We derive the Hamiltonian in the rotating frame for NMR quantum computing with homonucleus molecules as its computational resource. The Hamiltonian thus obtained is different from conventional Hamiltonians that appear in literature. It is shown that control pulses designed for heteronucleus spins can be translated to pulses for homonucleus spins by simply replacing hard pulses by soft pulses with properly chosen pulse width. To demonstrate the validity of our Hamiltonian, we conducted several experiments employing cytosine as a homonucleus molecule. All the experimental results demonstrate that our Hamiltonian accurately describes the dynamics of the spins, while the conventional Hamiltonian fails. Finally we use our Hamiltonian for precise control of field inhomogeneity compensation with a pair of $π$-pulses.
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…
The effect of Gaussian fluctuations of nanopores filled with a gas of spin-carrying molecules ($s=1/2$) on the multiple quantum (MQ) NMR dynamics is investigated at different variances and correlation times of the fluctuations. We show that the fluctuations smooth out the evolution of MQ NMR coherence intensities which rapidly oscillate as functions of time in the absence of fluctuations. The growth and decay of the MQ coherence clusters in the fluctuating nanopore are also investigated.
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…
Reported in this paper is the impact of the fluctuations of the geometry of the nano-meter gas containers in the medium on the NMR line shape of the gas inside of the nano-containers. We calculate exactly the NMR line shape of the gas of spin-1/2 carrying molecules for two typical dynamics of the nano-container volume and the orientation with respect to the external magnetic field: (i) for a Gaussian stochastic dynamics, and (ii) for the regular harmonic vibrations. For the Gaussian ensemble of static disordered containers having an infinite correlation time, $τ_{\sf c} \to \infty $, the overa…
A local orthogonal transformation that transforms any centrosymmetric (CS) matrix of fourth order to the X form is found. A picewise-analytic-numerical formula Q=min{Q_π/2,Q_θ,Q_0}, where Q_π/2 and Q_0 are analytical expressions and the branch Q_θ is found by numerical searching the optimal measurement angle θ\in(0,π/2), is proposed to calculate the quantum discord Q of general X state. The developed approaches are applied to a quantitative description of recently predicted flickerings (periodic birth and death) of the quantum-information pair correlation between nuclear 1/2 spin of atoms or m…
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…
Recent technological advances may lead to the development of small scale quantum computers capable of solving problems that cannot be tackled with classical computers. A limited number of algorithms has been proposed and their relevance to real world problems is a subject of active investigation. Analysis of many-body quantum system is particularly challenging for classical computers due to the exponential scaling of Hilbert space dimension with the number of particles. Hence, solving problems relevant to chemistry and condensed matter physics are expected to be the first successful applicatio…
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 consider the multiple quantum (MQ) NMR dynamics of a gas of spin carrying molecules in nanocavities. MQ NMR dynamics is determined by the residual dipole-dipole interactions which are not averaged completely due to the molecular diffusion in nanopores. Since the averaged non-secular Hamiltonian describing MQ NMR dynamics depends on only one coupling constant, this Hamiltonian commutes with the square of the total spin angular momentum $\hat I^2$. We use the basis of common eigenstates of $\hat I^2$ and the projection of $I$ on the external magnetic field for investigation of MQ NMR dynamics…
Quantum Information processing by NMR with small number of qubits is well established. Scaling to higher number of qubits is hindered by two major requirements (i) mutual coupling among qubits and (ii) qubit addressability. It has been demonstrated that mutual coupling can be increased by using residual dipolar couplings among spins by orienting the spin system in a liquid crystalline matrix. In such a case, the heteronuclear spins are weakly coupled but the homonuclear spins become strongly coupled. In such circumstances, the strongly coupled spins can no longer be treated as qubits. However,…
We present an experimental implementation of the coined discrete time quantum walk on a square using a three qubit liquid state nuclear magnetic resonance (NMR) quantum information processor (QIP). Contrary to its classical counterpart, we observe complete interference after certain steps and a periodicity in the evolution. Complete state tomography has been performed for each of the eight steps making a full period. The results have extremely high fidelity with the expected states and show clearly the effects of quantum interference in the walk. We also show and discuss the importance of choo…
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…
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…
Single-molecule sensitivity of nuclear magnetic resonance (NMR) and angstrom resolution of magnetic resonance imaging (MRI) are the highest challenges in magnetic microscopy. Recent development in dynamical-decoupling- (DD) enhanced diamond quantum sensing has enabled single-nucleus NMR and nanoscale NMR. Similar to conventional NMR and MRI, current DD-based quantum sensing utilizes the frequency fingerprints of target nuclear spins. The frequency fingerprints by their nature cannot resolve different nuclear spins that have the same noise frequency or differentiate different types of correlati…
Water is the most important solvent in nature. It is a crucial issue to study interactions among water molecules. Nuclear magnetic resonance (NMR) spectroscopy is one of the most powerful tools to detect magnetic interactions for the structure analysis of a molecule with broad applications. But conventional NMR spectroscopy requires macroscopic sample quantities with hampers in investigating nanoscale structures. Through quantum control of a single spin quantum sensor, magnetic resonance spectroscopy of nanoscale organic molecules and single molecules has been achieved. However, the measuremen…
By numerically simulating an implementation of the quantum baker's map on a 3-qubit NMR quantum computer based on the molecule trichloroethylene, we demonstrate the feasibility of quantum chaos experiments on present-day quantum computers. We give detailed descriptions of proposed experiments that investigate (a) the rate of entropy increase due to decoherence and (b) the phenomenon of hypersensitivity to perturbation.
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…
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 demonstrate a five-bit nuclear-magnetic-resonance quantum computer that distinguishes among various functions on four bits, making use of quantum parallelism. Its construction draws on the recognition of the sufficiency of linear coupling along a chain of nuclear spins, the synthesis of a suitably coupled molecule, and the use of a multi-channel spectrometer.
Liquid crystals offer several advantages as solvents for molecules used for nuclear magnetic resonance quantum computing (NMRQC). The dipolar coupling between nuclear spins manifest in the NMR spectra of molecules oriented by a liquid crystal permits a significant increase in clock frequency, while short spin-lattice relaxation times permit fast recycling of algorithms, and save time in calibration and signal-enhancement experiments. Furthermore, the use of liquid crystal solvents offers scalability in the form of an expanded library of spin-bearing molecules suitable for NMRQC. These ideas ar…
It is exponentially hard to simulate quantum systems by classical algorithms, while quantum computer could in principle solve this problem polynomially. We demonstrate such an quantum-simulation algorithm on our NMR system to simulate an hydrogen molecule and calculate its ground-state energy. We utilize the NMR interferometry method to measure the phase shift and iterate the process to get a high precision. Finally we get 17 precise bits of the energy value, and we also analyze the source of the error in the simulation.
Experimental NMR implementations of the Deutsch-Josza quantum algorithm based on pesudo-pure spin states exhibit an exponential sensitivity scaling with the number of qubits. By employing truly mixed spin states in spin Liouville space, where molecules with different nuclear spin configurations represent different input states, the Deutsch-Josza problem can be solved by single function evaluation without sensitivity loss concomitant with increase of the number of bits.
We present a method of using a nuclear magnetic resonance computer to solve the Deutsch-Jozsa problem in which: (1) the number of molecules in the NMR sample is irrelevant to the number of qubits available to an NMR quantum computer, and (2) the initial state is chosen to be the state of thermal equilibrium, thereby avoiding the preparation of pseudopure states and the resulting exponential loss of signal as the number of qubits increases. The algorithm is described along with its experimental implementation using four active qubits. As expected, measured spectra demonstrate a clear distinctio…
A three-qubit 13C solid-state nuclear magnetic resonance (NMR) system for quantum information processing, based on the malonic acid molecule, is used to demonstrate high-fidelity universal quantum control via strongly-modulating radio-frequency pulses. This control is achieved in the strong-coupling regime, in which the timescales of selective qubit addressing and of two-qubit interactions are comparable.
Internal states of different ions in an electrodynamic trap are coupled when a static magnetic field is applied -- analogous to spin-spin coupling in molecules used for NMR. This spin-spin interaction can be used, for example, to implement quantum logic operations in ion traps using NMR methods. The collection of trapped ions can be viewed as a $N$-qubit molecule with adjustable coupling constants.
It has been shown that inter-spin interaction strengths in a spins-1/2 chain can be evaluated by accessing one of the edge spins only. We demonstrate this experimentally for the simplest case, a three-spin chain, with nuclear magnetic resonance (NMR) technique. The three spins in the chain interact through nearest-neighbor Ising interactions under site-dependent transverse fields. The employed molecule is an alanine containing three $^{13}$C nuclei, each of which has spin-1/2.
We report the realization of a nuclear magnetic resonance (NMR) quantum computer which combines the quantum Fourier transform (QFT) with exponentiated permutations, demonstrating a quantum algorithm for order-finding. This algorithm has the same structure as Shor's algorithm and its speed-up over classical algorithms scales exponentially. The implementation uses a particularly well-suited five quantum bit molecule and was made possible by a new state initialization procedure and several quantum control techniques.
Nuclear magnetic resonance (NMR) imaging with shallow nitrogen-vacancy (NV) centers in diamond offers an exciting route toward sensitive and localized chemical characterization at the nanoscale. Remarkable progress has been made to combat the degradation in coherence time and stability suffered by near-surface NV centers using suitable chemical surface termination. However, approaches that also enable robust control over adsorbed molecule density, orientation, and binding configuration are needed. We demonstrate a diamond surface preparation for mixed nitrogen- and oxygen-termination that simu…
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…
Utilizing the highly correlated quantum NOON states of particles, we have implemented a proof-of-principle quantum thermometer using the NMR technique for measuring the variation of local magnetic field with the temperature variation. The system used was the star-topology system of hexafluorophosphate molecules and the thermometer showed a sensitivity of $85nT/ ^o C$. Using the hexafluorophosphate and the trimethylphosphite spin systems, we have quantified the advantage of the quantum protocol over the classical one for measuring magnetic field. The quantum protocol showed the best performance…
Nanoscale NMR of DNA-Functionalized Diamond Using Individual NV Centers
ETH Zürich（苏黎世联邦理工学院）；University of Calgary（卡尔加里大学）；National Institute of Standards and Technology（美国国家标准与技术研究院）；University of Colorado, Boulder（科罗拉多大学博尔德分校）；University of Fribourg（弗里堡大学）
Interaction of molecules with light may lead to electronic transitions and simultaneous vibrational excitations. Franck-Condon factors (FCFs) play an important role in quantifying the intensities of such vibronic transitions occurring during molecular photo-excitations. In this article, we describe a general method for estimating FCFs using a quantum information processor. The method involves the application of a translation operator followed by the measurement of certain projections. We also illustrate the method by experimentally estimating FCFs with the help of a three-qubit NMR quantum inf…
Nuclear magnetic resonance (NMR) spectroscopy is a powerful technique for analyzing the structure and function of molecules, and for performing three-dimensional imaging of the spin density. At the heart of NMR spectrometers is the detection of electromagnetic radiation, in the form of a free induction decay (FID) signal, generated by nuclei precessing around an applied magnetic field. While conventional NMR requires signals from 1e12 or more nuclei, recent advances in sensitive magnetometry have dramatically lowered this number to a level where few or even individual nuclear spins can be dete…
$^{31}$P NMR and MRI are commonly used to study organophosphates that are central to cellular energy metabolism. In some molecules of interest, such as adenosine diphosphate (ADP) and nicotinamide adenine dinucleotide (NAD), pairs of coupled $^{31}$P nuclei in the diphosphate moiety should enable the creation of nuclear spin singlet states, which may be long-lived and can be selectively detected via quantum filters. Here, we show that $^{31}$P singlet states can be created on ADP and NAD, but their lifetimes are shorter than T$_{1}$ and are strongly sensitive to pH. Nevertheless, the singlet s…
The repertoire of problems theoretically solvable by a quantum computer recently expanded to include the approximate evaluation of knot invariants, specifically the Jones polynomial. The experimental implementation of this evaluation, however, involves many known experimental challenges. Here we present experimental results for a small-scale approximate evaluation of the Jones Polynomial by nuclear-magnetic resonance (NMR), in addition we show how to escape from the limitations of NMR approaches that employ pseudo pure states. Specifically, we use two spin 1/2 nuclei of natural abundance chlor…
We have characterized spin-squeezed states produced at a temperature of $26^\circ{\mathrm C}$ on a Nuclear Magnetic Resonance (NMR) quadrupolar system. The implementation is carried out in an ensemble of $^{133}$Cs nuclei with spin $I=7/2$ of a lyotropic liquid crystal sample. We identify the source of spin squeezing due to the interaction between the quadrupole moment of the nuclei and the electric field gradients internally present in the molecules. We use the spin angular momentum representation to describe formally the nonlinear operators that produce the spin squeezing. The quantitative a…
The Greenberger-Horne-Zeilinger (GHZ) effect provides an example of quantum correlations that cannot be explained by classical local hidden variables. This paper reports on the experimental realization of GHZ correlations using nuclear magnetic resonance (NMR). The NMR experiment differs from the originally proposed GHZ experiment in several ways: it is performed on mixed states rather than pure states; and instead of being widely separated, the spins on which it is performed are all located in the same molecule. As a result, the NMR version of the GHZ experiment cannot entirely rule out class…
Efficient polarization of organic molecules is of extraordinary relevance when performing nuclear magnetic resonance (NMR) and imaging. Commercially available routes to dynamical nuclear polarization (DNP) work at extremely low-temperatures, thus bringing the molecules out of their ambient thermal conditions and relying on the solidification of organic samples. In this work we investigate polarization transfer from optically-pumped nitrogen vacancy centers in diamond to external molecules at room temperature. This polarization transfer is described by both an extensive analytical analysis and …
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…
We report the first experimental demonstration of quantum delayed-choice experiment via nuclear magnetic resonance techniques. An ensemble of molecules each with two spin-1/2 nuclei are used as target and the ancilla qubits to perform the quantum circuit corresponding the delayed-choice setup. As expected in theory, our experiments clearly demonstrate the continuous morphing of the target qubit between particle-like and wave-like behaviors. The experimental visibility of the interference patterns shows good agreement with the theory.
An array of planar Penning traps, holding single electrons, can realize an artificial molecule suitable for NMR-like quantum information processing. The effective spin-spin coupling is accomplished by applying a magnetic field gradient, combined to the Coulomb interaction acting between the charged particles. The system lends itself to scalability, since the same substrate can easily accommodate an arbitrary number of traps. Moreover, the coupling strength is tunable and under experimental control. Our theoretical predictions take into account a realistic setting, within the reach of current t…
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…
Conventional nuclear magnetic resonance (NMR) spectroscopy relies on acquiring signal from a macroscopic ensemble of molecules to gain information about molecular structure and dynamics. Transferring this technique to nanoscale sample sizes would enable molecular analysis without the effects of averaging over spatial and temporal inhomogeneities and without the need for macroscopic volumes of analyte, both inherent to large ensemble measurements. Nanoscale NMR based on nitrogen vacancy (NV) centers inside bulk diamond chips achieves single nuclear spin sensitivity and the resolution required t…
The nitrogen vacancy (NV) color center in diamond is an enormously important platform for the development of quantum sensors, including for single spin and single molecule NMR. Detection of weak single-spin signals is greatly enhanced by repeated sequences of microwave pulses; in these dynamical decoupling (DD) techniques, the key control parameters swept in the experiment are the time intervals, $τ$, between pulses. Here we show that, in fact, the pulse duration offers a powerful additional control parameter. While previously, a non-negligible pulse-width has been considered simply a source o…
An efficient technique to generate ensembles of spins that are highly polarized by external magnetic fields is the Holy Grail in Nuclear Magnetic Resonance (NMR) spectroscopy. Since spin-half nuclei have steady-state polarization biases that increase inversely with temperature, spins exhibiting high polarization biases are considered cool, even when their environment is warm. Existing spin-cooling techniques are highly limited in their efficiency and usefulness. Algorithmic cooling is a promising new spin-cooling approach that employs data compression methods in open systems. It reduces the en…
This paper presents a systematic study of applying composite method approximations with locally dense basis sets (LDBS) to efficiently calculate NMR shielding constants in small and medium-sized molecules. The pcSseg-n series of basis sets are shown to have similar accuracy to the pcS-n series when n $\geq1$ and can slightly reduce compute costs. We identify two different LDBS partition schemes that perform very effectively for density functional calculations. We select a large subset of the recent NS372 database containing 290 H, C, N, and O shielding values evaluated by reference methods on …
We investigate analytically and numerically the Multiple Quantum (MQ) NMR dynamics in dipolar ordered spin systems of nuclear spins 1/2 at a low temperatures. We suggest two different methods of MQ NMR. One of them is based on the measurement of the dipolar energy. The other method uses an additional resonance (π/4)_{y}-pulse after the preparation period of the standard MQ NMR experiment in solids and allows one to measure the Zeeman energy. The both considered methods are sensitive to the contribution of remote spins in the interaction and to the spin system structure. The QS method is sensit…
The Yang-Baxter equation is an important tool in theoretical physics, with many applications in different domains that span from condensed matter to string theory. Recently, the interest on the equation has increased due to its connection to quantum information processing. It has been shown that the Yang-Baxter equation is closely related to quantum entanglement and quantum computation. Therefore, owing to the broad relevance of this equation, besides theoretical studies, it also became significant to pursue its experimental implementation. Here, we show an experimental realization of the Yang…
Pure, highly nuclear-spin-polarized molecules have only been produced with molecular beam-separation methods, with production rates up to ${\sim}3{\times}10^{12}$ s$^{-1}$. Here, we propose the production of spin-polarized molecular photofragments from the IR-excitation and photodissociation of molecular beams, with production rates approaching the tabletop-IR-laser photon fluxes of $10^{21}$ s$^{-1}$. We give details on the production of spin-polarized molecular hydrogen and water isotopes, from formaldehyde and formic acid beams, respectively. Macroscopic quantities of these molecules are im…
