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Kinetics the proliferation of correlations in multiple quantum NMR spectroscopy

Valeria L. Bodneva

Published Jan 1, 2025• 0 citations
Publisher

Abstract

It is shown that the number of spins in clusters of coherently correlated states arising under conditions of multiplequantum NMR – spectroscopy in a solid increases exponentially with time. The Smolukhovsky equation was used to study the above processes. Possible processes of cluster degradation were not taken into account. The results obtained are in good agreement with the experimental data, at least up to about 105 spins in the cluster.

DOI
10.7868/s3034612625010026

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It is shown that the number of spins in clusters of coherently correlated states arising under conditions of multiplequantum NMR – spectroscopy in a solid increases exponentially with time. The Smolukhovsky equation was used to study the above processes. Possible processes of cluster degradation were not taken into account. The results obtained are in good agreement with the experimental data, at least up to about 105 spins in the cluster.
Multiple-quantum (MQ) solid-state NMR spectroscopy allows the growth of multiple-spin correlations and, thus, the spreading of quantum information in the object under study to be observed. Recently, in [11] it was proposed to control this process through a controlled perturbation added to the effective Hamiltonian that causes degradation of correlated spin clusters with a rate determined by the number of spins K in a cluster. However, this perturbation can also lead to degradation whose rate is determined by the coherence order M. In this paper, to investigate the influence of a small added perturbation, we used an expansion into orthogonal operators that allowed the cluster size distribution to be taken into account. In our calculations we realized a simple model with known amplitudes of the expansion into a complete set of orthogonal operators in the absence of a perturbation. We performed numerical calculations of the “preparation time” dependences of the MQ spectra, their second moments, and the coherence orders at which the MQ spectra decrease by a factor of e as well as the average correlated spin cluster sizes Kˉ\bar {K}Kˉ . The coherence-order-dependent contribution to the degradation is shown to change the shape of the MQ spectrum. In particular, as the preparation time increases, the MQ spectrum can be stabilized, while the growth of Kˉ\bar {K}Kˉ is retained. Due to the change in the shape of the MQ spectrum, the relations of its characteristics to the number Kˉ\bar {K}Kˉ change compared to those for the Gaussian function (traditionally used to process the experiments). These changes should be taken into account when studying the spreading of quantum information through MQ spectroscopy.
Abstract On the basis of the earlier developed statistical theory of the growth of the effective size of correlated clusters (the number of correlated spins), an expression for the shape of the multiple-quantum (MQ) NMR spectrum is obtained that takes into account the loss of coherence in a spin system due, for example, to the controlled intervention of the experimenter. It is shown that the scrambling and decoherence processes in the MQ spectrum of the multiparticle system of a solid are not separated, unlike the corresponding spectra of some large isolated molecules [27] in a solution. The relations obtained allow one to extract the necessary information about the above processes (scrambling and decoherence) from the dependence of the MQ spectra on experimental parameters.
A change in the time dependence of the second moment of the distribution of intensities of coherences with various orders in the spectrum of multiple-quantum NMR in a solid at the inclusion of an inhomogeneous magnetic field in the effective interaction is studied. Both the secular dipole–dipole and nonspecular twoquantum interactions are considered as nucleus–nucleus interactions, which correspond to traditional experimental realizations. It is shown that, with an increase in the magnitude of the inhomogeneous field, an exponential increase in the second moment of multiple-quantum NMR with time changes to a power-law increase. The results obtained in this work indicate that this second moment, which determines the average number of dynamically correlated spins, can be used as a convenient characteristic for studying a transition to a many-body localized state.
Among the most important parameters for the usefulness of quantum computers are the size of the quantum register and the decoherence time for the quantum information. The decoherence time is expected to get shorter with the number of correlated qubits, but experimental data are only available for small numbers of qubits. Solid-state nuclear magnetic resonance allows one to correlate large numbers of qubits (several hundred) and measure their decoherence rates. We use a modified magnetic dipole-dipole interaction to correlate the proton spins in a solid sample and observe the decay of the resulting highly correlated states. By systematically varying the number of correlated spins, we measure the increase of the decoherence rate with the size of the quantum register.
Multiple quantum (MQ) NMR is an effective tool for the generation of a large cluster of correlated particles, which, in turn, represent a basis for quantum information processing devices. Studying the available exactly solvable models clarifies many aspects of the quantum information. In this study, we consider two exactly solvable models in the MQ NMR experiment: (i) the isolated system of two spin-1/2 particles (dimers) and (ii) the large system of equivalent spin-1/2 particles in a nanopore. The former model is used to describe the quantum correlations and their relations with the MQ NMR coherences, whereas the latter helps one to model the creation and decay of large clusters of correlated particles.
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.