Multispin correlations and pseudo-thermalization of the transient density matrix in solid-state NMR: free induction decay and magic echo

TL;DR

This paper investigates how magic echo sequences can reverse quantum spin dynamics in solid-state NMR, revealing universal long-time behavior of spin correlations and pseudo-thermalization in the density matrix.

Contribution

It combines analytic, numerical, and experimental approaches to analyze the degradation of magic echoes and the growth of multispin correlations in quantum spin systems.

Findings

Long-time density matrix behavior is universal across initial states.

Low order multispin correlations decay exponentially at the same rate.

The process of correlation growth is constrained by spectral second moment conservation.

Abstract

Quantum unitary evolution typically leads to thermalization of generic interacting many-body systems. There are very few known general methods for reversing this process, and we focus on the magic echo, a radio-frequency pulse sequence known to approximately "rewind" the time evolution of dipolar coupled homonuclear spin systems in a large magnetic field. By combining analytic, numerical, and experimental results we systematically investigate factors leading to the degradation of magic echoes, as observed in reduced revival of mean transverse magnetization. Going beyond the conventional analysis based on mean magnetization we use a phase encoding technique to measure the growth of spin correlations in the density matrix at different points in time following magic echoes of varied durations and compare the results to those obtained during a free induction decay (FID). While considerable differences are documented at short times, the long-time behavior of the density matrix appears to be remarkably universal among the types of initial states considered - simple low order multispin correlations are observed to decay exponentially at the same rate, seeding the onset of increasingly complex high order correlations. This manifestly athermal process is constrained by conservation of the second moment of the spectrum of the density matrix and proceeds indefinitely, assuming unitary dynamics.