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arXiv:2602.05661

Investigations on Quantum Correlations and Open Quantum System Dynamics Through Nuclear Spins

Arijit Chatterjee

quant-phSubmitted Feb 5, 2026• Announced Feb 6, 2026• 0 citations
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Abstract

Nuclear spins provide an ideal platform for studying quantum correlations and open quantum system dynamics across diverse areas, including quantum information, quantum foundations, and many-body physics. This is enabled by their long longitudinal (T1) and transverse (T2) coherence times and precise control using radio frequency pulses. In this thesis, I present my work using nuclear spins to explore these themes. First, I study temporal quantum correlations quantified by the Leggett Garg inequality (LGI) for a qubit evolving under a superposition of unitary operators. Using a three qubit quantum register, we experimentally realized superposed unitaries and observed LGI violations exceeding the maximal quantum bound of 1.5, indicating enhanced non-classicality. Notably, this superposed unitary dynamics also showed improved robustness against decoherence. Next, I investigate Lee Yang zeros, which are zeros of the partition function in the complex plane that reveal thermodynamic behavior near criticality. We proposed and experimentally demonstrated a method to determine the full set of Lee Yang zeros of an asymmetric Ising model using a single quantum probe in a three-qubit nuclear spin register. We further showed that the mutual information between the probe and system peaks at times corresponding to these zeros. I then report our study of the quantum Mpemba effect in nuclear spin relaxation, where systems farther from equilibrium can relax faster than those closer to steady state, verified both theoretically and experimentally using NMR. Finally, I discuss our work on entanglement localization and delocalization induced by local interactions, leading to an apparent violation of the quantum data processing inequality. We showed that this violation is only apparent by constructing a completely positive and trace preserving map describing the dynamics.

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PhD thesis

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Nuclear spins provide an ideal platform for studying quantum correlations and open quantum system dynamics across diverse areas, including quantum information, quantum foundations, and many-body physics. This is enabled by their long longitudinal (T1) and transverse (T2) coherence times and precise control using radio frequency pulses. In this thesis, I present my work using nuclear spins to explore these themes.
First, I study temporal quantum correlations quantified by the Leggett Garg inequality (LGI) for a qubit evolving under a superposition of unitary operators. Using a three qubit quantum register, we experimentally realized superposed unitaries and observed LGI violations exceeding the maximal quantum bound of 1.5, indicating enhanced non-classicality. Notably, this superposed unitary dynamics also showed improved robustness against decoherence.
Next, I investigate Lee Yang zeros, which are zeros of the partition function in the complex plane that reveal thermodynamic behavior near criticality. We proposed and experimentally demonstrated a method to determine the full set of Lee Yang zeros of an asymmetric Ising model using a single quantum probe in a three-qubit nuclear spin register. We further showed that the mutual information between the probe and system peaks at times corresponding to these zeros.
I then report our study of the quantum Mpemba effect in nuclear spin relaxation, where systems farther from equilibrium can relax faster than those closer to steady state, verified both theoretically and experimentally using NMR. Finally, I discuss our work on entanglement localization and delocalization induced by local interactions, leading to an apparent violation of the quantum data processing inequality. We showed that this violation is only apparent by constructing a completely positive and trace preserving map describing the dynamics.
In this Thesis, we study open quantum spin systems from di↵erent perspectives.The first part is motivated by technological challenges of quantum computation.An important building block for quantum computation and quantum communication networks is an interface between material qubits for storage and data processing and travelling photonic qubits for communication.We propose the realisation of a quantum interface between a travelling-wave light field and the nuclear spins in a quantum dot strongly coupled to a cavity.Our scheme is robust against cavity decay as it uses the decay of the cavity to achieve the coupling between nuclear spins and the travelling-wave light fields.A prerequiste for such a quantum interface is a highly polarized ensemble of nuclear spins.High polarization of the nuclear spin ensemble is moreover highly desirable as it protects the potential electron spin qubit from decoherence.Here we present the theoretical description of an experiment in which highly asymmetric dynamic nuclear spin pumping is observed in a single self-assembled InGaAs quantum dot.The second part of this Thesis is devoted to fundamental studies of dissipative spin systems.We study general one-dimensional spin chains under dissipation and propose a scheme to realize a quantum spin system using ultracold atoms in an optical lattice in which both coherent interaction and dissipation can be engineered and controlled.This system enables the study of non-equilibrium and steady state physics of open and driven spin systems.We find, that the steady state expectation values of di↵erent spin models exhibit discontinuous behaviour at degeneracy points of the Hamiltonian in the limit of weak dissipation.This e↵ect can be used to dissipatively probe the spectrum of the Hamiltonian.We moreover study spin models under the aspect of state preparation and show that dissipation drives certain spin models into highly entangled state.Finally,
Quantum simulations, where controllable quantum systems are used to simulate other quantum systems, originally proposed by Richard Feynman, are one of the most remarkable applications of quantum information science. Compared to computation, quantum simulations require much less number of qubits for the m to be practical. In the work described in this thesis, we have performed a few quantum simulations of small quantum systems using Nuclear Magnetic Resonance(NMR) techniques. These simulations have been used to experimentally demonstrate the underlying interesting quantum protocols. All the experiments presented have been carried out using liquid-state or liquid crystal NMR. Numerical pulse optimization techniques have been utilized in some of the experiments, to achieve better control over the spin systems. The first chapter contains “Introduction” to quantum information processing, NMR, and numerical pulse optimization techniques. In chapter 2, we describe quantum simulation of a 3-spin Heisenberg-XY spin chain having only nearest neighbour interactions. Recently, spin chains having pre-engineered short-range interactions have been proposed to efficiently transfer quantum information between different parts of a quantum information processor. Other important proposals involving these spin chains include generating entangled states and universal quantum computation. However, such engineered interactions do not occur naturally in any system. In such a scenario, the experimental viability of these proposals can be tested by simulating the spin chains in other controllable quantum systems. In this work, we first theoretically study the time evolution of bipartite and tripartite entanglement measures for a 3-spin open ended XY spin chain. Then, by simulating the XY interactions in a 3-spin nuclear spin system, we experimentally generate, (i)a bipartite maximally(pseudo-)entangled state(Bell state) between end qubits, and(ii) multipartite(pseudo-)entangled states(Wand GHZ states),starting from separable pseudo-pure states. Bell state has been generated by using only the natural unitary evolution of the XY spin chain. W-state and GHZ-state have been generated by applying a single-qubit rotation to the second qubit, and a global rotation of all the three qubits respectively after the unitary evolution of the spin chain. In chapter 3, we simulate a 3-spin quantum transverse Ising spin system in a triangular configuration, and show that multipartite quantum correlations can be used to distinguish between the frustrated and non-frustrated regimes in the ground state of this spin system. The ground state of the spin system has been prepared by using adiabatic state preparation method. Gradient ascent pulse engineering technique has been utilized to efficiently realize the adiabatic evolution of the spin system. To analyse the experimental ground state of the system, we employ two different multipartite quantum correlation measures, generated from monogamy studies of bipartite quantum correlations. Chapter 4 contains a digital…
The work presented in this thesis is divided into two main parts: strong zero modes in quantum spin chains with open boundaries and large deviations in classical spin systems. The results concerning the strong zero modes are presented in chapters 2 and 3, while chapter 4 contains the results about large deviations in systems of many, but independent, classical degrees of freedom. These two distinct classes of problems in spin chains are both about aspects of slow relaxation to equilibrium in many-body systems. Nowadays slow dynamics and non-ergodicity in many-body quantum systems are receiving much attention due to their notable technological potential for storing and processing, for very long times, the quantum information encoded in boundary degrees of freedom. In the first part of the work presented in this thesis we mainly focus on quantum spin chains with open boundaries, which can display coherence times for edge spins, that diverge with the system size, as a consequence of the emergence, in the thermodynamic limit, of conserved local quantities, called strong zero modes. First, we discuss the fate of these coherence times when dynamics becomes dissipative. Understanding the behavior of these long correlation times in open quantum systems, undergoing Markovian (memoryless) dynamics, would allow for the possibility of exploiting the protected information encoded in the boundary spins for applications in quantum devices in realistic non-equilibrium settings. Second, we study one possible simple generalization of the transverse field Ising model to a class of ladder spin systems with plaquette interactions in the presence of a transverse field. Also for these systems one can explicitly construct the strong zero mode operators and understand the behavior of the consequential long coherence times for the edge degrees of freedom under isolated (unitary) dynamics. This is possible because the models we consider, while appearing complex superficially, can be brought to simple forms by exploiting an extensive number of conserved quantities they possess. The results presented in chapters 2 and 3 are closely related, even if they focus on different models and investigate different aspects of their dynamics. Nevertheless, the underlying concept they are based on is the same one, that is, an eigenstate phase transition for the strong zero modes that has interesting consequences for the full energy spectrum. In the second part of the thesis we focus on a different type of phase transitions. Here we address the issue of dynamical large deviation phase transitions from a disordered phase to an ordered one, in classical systems which consist in a collection of independent Ising spins evolving stochastically. Surprisingly, by reweighing trajectories accordingly to a certain type of time-integrated observable, even a system of independently evolving spins can display some critical behavior, at the fluctuation level, in trajectory space in the large size and long time limit. By making use of the tilted generator techniques we study the statistics of two particular time-integrated observables. Their associated tilted generators have an exact Kramers-Wannier duality and they look like, up to a sign and an additive constant, some specific well known quantum Hamiltonians. In this sense, the dynamical large deviation phase transitions we observe in these classical stochastic systems translate in ground state quantum phase transitions taking place at the self dual point of the tilted generators we study.
Solid-state nuclear magnetic resonance (NMR) has emerged as an important technique for material characterization, finding extensive applications across a diverse range of disciplines including physics, materials science, chemistry, and biology. Its utility stems from the ability to probe the local atomic environments and molecular dynamics within solid materials, which provides information on the composition of the material. In recent years, the scope of solid-state NMR has expanded into the realm of quantum information science and technology, where its abundant many-body interactions pulse control methodologies make it have significant research value and application potential. This paper offers a comprehensive overview of the research objects and theoretical underpinnings of solid-state NMR, delving into the critical nuclear spin interaction mechanisms and their corresponding Hamiltonian forms. These interactions, which include dipolar coupling, chemical shift anisotropy, and quadrupolar interactions, are fundamental to the interpretation of NMR spectra and the understanding of material properties at the atomic level. Moreover, the paper introduces typical dynamical control methods employed in the manipulation of solid-state nuclear spins. Techniques such as dynamical decoupling, which mitigates the effects of spin-spin interactions to extend coherence times, and magic-angle spinning, which averages out anisotropic interactions to yield high-resolution spectra. These methods are essential for enhancing the sensitivity and resolution of NMR experiments, enabling the extraction of detailed structural and dynamic information from complex materials. Then we introduce some recent advancements in quantum control based on solid-state NMR, such as nuclear spin polarization enhancement techniques, which include dynamic nuclear polarization (DNP) and cross polarization (CP), significantly boost the sensitivity of NMR measurements. Additionally, the control techniques of Floquet average Hamiltonians are mentioned, showcasing their role in the precise manipulation of quantum states and the realization of quantum dynamics. Finally, the paper presents a series of seminal research works that illustrate the application of solid-state NMR quantum control technologies in the field of quantum simulation. These studies demonstrate how solid-state NMR can be leveraged to simulate and investigate quantum many-body systems, providing valuable insights into quantum phase transitions, entanglement dynamics, and other phenomena relevant to quantum information science. By bridging the gap between fundamental research and practical applications, solid-state NMR continues to play a crucial role in advancing our understanding of quantum materials and technologies.
Quantum theory contravenes classical macrorealism by allowing a system to be in a superposition of two or more physically distinct states, producing physical consequences radically different from that of classical physics. We show that a system, upon subjecting to transform under superposition of unitary operators, exhibits enhanced non-macrorealistic feature - as quantified by violation of the Leggett-Garg inequality (LGI) beyond the temporal Tsirelson bound. Moreover, this superposition of unitaries also provides robustness against decoherence by allowing the system to violate LGI and thereby retain its non-macrorealistic behavior for a strikingly longer duration. Using an NMR register, we experimentally demonstrate the superposition of unitaries with the help of an ancillary qubit and verify these theoretical predictions.
Quantum simulation platforms such as cold atoms, superconducting circuits, and trapped ions enable the experimental investigation of quantum many-body systems, with important implications for quantum technologies. In this thesis, we investigate how entanglement and correlations develop in such systems and how they can be harnessed both for the theoretical study of models relevant to condensed matter physics and for practical applications in quantum metrology. We begin by focusing on the adiabatic preparation of quantum many-body ground states. In particular, we show that quantum simulators can probe the link between spectral degeneracy and Spontaneous Symmetry Breaking, as pioneered by P.W. Anderson. We prove that odd-sized spin-½ systems exhibiting time-reversal symmetry sustain a net magnetization even away from the thermodynamic limit, thanks to an exact spectral degeneracy. Moreover, the symmetry-broken state exhibits scalable spin squeezing, a key resource for quantum metrology. We then turn to a different paradigm of evolution: quench dynamics. In particular, we show that monitoring the real-time evolution of correlations allows for the experimental measurement of the dispersion relation of fundamental excitations. In the case of two-dimensional long-range ordered systems, such as the dipolar XY model, these excitations are spin waves, leading to sharp features in the evolution of two-point correlation functions. Conversely, in one-dimensional systems, fundamental excitations have a fermionic nature, and their detection requires the measurement of non-local correlation functions. The latter, while inaccessible in condensed matter, are instead well suited to quantum simulators with individually addressable degrees of freedom.