFe3 grains, and ferritin molecules. Our results have general implications for the observation of mesoscopic and macroscopic quantum coherence, and for the foundations of quantum mechanics. They show that a spin environment usually has a very destructive effect on coherence, which cannot be understood using the conventional "oscillator bath" models of quantum environments.
Mesoscopic physics is a sub-discipline of condensed-matter physics that focuses on the properties of solids in a size range intermediate between bulk matter and individual atoms. In particular, it is characteristic of a domain where a certain number of interacting objects can easily be tuned between classical and quantum regimes, thus enabling studies at the border of the two. In magnetism, such a tuning was first realized with large-spin magnetic molecules called single-molecule magnets (SMMs) with archetype Mn(12)-ac. In general, the mesoscopic scale can be relatively large (e.g. micrometre-sized superconducting circuits), but, in magnetism, it is much smaller and can reach the atomic scale with rare earth (RE) ions. In all cases, it is shown how quantum relaxation can drastically reduce classical irreversibility. Taking the example of mesoscopic spin systems, the origin of irreversibility is discussed on the basis of the Landau-Zener model. A classical counterpart of this model is described enabling, in particular, intuitive understanding of most aspects of quantum spin dynamics. The spin dynamics of mesoscopic spin systems (SMM or RE systems) becomes coherent if they are well isolated. The study of the damping of their Rabi oscillations gives access to most relevant decoherence mechanisms by different environmental baths, including the electromagnetic bath of microwave excitation. This type of decoherence, clearly seen with spin systems, is easily recovered in quantum simulations. It is also observed with other types of qubits such as a single spin in a quantum dot or a superconducting loop, despite the presence of other competitive decoherence mechanisms. As in the molecular magnet V(15), the leading decoherence terms of superconducting qubits seem to be associated with a non-Markovian channel in which short-living entanglements with distributions of two-level systems (nuclear spins, impurity spins and/or charges) leading to 1/f noise induce τ(1)-like relaxation of S(z) with dissipation to the bath of two-level systems with which they interact most. Finally, let us mention that these experiments on quantum oscillations are, most of the time, performed in the classical regime of Rabi oscillations, suggesting that decoherence mechanisms might also be treated classically.