We use multiple quantum (MQ) NMR dynamics of a gas of spin-carrying molecules in nanocavities at high and low temperatures for an investigation of many-particle entanglement. A distribution of MQ NMR intensities is obtained at high and low temperatures in a system of 201 spins 1/2. The second moment of the distribution, which provides a lower bound on the quantum Fisher information, sheds light on the many-particle entanglement in the system. The dependence of the many-particle entanglement on the temperature is investigated. Almost all spins are entangled at low temperatures.
We show that it is possible to transfer two-bit information via encoding a single qubit in a conventional nuclear magnetic resonance (NMR) experiment with two very weakly polarized nuclear spins. Nevertheless, the experiment can not be regarded as a demonstration of superdense coding by means of NMR because it is based on the large number of molecules being involved in the ensemble state rather than the entanglement of the NMR states. Following the discussions, an entanglement witness, particularly applicable for NMR, is introduced based on separate and simultaneous measurement of the individu…
Multiple quantum (MQ) NMR with a dipolar ordered initial state opens new possibilities for the exploration of many-spin entanglement. In this paper, we investigate many-spin entanglement in a gas of spin-carrying molecules (atoms) in nanocavities in the conditions of MQ NMR with a dipolar ordered initial state. The second moment of the distribution of the intensities of MQ NMR coherences, which provides a lower bound on the quantum Fisher information, is used for an estimate of the number of the entangled spins. Many-spin entanglement is investigated at different temperatures and different num…
In this essay we discuss the issue of quantum information and recent nuclear magnetic resonance (NMR) experiments. We explain why these experiments should be regarded as quantum information processing (QIP) despite the fact that, in present liquid state NMR experiments, no entanglement is found. We comment on how these experiments contribute to the future of QIP and include a brief discussion on the origin of the power of quantum computers.
Random local measurements have recently been proposed to construct entanglement witnesses and thereby detect the presence of bipartite entanglement. We experimentally demonstrate the efficacy of one such scheme on a two-qubit NMR quantum information processor. We show that a set of three random local measurements suffices to detect the entanglement of a general two-qubit state. We experimentally generate states with different amounts of entanglement, and show that the scheme is able to clearly witness entanglement. We perform complete quantum state tomography for each state and compute state f…
We describe the experimental implementation of a recently proposed quantum algorithm involving quantum entanglement at the level of two qubits using NMR. The algorithm solves a generalisation of the Deutsch problem and distinguishes between even and odd functions using fewer function calls than is possible classically. The manipulation of entangled states of the two qubits is essential here, unlike the Deutsch-Jozsa algorithm and the Grover's search algorithm for two bits.
In recent years, the performance of different entanglement indicators obtained directly from tomograms has been assessed in continuous-variable and hybrid quantum systems. In this paper, we carry out this task in the case of spin systems. We compute the entanglement indicators from actual experimental data obtained from three liquid-state NMR experiments, and compare them with standard entanglement measures calculated from the corresponding density matrices, both experimentally reconstructed and numerically computed. The gross features of entanglement dynamics and spin squeezing properties are…
A scheme to execute an n-bit Deutsch-Jozsa (D-J) algorithm using n qubits has been implemented for up to three qubits on an NMR quantum computer. For the one and two bit Deutsch problem, the qubits do not get entangled, hence the NMR implementation is achieved without using spin-spin interactions. It is for the three bit case, that the manipulation of entangled states becomes essential. The interactions through scalar J-couplings in NMR spin systems have been exploited to implement entangling transformations required for the three bit D-J algorithm.
Quantum correlations in multiple quantum (MQ) NMR experiments are investigated in two-spin systems (dimers). In the initial moment of time one spin is in a pure quantum polarized state and the other spin is in the thermodynamic equilibrium state defined by the temperature of the sample. MQ NMR dynamics of dimers is investigated. It is shown that MQ NMR coherences of only the zeroth and second orders emerge in such a system. The intensities of those coherences are calculated. Entangled states appear in the course of the system evolution in the MQ NMR experiment. The quantum discord is obtained …
We investigate the dynamics of entanglement and quantum discord of two qubits in liquid state homonuclear NMR. Applying a phenomenological description for NMR under relaxation process, and taking a group of typical parameters of NMR, we show that when a zero initial state $|00> $ experiences a relaxation process, its entanglement disappears completely after a sequence of so-called sudden deaths and revivals, while the quantum discord retains remarkable values after a sequence of oscillations. That is to say, the quantum discord is more robust than entanglement.
In the discussion about the quantumness of NMR computation a conclusion is done that computational states are separable and therefore can not be entangled. This conclusion is based on the assumption that the initial density matrix of an individual molecule coincides with whole sample molecules distribution over single molecule energy levels. This means that quantum stochasticity is replaced by classical stochasticity. In the present paper it is shown, that quantum NMR computation can create genuine entangled states if initial system states are thermodynamical equilibrium ones. A separability a…
Using an NMR quantum computer, we experimentally simulate the quantum phase transition of a Heisenberg spin chain. The Hamiltonian is generated by a multiple pulse sequence, the nuclear spin system is prepared in its (pseudo-pure) ground state and the effective Hamiltonian varied in such a way that the Heisenberg chain is taken from a product state to an entangled state and finally to a different product state.
Entanglement witnesses (EW) allow the detection of entanglement in a quantum system, from the measurement of some few observables. They do not require the complete determination of the quantum state, which is regarded as a main advantage. On this paper it is experimentally analyzed an entanglement witness recently proposed in the context of Nuclear Magnetic Resonance (NMR) experiments to test it in some Bell-diagonal states. We also propose some optimal entanglement witness for Bell-diagonal states. The efficiency of the two types of EW's are compared to a measure of entanglement with tomograp…
The ultimate precision limit in estimating the Larmor frequency of $N$ unentangled rotating spins is well established, and is highly important for magnetometers, gyroscopes and many other sensors. However this limit assumes perfect, single addressing, measurements of the spins. This requirement is not practical in NMR spectroscopy, as well as other physical systems, where a weakly interacting external probe is used as a measurement device. Here we show that in the framework of quantum nano-NMR spectroscopy, in which these limitations are inherent, the ultimate precision limit is still achievab…
Entanglement control of qubits in a photoisomerizing molecule is studied in the context of an NMR quantum computer by taking azobenzene as an example. Azobenzene has two different isomers, {\it{}trans}-azobenzene (TAB) and {\it{}cis}-azobenzene (CAB), which can be interconverted by photoisomerization. Changing molecular structure leads to change in the spin-spin coupling constant, and hence leads to change in entangling operation time. We first obtain stable structures of TAB and CAB by {\it ab initio} calculation. Then, we calculate the NMR spectra of these isomers and verify that they reprod…
We investigate numerically the time dependence of the multiple quantum coherences and entanglement in linear chains up to nine nuclear spins of 1/2 coupled by the dipole-dipole interactions. Two models are considered: (1) a spin chain with nearest-neighbor dipole -dipole interactions; (2) a more realistic model with interactions between all spins. It is shown that the entangled states appear between remote particles which do not interact directly (model 1), while the interaction between all spins (model 2) not always results in entanglement between remote spins.
Hadamard spectroscopy has earlier been used to speed-up multi-dimensional NMR experiments. In this work we speed-up the two-dimensional quantum computing scheme, by using Hadamard spectroscopy in the indirect dimension, resulting in a scheme which is faster and requires the Fourier transformation only in the direct dimension. Two and three qubit quantum gates are implemented with an extra observer qubit. We also use one-dimensional Hadamard spectroscopy for binary information storage by spatial encoding and implementation of a parallel search algorithm.
The quantum nature of bulk ensemble NMR quantum computing --the center of recent heated debate, is addressed. Concepts of the mixed state and entanglement are examined, and the data in a 2 qubit liquid NMR quantum computation are analyzed. It is pointed out that the key problem in the current debate is the understanding of entanglement in a mixed state system. The following points are concluded in this Letter: 1)Density matrix describes the "state" of an average particle in an ensemble. It can not describe the state of an individual particle in an ensemble in detail; 2) Entanglement is a prope…
The evolution of entanglement in a 3-spin chain with nearest-neighbor Heisenberg-XY interactions for different initial states is investigated here. In an NMR experimental implementation, we generate multipartite entangled states starting from initial separable pseudo-pure states by simulating nearest-neighbor XY interactions in a 3-spin linear chain of nuclear spin qubits. For simulating XY interactions, we follow algebraic method of Zhang et al. [Phys. Rev. A 72, 012331 (2005)]. Bell state between end qubits has been generated by using only the unitary evolution of the XY Hamiltonian. For gen…
Nano-NMR spectroscopy with nitrogen-vacancy centers holds the potential to provide high resolution spectra of minute samples. This is likely to have important implications for chemistry, medicine and pharmaceutical engineering. One of the main hurdles facing the technology is that diffusion of unpolarized liquid samples broadens the spectral lines thus limiting resolution. Experiments in the field are therefore impeded by the efforts involved in achieving high polarization of the sample which is a challenging endeavor. Here we examine a scenario where the liquid is confined to a small volume. …
Nuclear magnetic resonance (NMR) has enormous applications. Two-dimensional NMR is an essential technique to characterize correlations between nuclei and, hence, molecule structures. Towards the ultimate goal of single-molecule NMR, dynamical-decoupling- (DD) enhanced diamond quantum sensing enables the detection of single nuclear spins and nanoscale NMR. However, there is still the lack of a standard method in DD-based quantum sensing to characterize correlations between nuclear spins in single molecules. Here we present a scheme of two-dimensional DD-based quantum sensing, as a universal met…
We undertake experimental detection of the entanglement present in arbitrary three-qubit pure quantum states on an NMR quantum information processor. Measurements of only four observables suffice to experimentally differentiate between the six classes of states which are inequivalent under stochastic local operation and classical communication (SLOCC). The experimental realization is achieved by mapping the desired observables onto Pauli $z$-operators of a single qubit, which is directly amenable to measurement. The detection scheme is applied to known entangled states as well as to states ran…
We investigate the evolution of entanglement in multiple-quantum (MQ) NMR experiments in crystals with pairs of close nuclear spins-1/2. The initial thermodynamic equilibrium state of the system in a strong external magnetic field evolves under the non-secular part of the dipolar Hamiltonian. As a result, MQ coherences of the zeroth and plus/minus second orders appear. A simple condition for the emergence of entanglement is obtained. We show that the measure of the spin pair entanglement, concurrence, coincides qualitatively with the intensity of MQ coherences of the plus/minus second order an…
We experimentally demonstrate a new dynamic fashion of quantum Zeno effect in nuclear magnetic resonance systems. The frequent measurements are implemented through quantum entanglement between the target qubit(s) and the measuring qubit, which dynamically results from the unitary evolution of duration $τ_{m}$ due to dispersive-coupling. Experimental results testify the presence of "the critical measurement time effect", that is, the quantum Zeno effect does not occur when $τ_{m}$ takes the some critical values, even if the measurements are frequent enough. Moreover, we provide a first experime…
We revisit the phenomenon of quantum stochastic resonance in the regime of validity of the Bloch equations. We find that a stochastic resonance behavior in the steady-state response of the system is present whenever the noise-induced relaxation dynamics can be characterized via a single relaxation time scale. The picture is validated by a simple nuclear magnetic resonance experiment in water.
NMR is emerging as a valuable testbed for the investigation of foundational questions in quantum mechanics. The present paper outlines the preparation of a class of mixed states, called pseudo-pure states, that emulate pure quantum states in the highly mixed environment typically used to describe solution-state NMR samples. It also describes the NMR observation of spinor behavior in spin 1/2 nuclei, the simulation of wave function collapse using a magnetic field gradient, the creation of entangled (or Bell) pseudo-pure states, and a brief discussion of quantum computing logic gates, including …
We propose two dimensional x-ray coherent correlation spectroscopy (2DXCS) for the study of interactions between core-electron and valence transitions. This technique might find experimental applications in the future when very high intensity x-ray sources become available. Spectra obtained by varying two delay periods between pulses show off-diagonal cross-peaks induced by coupling of core transitions of two different types. Calculations of the N1s and O1s signals of aminophenol isomers illustrate how novel information about many-body effects in electronic structure and excitations of molecul…
This paper surveys our recent research on quantum information processing by nuclear magnetic resonance (NMR) spectroscopy. We begin with a geometric introduction to the NMR of an ensemble of indistinguishable spins, and then show how this geometric interpretation is contained within an algebra of multispin product operators. This algebra is used throughout the rest of the paper to demonstrate that it provides a facile framework within which to study quantum information processing more generally. The implementation of quantum algorithms by NMR depends upon the availability of special kinds of m…
We established important relationships between entanglement measures and the order parameter (spin polarization) in nuclear spin systems controlled by the nuclear magnetic resonance (NMR) technique. Since spin polarization can be easily manipulated by the NMR technique, experimentalists are presented with an opportunity to study the dynamic properties of entanglement, i.e., the creation and evolution of entangled states. Our approach may constitute the basis for researching the relations between the entanglement measures and measurable parameters of order in other quantum systems.
Quantum correlations are investigated theoretically in a two-spin system with the dipole-dipole interactions in the NMR multiple-pulse spin-locking experiments. We consider two schemes of the multiple-pulse spin-locking. The first scheme consists of $π/2$-pulses only and the delays between the pulses can differ. The second scheme contains $φ$-pulses ($0<φ<π$) and has equal delays between them. We calculate entanglement for both schemes for an initial separable state. We show that entanglement is absent for the first scheme at equal delays between $π/2$-pulses at arbitraty temperatures. Entangl…
Nuclear magnetic resonance (NMR) spectroscopy is a widely used tool for chemical analysis and molecular structure identification. Because it typically relies on the weak magnetic fields produced by a small thermal nuclear spin polarization, NMR suffers from poor molecule-number sensitivity compared to other analytical techniques. Recently, a new class of NMR sensors based on optically-probed nitrogen-vacancy (NV) quantum defects in diamond have allowed molecular spectroscopy from sample volumes several orders of magnitude smaller than the most sensitive inductive detectors. To date, however, N…
We employ a nuclear magnetic resonance (NMR) quantum information processor to simulate the ground state of an XXZ spin chain and measure its NMR analog of entanglement, or pseudo-entanglement. The observed pseudo-entanglement for a small-size system already displays singularity, a signature which is qualitatively similar to that in the thermodynamical limit across quantum phase transitions, including an infinite-order critical point. The experimental results illustrate a successful approach to investigate quantum correlations in many-body systems using quantum simulators.
An extension of the product operator formalism of NMR is introduced, which uses the Hadamard matrix product to describe many simple spin 1/2 relaxation processes. The utility of this formalism is illustrated by deriving NMR gradient-diffusion experiments to simulate several decoherence models of interest in quantum information processing, along with their Lindblad and Kraus representations. Gradient-diffusion experiments are also described for several more complex forms of decoherence, including the well-known collective isotropic model. Finally, it is shown that the Hadamard formalism gives a…
In this work, we have been working on the concept of quantum entanglement. At first, we studied the theory of entanglement in its characterization and measurement, introducing a new scheme for detection of entanglement. The new approach links molecular-spin entities involving nuclear spins to quantum computing as more appropriate physical systems of interest. Then, we continued with the realization of entanglement in experiments. NMR has been the first choice due to its well approved advantages for quantum computing. NMR, however, has not been an appropriate system for demonstrating entangled …
The nitrogen-vacancy (NV) center has enabled widespread study of nanoscale nuclear magnetic resonance (NMR) spectroscopy at low magnetic fields. NMR spectroscopy at high magnetic fields significantly improves the technique's spectral resolution, enabling clear identification of closely related chemical species. However, NV-detected NMR is typically performed using AC sensing through electron spin echo envelope modulation (ESEEM), a hyperfine spectroscopic technique that is not feasible at high magnetic fields. Within this paper, we have explored an NV-detected NMR technique for applications of…
Two-dimensional Nuclear Magnetic Resonance (NMR) is essential in molecular structure determination. The Nitrogen-Vacancy (NV) center in diamond has been proposed and developed as an outstanding quantum sensor to realize NMR in nanoscale. In this work, we develop a scheme for two-dimensional nanoscale NMR spectroscopy based on quantum controls on an NV center. We carry out a proof of principle experiment on a target of two coupled $^{13}$C nuclear spins in diamond. A COSY-like sequences is used to acquire the data on time domain, which is then converted to frequency domain with the fast Fourier…
Quantum technologies have seen a rapid developmental surge over the last couple of years. Though often overshadowed by quantum computation, quantum sensors show tremendous potential for widespread applications in chemistry and biology. One system stands out in particular: the nitrogen-vacancy (NV) center in diamond, an atomic-sized sensor allowing the detection of nuclear magnetic resonance (NMR) signals at unprecedented length scales down to a single proton. In this article, we review the fundamentals of NV center-based quantum sensing and its distinct impact on nano- to microscale NMR spectr…
Nanomagnetometry using the nitrogen-vacancy (NV) centre in diamond has attracted a great deal of interest because of the combined features of room temperature operation, nanoscale resolution and high sensitivity. One of the important goals for nano-magnetometry is to be able to detect nanoscale nuclear magnetic resonance (NMR) in individual molecules. Our theoretical analysis shows how a single molecule at the surface of diamond, with characteristic NMR frequencies, can be detected using a proximate NV centre on a time scale of order seconds with nanometer precision. We perform spatio-temporal…
Quantum error correcting codes enable the information contained in a quantum state to be protected from decoherence due to external perturbations. Applied to NMR, quantum coding does not alter normal relaxation, but rather converts the state of a ``data'' spin into multiple quantum coherences involving additional ancilla spins. These multiple quantum coherences relax at differing rates, thus permitting the original state of the data to be approximately reconstructed by mixing them together in an appropriate fashion. This paper describes the operation of a simple, three-bit quantum code in the …
The existence of quantum correlation (as revealed by quantum discord), other than entanglement and its role in quantum-information processing (QIP), is a current subject for discussion. In particular, it has been suggested that this nonclassical correlation may provide computational speedup for some quantum algorithms. In this regard, bulk nuclear magnetic resonance (NMR) has been successfully used as a test bench for many QIP implementations, although it has also been continuously criticized for not presenting entanglement in most of the systems used so far. In this paper, we report a theoret…
The quantum search problem is an important problem due to the fact that a general NP problem can be solved efficiently by an unsorted quantum search algorithm. Here it has been shown that the quantum search problem could be solved in polynomial time on an NMR quantum computer. The NMR ensemble quantum computation is based on the quantum mechanical unitary dynamics that both a closed quantum system and its ensemble obey the same quantum mechanical unitary dynamics instead of on the pseudopure state or the effective pure state of the classical NMR quantum computation. Based on the new principle …
Nuclear magnetic resonance (NMR) provides an experimental setting to explore physical implementations of quantum information processing (QIP). Here we introduce the basic background for understanding applications of NMR to QIP and explain their current successes, limitations and potential. NMR spectroscopy is well known for its wealth of diverse coherent manipulations of spin dynamics. Ideas and instrumentation from liquid state NMR spectroscopy have been used to experiment with QIP. This approach has carried the field to a complexity of about 10 qubits, a small number for quantum computation …
A connection of the Wigner-Yanase skew information and multiple quantum (MQ) NMR coherences is considered at different temperatures and evolution times of nuclear spins with dipole-dipole interactions in MQ NMR experiments in solids. It is shown that the Wigner-Yanase skew information at temperature $T$ is equal to the double second moment of the MQ NMR spectrum at the double temperature for any evolution times. A comparison of the many-spin entanglement obtained with the Wigner-Yanase information and the Fisher information is conducted.
We demonstrate a synchronized readout (SR) technique for spectrally selective detection of oscillating magnetic fields with sub-millihertz resolution, using coherent manipulation of solid state spins. The SR technique is implemented in a sensitive magnetometer (~50 picotesla/Hz^(1/2)) based on nitrogen vacancy (NV) centers in diamond, and used to detect nuclear magnetic resonance (NMR) signals from liquid-state samples. We obtain NMR spectral resolution ~3 Hz, which is nearly two orders of magnitude narrower than previously demonstrated with NV based techniques, using a sample volume of ~1 pic…
Experimental construction of a symmetric three-qubit entangled state and its utility in testing the violation of a Bell inequality on an NMR quantum simulator
We performed a banged-digital-analog simulation of a quantum annealing protocol in a two-qubit Nuclear Magnetic Resonance (NMR) quantum computer. Our experimental simulation employed up to 235 Trotter steps, with more than 2000 gates (pulses), and we obtained a protocol success above 80%. Given the exquisite control of the NMR quantum computer, we performed the simulation with different noise levels. We thus analyzed the reliability of the quantum annealing process, and related it to the level of entanglement produced during the protocol. Although the presence of entanglement is not a sufficie…
We propose a new approach to the measurement of a single spin state, based on nuclear magnetic resonance (NMR) techniques and inspired by the coherent control over many-body systems envisaged by Quantum Information Processing (QIP). A single target spin is coupled via the natural magnetic dipolar interaction to a large ensemble of spins. Applying external radio frequency (rf) pulses, we can control the evolution of the system so that the spin ensemble reaches one of two orthogonal states whose collective properties differ depending on the state of the target spin and are easily measured. We fi…
Nitrogen vacancy (NV) centers in diamond have been used as ultrasensitive magnetometers to perform nuclear magnetic resonance (NMR) spectroscopy of statistically polarized samples at 1 - 100 nm length scales. However, the spectral linewidth is typically limited to the kHz level, both by the NV sensor coherence time and by rapid molecular diffusion of the nuclei through the detection volume which in turn is critical for achieving long nuclear coherence times. Here we provide a blueprint for a set-up that combines a sensitivity sufficient for detecting NMR signals from nano- to micron-scale samp…
This thesis addresses the problems of initialization and separability in liquid state NMR based quantum information processors. We prepare pure quantum states lying above the entanglement threshold. Our pure state quantum computer derives its purity from the highly polarized nuclear spin states in the para-hydrogen molecule. The thesis begins with a critique of conventional NMR based quantum information processing outlining the major strengths and weaknesses of the technology. We describe the enhanced magnetic ordering of the nuclear spin states in para-hydrogen and an initialization experimen…
