NMR spectroscopy relies on the fact that nuclear spin ensembles in bulk samples under ambient conditions sustain quantum superpositions for durations long enough to implement intricate quantum dynamics. The discovery of long-lived nuclear spin order further enhanced the scope of NMR experiments paving the way for novel applications. In this chapter, we look at the long-lived singlet state (LLSS) from the perspectives of NMR quantum information, wherein the two Zeeman eigenstates of a spin-1/2 nucleus are treated as 0 and 1 states of a quantum bit. In particular, we discuss the following topics: density matrix tomography of the LLSS, initialization of a quantum register via the LLSS, noise spectroscopy of the LLSS, and numerical optimization methods to prepare the LLSS.
Algorithmic cooling methods manipulate an open quantum system in order to lower its temperature below that of the environment. We achieve significant cooling of an ensemble of nuclear spin-pair systems by exploiting the long-lived nuclear singlet state, which is an antisymmetric quantum superposition of the “up” and “down” Zeeman states. The effect is demonstrated by nuclear magnetic resonance experiments on a molecular system containing a coupled pair of near-equivalent 13C nuclei. The populations of the system are subjected to a repeating sequence of cyclic permutations separated by relaxation intervals. The long-lived nuclear singlet order is pumped well beyond the unitary limit. The pumped singlet order is converted into nuclear magnetization which is enhanced by 21% relative to its thermal equilibrium value.
Delocalized long-lived states (LLSs) and collective zero-quantum long-lived coherences (LLCs) in aliphatic chains provide a promising route for preserving nuclear spin order with lifetimes that exceed the conventional
T1 and
T2 relaxation times, respectively. Their extended lifetimes make them attractive for applications including hyperpolarization storage, ligand-observed drug screening based on the loss of longevity upon binding to a target protein, and quantum information processing exploiting the collective properties of many-body spin systems. Although LLSs and LLCs have been observed experimentally in methylene networks, their origin and general structure in chains of arbitrary length have remained unclear. Here we show that these relaxation-protected modes follow directly from Redfield relaxation theory. Specifically, we construct the long-lived subspace, i.e., the zero-eigenvalue subspace of the relaxation superoperator associated with the dominant intra-pair dipole--dipole relaxation mechanism. The long-lived subspace contains
2N−1 independent non-trivial operators, which excludes the identity operator, where
N>1 is the number of
−CH2− groups in the chain. In achiral molecules, conservation of the global intra-pair permutation parity restricts experimental access to at most
2N−2 of these operators, whereas in chiral molecules this parity is not conserved, making up to
2N−1 long-lived operators accessible. We further develop a general framework for constructing both LLSs and LLCs in aliphatic chains containing an arbitrary number of
−CH2− groups in achiral molecules, and illustrate the approach explicitly for chains with
N=2, 3, and 4 methylene groups.
Nuclear Magnetic Resonance (NMR) forms a natural test-bed to perform quantum information processing (QIP) and has so far proven to be one of the most successful quantum information processors. The nuclear spins in a molecule treated as quantum bits or qubits which are the basic building blocks of a quantum computer. The development of NMR over half a century puts it in a platform where we can utilize its excellent control techniques over an ensemble of spin systems and perform quantum computation in a highly controlled way. Apart from a successful quantum information processor, NMR is also a highly powerful quantum platform where many of the potentially challenging quantum mechanical experiments can be performed.
Dynamical polarization of nuclear spin ensembles is of central importance for magnetic resonance studies, precision sensing and for applications in quantum information theory. Here we propose a scheme to generate long-lived singlet pairs in an unpolarized nuclear spin ensemble which is dipolar coupled to the electron spins of a Nitrogen Vacancy center in diamond. The quantum mechanical back-action induced by frequent spin-selective readout of the NV centers allows the nuclear spins to pair up into maximally entangled singlet pairs. Counterintuitively, the robustness of the pair formation to dephasing noise improves with increasing size of the spin ensemble. We also show how the paired nuclear spin state allows for enhanced sensing capabilities of NV centers in diamond.
Rapid developments in quantum information processing have been made, and remarkable achievements have been obtained in recent years, both in theory and experiments. Coherent control of nuclear spin dynamics is a powerful tool for the experimental implementation of quantum schemes in liquid and solid nuclear magnetic resonance (NMR) system, especially in liquid-state NMR. Compared with other quantum information processing systems, the NMR platform has the advantages such as the long coherence time, the precise manipulation, and well-developed quantum control techniques, which make it possible to accurately control a quantum system with up to 12-qubits. Extensive applications of liquid-state NMR spectroscopy in quantum information processing such as quantum communication, quantum computing, and quantum simulation have been thoroughly studied over half a century. This article introduces the general principles of NMR quantum information processing, and reviews the new-developed techniques. The review will also include the recent achievements of the experimental realization of quantum algorithms for machine learning, quantum simulations for high energy physics, and topological order in NMR. We also discuss the limitation and prospect of liquid-state NMR spectroscopy and the solid-state NMR systems as quantum computing in the article.