A procedure is described for storing a 2D pattern consisting of 32x32 = 1024 bits in a spin state of a molecular system and then retrieving the stored information as a stack of NMR spectra. The system used is a nematic liquid crystal, the protons of which act as spin clusters with strong intramolecular interactions. The technique used is a programmable multi-frequency irradiation with low amplitude. When it is applied to the liquid crystal, a large number of coherent long-lived 1H response signals can be excited, resulting in a spectrum showing many sharp peaks with controllable frequencies and amplitudes. The spectral resolution is enhanced by using a second weak pulse with a 90 phase shift, so that the 1024 bits of information can be retrieved as a set of well-resolved pseudo-2D spectra reproducing the input pattern.
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.
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.
We present a simple $^1$H NMR approach for characterizing intermediate to fast regime molecular motions using $^1$H time-domain NMR at low magnetic field. The method is based on a Goldmann Shen dipolar filter (DF) followed by a Mixed Magic Sandwich Echo (MSE). The dipolar filter suppresses the signals arising from molecular segments presenting sub kHz mobility, so only signals from mobile segments are detected. Thus, the temperature dependence of the signal intensities directly evidences the onset of molecular motions with rates higher than kHz. The DF-MSE signal intensity is described by an a…
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…
The algebraic reformulation of molecular Quantum Electrodynamics (mQED) at finite temperatures is applied to Nuclear Magnetic Resonance (NMR) in order to provide a foundation for the reconstruction of much more detailed molecular structures, than possible with current methods. Conventional NMR theories are based on the effective spin model which idealizes nuclei as fixed point particles in a lattice $L$, while molecular vibrations, bond rotations and proton exchange cause a delocalization of nuclei. Hence, a lot information on molecular structures remain hidden in experimental NMR data, if the…
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…
Characterization of the molecular properties of surfaces under ambient or chemically reactive conditions is a fundamental scientific challenge. Moreover, many traditional analytical techniques used for probing surfaces often lack dynamic or molecular selectivity, which limits their applicability for mechanistic and kinetic studies under realistic chemical conditions. Nuclear magnetic resonance spectroscopy (NMR) is a widely used technique and would be ideal for probing interfaces due to the molecular information it provides noninvasively. However, it lacks the sensitivity to probe the small nu…
In this work we experimentally study the efficiency of various dynamical decoupling sequences for suppressing decoherence of single as well as multiple quantum coherences on large spin-clusters. The system involves crystallites of a powdered sample containing a large number of molecular protons interacting via long-range dipole-dipole interaction. The multiple quantum coherences are prepared by progressively creating correlations in the spin lattice using standard pulse sequences implementing two-quantum average Hamiltonian. The spin system is then subjected to various dynamical decoupling seq…
The control of open quantum systems has a fundamental relevance for fields ranging from quantum information processing to nanotechnology. Typically, the system whose coherent dynamics one wants to manipulate, interacts with an environment that smoothly degrades its quantum dynamics. Thus, a precise understanding of the inner mechanisms of this process, called "decoherence", is critical to develop strategies to control the quantum dynamics. In this thesis we solved the generalized Liouville-von Neumann quantum master equation to obtain the dynamics of many-spin systems interacting with a spin b…
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…
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 …
Here we demonstrate that a term in the nuclear spin Hamiltonian, the antisymmetric \textit{J}-coupling, is fundamentally connected to molecular chirality. We propose and simulate a nuclear magnetic resonance (NMR) experiment to observe this interaction and differentiate between enantiomers without adding any additional chiral agent to the sample. The antisymmetric \textit{J}-coupling may be observed in the presence of molecular orientation by an external electric field. The opposite parity of the antisymmetric coupling tensor and the molecular electric dipole moment yields a sign change of the…
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…
We experimentally demonstrate quantum machine learning using NMR based on a framework of quantum reservoir computing. Reservoir computing is for exploiting natural nonlinear dynamics with large degrees of freedom, which is called a reservoir, for a machine learning purpose. Here we propose a concrete physical implementation of a quantum reservoir using controllable dynamics of a nuclear spin ensemble in a molecular solid. In this implementation, we demonstrate learning of nonlinear functions with binary or continuous variable inputs with low mean squared errors. Our implementation and demonstr…
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）
High-Field NMR Characterization and Indirect $J$-Spectroscopy of a Nuclear Spin Chain [U-$^{13}$C,$^{15}$N]-butyronitrile
Novosibirsk State University（新西伯利亚国立大学）；International Tomography Center SB RAS（俄罗斯科学院西伯利亚分院国际 tomography 中心）；Johannes Gutenberg University Mainz（美因茨约翰内斯·古腾堡大学）；Helmholtz Institute Mainz（美因茨亥姆霍兹研究所）；Department of Chemistry, University of Miami（迈阿密大学化学系）；Frost Institute for Chemistry and Molecular Science（弗斯特化学与分子科学研究所）
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…
The nitrogen-vacancy (NV) centre in diamond has emerged as a candidate to non-invasively hyperpolarise nuclear spins in molecular systems to improve the sensitivity of nuclear magnetic resonance (NMR) experiments. Several promising proof of principle experiments have demonstrated small-scale polarisation transfer from single NVs to hydrogen spins outside the diamond. However, the scaling up of these results to the use of a dense NV ensemble, which is a necessary prerequisite for achieving realistic NMR sensitivity enhancement, has not yet been demonstrated. In this work, we present evidence fo…
Zero- to ultra-low-field nuclear magnetic resonance (ZULF NMR) provides a new regime for the measurement of nuclear spin-spin interactions free from effects of large magnetic fields, such as truncation of terms that do not commute with the Zeeman Hamiltonian. One such interaction, the magnetic dipole-dipole coupling, is a valuable source of spatial information in NMR, though many terms are unobservable in high-field NMR, and the coupling averages to zero under isotropic molecular tumbling. Under partial alignment, this information is retained in the form of so-called residual dipolar couplings…
The hyperpolarisation of nuclear spins within target molecules is a critical and complex challenge in magnetic resonance imaging (MRI) and nuclear magnetic resonance (NMR) spectroscopy. Hyperpolarisation offers enormous gains in signal and spatial resolution which may ultimately lead to the development of molecular MRI and NMR. At present, techniques used to polarise nuclear spins generally require low temperatures and/or high magnetic fields, radio-frequency control fields, or the introduction of catalysts or free-radical mediators. The emergence of room temperature solid-state spin qubits ha…
