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arXiv:1110.1473

Dynamical Decoupling of Spin-Clusters using Solid State NMR

Abhishek Shukla, T. S. Mahesh

Published Oct 7, 2011• 2 citations
arXivHTMLPDF

Abstract

In this work we experimentally study the efficiency of various dynamical decoupling sequences for suppressing decoherence of single as well as multiple quantum coherences on large spin-clusters. The system involves crystallites of a powdered sample containing a large number of molecular protons interacting via long-range dipole-dipole interaction. The multiple quantum coherences are prepared by progressively creating correlations in the spin lattice using standard pulse sequences implementing two-quantum average Hamiltonian. The spin system is then subjected to various dynamical decoupling sequences, followed by conversion into observable single quantum coherence by using time-reversal sequence. The experiments reveal superior performance of the recently introduced RUDD sequences in suppressing the decoherence.

DOI
10.48550/arxiv.1110.1473

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In this work we experimentally study the efficiency of various dynamical decoupling sequences for suppressing decoherence of single as well as multiple quantum coherences on large spin-clusters. The system involves crystallites of a powdered sample containing a large number of molecular protons interacting via long-range dipole-dipole interaction. The multiple quantum coherences are prepared by progressively creating correlations in the spin lattice using standard pulse sequences implementing two-quantum average Hamiltonian. The spin system is then subjected to various dynamical decoupling sequences, followed by conversion into observable single quantum coherence by using time-reversal sequence. The experiments reveal superior performance of the recently introduced RUDD sequences in suppressing the decoherence.
Dense spin ensembles in solids present a natural platform for studying quantum many-body dynamics. Multiple-pulse coherent control can be used to manipulate the magnetic dipolar interaction between the spins to engineer their dynamics. Here, we investigate the performance of a series of well-known pulse sequences that aim to suppress interspin dipolar couplings. We use a combination of numerical simulations and solid-state nuclear magnetic resonance experiments on adamantane to evaluate and compare sequence performance. We study the role of sequence parameters like interpulse delays and resonance offsets. Disagreements between experiments and theory are typically explained by the presence of control errors and experimental nonidealities. The simulations allow us to explore the influence of factors such as finite pulse widths, rotation errors, and phase transient errors. We also investigate the role of local disorder and establish that it is, perhaps unsurprisingly, a distinguishing factor in the decoupling efficiency of spectroscopic sequences (that preserve Hamiltonian terms proportional to S z ) and time-suspension sequences (which refocus all terms in the internal Hamiltonian). We discuss our findings in the context of previously known analytical results from average Hamiltonian theory. Finally, we explore the ability of time-suspension sequences to protect multispin correlations in the system.
One of the fundamental problems of chemistry is the difficulty in determining full quantum mechanical descriptions of molecules. Molecules contain many degrees of freedom and as a result the classical description scales factorially with the number of electrons. One way to overcome this mismatch between quantum and classical pictures is to use one quantum system, a quantum computer, to simulate another. Quantum computation is based upon a two-level system, a qubit, which is analogous to a bit in classical computation. Unlike a classical bit, a qubit can exist in a superposition of quantum states. The interaction between a quantum system and its environment results in the decay of the superposition state of the system into a probability density of classical states [1]. This is known as decoherence. A realistic quantum computer requires qubits with long coherence times; with respect to the achievable gating times, for a formal relation refer to section 1.2.2. The spin echo effect in nuclear magnetic resonance (NMR) offers a way to increase the coherence time of a qubit and has been studied as a way to mitigate decoherence in quantum computation[2][3]. By applying an appropriate Π pulse to a system under the influence of a large external field, as in NMR, the interaction term of the Hamiltonian between the qubit and environment can be eliminated[3][4]. Periodic implementation of such pulses is known as periodic dynamic decoupling (PDD). Similar to PDD, concatenated dynamic decoupling (CDD) is a periodic pulse sequence which removes the interaction term of the Hamiltonian, however in CDD pulse sequences are recursively embedded within the overall pulse train. Such pulse sequences have been shown theoretically to work for model quantum systems such as GaAs quantum dots, and theoretically such pulse sequences vastly improve the coherence time of a qubit [5]. There have been many calculations showing that by progressively increasing the number of concatenated pulse sequences increasingly longer coherence times can be achieved [6][7]. These techniques have not been tested in the laboratory and experimental implementation of these promising techniques motivates current research. There also continues to be extensive work on developing novel pulse sequences which may improve coherence times even further. The goal of this research is to experimentally determine the coherence times which can be achieved with a trapped calcium atom by applying these pulse sequences.
Avoiding the loss of coherence of quantum mechanical states is an important prerequisite for quantum information processing. Dynamical decoupling (DD) is one of the most effective experimental methods for maintaining coherence, especially when one can access only the qubit system and not its environment (bath). It involves the application of pulses to the system whose net effect is a reversal of the system-environment interaction. In any real system, however, the environment is not static, and therefore the reversal of the system-environment interaction becomes imperfect if the spacing between refocusing pulses becomes comparable to or longer than the correlation time of the environment. The efficiency of the refocusing improves therefore if the spacing between the pulses is reduced. Here, we quantify the efficiency of different DD sequences in preserving different quantum states. We use 13C^{13}\mathrm{C}13C nuclear spins as qubits and an environment of 1H^{1}\mathrm{H}1H nuclear spins as the environment, which couples to the qubit via magnetic dipole-dipole couplings. Strong dipole-dipole couplings between the proton spins result in a rapidly fluctuating environment with a correlation time of the order of 100 $\ensuremath{\mu}$s. Our experimental results show that short delays between the pulses yield better performance if they are compared with the bath correlation time. However, as the pulse spacing becomes shorter than the bath correlation time, an optimum is reached. For even shorter delays, the pulse imperfections dominate over the decoherence losses and cause the quantum state to decay.
We present an improved approach for the study of the evolution of spin correlations and decoherence in multiple quantum nuclear magnetic resonance experiments. The infinite system, constituted by the protons of a polycrystalline adamantane sample, evolves under a double quantum Hamiltonian. The distribution of multiple quantum coherence orders is represented by a contribution of spin clusters with different sizes that exchange spins, increasing their size with the evolution time. A cluster with nearly exponential growth at all times is observed, in agreement with previous models. Remarkably, a small cluster that stabilizes in a size corresponding to 18 correlated spins is revealed. In addition, by performing a renormalization of the obtained data with the experimental Loschmidt echo, the contribution of the different clusters to the observable signal is determined. This procedure accounts for the effect of decoherence on the evolution of the system, and allows setting the range of confidence of the experimental data. Our analysis confirms the natural hint that, correlated states involving higher coherence orders are far more sensitive to the uncontrolled decoherent interactions, than those involving lower orders.
Dynamical decoupling (DD) is a well-known open-loop protocol for suppressing unwanted interactions in a quantum system, thereby drastically extending the coherence time of useful quantum states. In the original framework of evolution symmetrization, a DD sequence was shown to enforce a symmetry on the unwanted Hamiltonian, thereby suppressing it if the symmetry was inaccessible. In this work, we show how symmetries already present in the undesired Hamiltonian can be harnessed to reduce the complexity of decoupling sequences and to construct nested protocols that correct dominant errors at shorter timescales, using the factorization of DD symmetry groups into a product of its subgroups. We provide many relevant examples in various spin systems, using the Majorana constellation and point-group factorization to identify and exploit symmetries in the interaction Hamiltonian. Our framework recovers tailored pulse sequences developed in the context of NMR, including the classical Lee-Goldburg protocol, and further produces novel short and robust sequences capable of suppressing on-site disorder, dipole-dipole interactions, and more exotic many-body interactions in spin ensembles.
We investigate analytically and numerically the multiple-quantum (MQ) NMR dynamics in systems of nuclear spins 1∕21∕21∕2 coupled by the dipole-dipole interactions in the case of the dipolar ordered initial state. We suggest two different methods of MQ NMR. One of them is based on the measurement of the dipolar temperature in the quasiequilibrium state which is established after the time of order ${\ensuremath{\omega}}_{\mathit{loc}}^{\ensuremath{-}1}$ (${\ensuremath{\omega}}_{\mathit{loc}}$ is the dipolar local field) after the MQ NMR experiment. The other method uses an additional resonance ${(\ensuremath{\pi}∕4)}_{y}$ pulse after the preparation period of the standard MQ NMR experiment in solids. Many-spin clusters and correlations are created faster in such experiments than in the usual MQ NMR experiments and can be used for the investigation of many-spin dynamics of nuclear spins in solids.