As a complementary analysis tool to conventional high-field NMR, zero- to ultralow-field (ZULF) NMR detects nuclear magnetization signals in the sub-microtesla regime. Spin-exchange relaxation-free (SERF) atomic magnetometers provide a new generation of sensitive detector for ZULF NMR. Due to the features such as low-cost, high-resolution and potability, ZULF NMR has recently attracted considerable attention in chemistry, biology, medicine, and tests of fundamental physics. This review describes the basic principles, methodology and recent experimental and theoretical development of ZULF NMR, as well as its applications in spectroscopy, quantum control, imaging, NMR-based quantum devices, and tests of fundamental physics. The future prospects of ZULF NMR are also discussed.
Ultralow-field nuclear magnetic resonance (NMR) provides a new regime for many applications ranging from materials science to fundamental physics. However, the experimentally observed spectra show asymmetric amplitudes, differing greatly from those predicted by the standard theory. Its physical origin remains unclear, as well as how to suppress it. Here we provide a comprehensive model to explain the asymmetric spectral amplitudes, further observe more unprecedented asymmetric spectroscopy and find a way to eliminate it. Moreover, contrary to the traditional idea that asymmetric phenomena were…
We use an atomic fountain clock to measure quantum scattering phase shifts precisely through a series of narrow, low-field Feshbach resonances at average collision energies below $1\,μ$K. Our low spread in collision energy yields phase variations of order $\pm π/2$ for target atoms in several $F,m_F$ states. We compare them to a theoretical model and establish the accuracy of the measurements and the theoretical uncertainties from the fitted potential. We find overall excellent agreement, with small statistically significant differences that remain unexplained.
Quadrature-detected zero-to-ultralow-field nuclear magnetic resonance
Physikalisch-Technische Bundesanstalt (PTB)（德国联邦物理技术研究院）；New York University（纽约大学）；North Carolina State University（北卡罗来纳州立大学）；Jagiellonian University in Kraków（克拉科夫雅盖隆大学）；Johannes Gutenberg University of Mainz（美因茨约翰内斯·古腾堡大学）
We propose a laser cooling mechanism that leads to a temperature significantly lower than the single-photon recoil limit, about $4\times 10^{-4}\,E_{r}$. This mechanism benefits from sharp and high-contrast spectra which are induced by interacting dark-state resonances. It is theoretically demonstrated that four-level atoms illuminated by two counter-propagating probe beams and two additional beams directed perpendicularly to other two, exhibit new cooling effects; For red detuned probe lasers, atoms can be subject to a strong viscous force with an extremely small diffusion, characteristic of …
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）
Nuclear-spin qubits have long coherence time and are desirably applied into quantum information processing. However, the existing methods either fail to address single nucleus (such as nuclear magnetic resonance), or severely affect nuclear coherence time (such as electrical nuclear manipulation based on hyperfine stark effect, ENMHSE). Here we propose an electrical nuclear manipulation called nuclear electric resonance which can on the one hand address the single nuclear qubit, and on the other keep the long coherence time. Applying this, we construct universal quantum gates with external ele…
We report here the experimental realization of multi-step cooling of a quantum system via heat-bath algorithmic cooling. The experiment was carried out using nuclear magnetic resonance (NMR) of a solid-state ensemble three-qubit system.
Here we describe a Nuclear Magnetic Resonance (NMR) experiment that uses a three qubit NMR device to implement the one to two approximate quantum cloning network of Buzek et al.
Quantum decoherence has been studied using nuclear magnetic resonance(NMR). By choosing one qubit to simulate environment, we examine the decoherence behavior of two quantum systems: a one qubit system and a two qubit system. The experimental results show agreements with the theoretical predictions. Our experiment schemes can be generalized to the case that the environment is composed of multiple qubits.
According to the theoretical results, the quantum searching algorithm can be generalized by replacing the Walsh-Hadamard(W-H) transform by almost any quantum mechanical operation. We have implemented the generalized algorithm using nuclear magnetic resonance techniques with a solution of chloroform molecules. Experimental results show the good agreement between theory and experiment.
An unusual regime for liquid-state nuclear magnetic resonance (NMR) where the magnetic field strength is so low that the $J$-coupling (intramolecular spin-spin) interactions dominate the spin Hamiltonian opens a new paradigm with applications in spectroscopy, quantum control, and in fundamental-physics experiments, including searches for well-motivated dark-matter candidates. An interesting possibility is to bring this kind of "extreme NMR" together with another one---single nuclear spin detected with a single-spin quantum sensor. This would enable single-molecule $J$-spectroscopy.
The quantum clock synchronization algorithm proposed by I. L. Chuang (Phys. Rev. Lett, 85, 2006(2000)) has been implemented in a three qubit nuclear magnetic resonance quantum system. The effective-pure state is prepared by the spatial averaging approach. The time difference between two separated clocks can be determined by reading out directly through the NMR spectra.
It is demonstrated that nuclear magnetic resonance experiments using pseudopure spin states can give possible outcomes of projective quantum measurement and probabilities of such outcomes. The physical system is a cluster of six dipolar-coupled nuclear spins of benzene in a liquid-crystalline matrix. For this system with the maximum total spin S=3, the results of measuring $S_X$ are presented for the cases when the state of the system is one of the eigenstates of $S_Z$.
We propose a nuclear spin quantum computer based on magnetic resonance force microscopy (MRFM). It is shown that an MRFM single-electron spin measurement provides three essential requirements for quantum computation in solids: (a) preparation of the ground state, (b) one- and two- qubit quantum logic gates, and (c) a measurement of the final state. The proposed quantum computer can operate at temperatures up to 1K.
Magnetic Resonance Force Microscopy (MRFM) is a powerful technique to detect a small number of spins that relies on force-detection by an ultrasoft magnetically tipped cantilever and selective magnetic resonance manipulation of the spins. MRFM would greatly benefit from ultralow temperature operation, because of lower thermomechanical noise and increased thermal spin polarization. Here, we demonstrate MRFM operation at temperatures as low as 30 mK, thanks to a recently developed SQUID-based cantilever detection technique which avoids cantilever overheating. In our experiment, we detect danglin…
By choosing H nucleus in Carbon-13 labelled trichloroethylene as one qubit environment, and two C nuclei as a two-qubit system, we have simulated quantum decoherence when the system lies in an entangled state using nuclear magnetic resonance (NMR). Decoupling technique is used to trace over the environment degrees of freedom. Experimental results show agreements with the theoretical predictions. Our experiment scheme can be generalized to the case that environment is composed of multiple qubits.
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…
An experimental platform of ultralow-temperature pulsed ENDOR (electron-nuclear double resonance) spectroscopy is constructed for the bulk materials. Coherent property of the coupled electron and nuclear spins of the rare-earth (RE) dopants in a crystal (143Nd3+:Y2SiO5) is investigated from 100 mK to 6 K. At the lowest working temperatures, two-pulse-echo coherence time exceeding 2 ms and 40 ms are achieved for the electron and nuclear spins, while the electronic Zeeman and hyperfine population lifetimes are more than 15 s and 10 min. With the aid of the near-unity electron spin polarization a…
Four-body interaction plays an important role in many-body systems, and it can exhibit interesting phase transition behaviors. Historically it was the need to efficiently simulate quantum systems that lead the idea of a quantum computer. In this Letter, we report the experimental demonstration of a four-body interaction in a four- qubit nuclear magnetic resonance quantum information processor. The strongly modulating pulse is used to implement spin selective excitation. The results show a good agreement between theory and experiment.
The three- spin chain with Heisenberg XY- interaction is simulated in a three- qubit nuclear magnetic resonance (NMR) quantum computer. The evolution caused by the XY- interaction is decomposed into a series of single- spin rotations and the $J$- coupling evolutions between the neighboring spins. The perfect state transfer (PST) algorithm proposed by M. Christandl et al [Phys. Rev. Lett, 92, 187902(2004)] is realized in the XY- chain.
Entangled quantum states are an important element of quantum information techniques. We determine the requirements for states of quadrupolar nuclei with spins >1/2 to be entangled. It was shown that entanglement is achieved at low temperature by applying a magnetic field to a quadrupolar nuclei possess quadrupole moments, which interacts with the electricfield gradient produced by the charge distribution in their surroundings.
A multiple round quantum dense coding (MRQDC) scheme based on the quantum phase estimation algorithm is proposed. Using an $m+1$ qubit system, Bob can transmit $2^{m+1}$ messages to Alice, through manipulating only one qubit and exchanging it between Alice and Bob for $m$ rounds. The information capacity is enhanced to $m+1$ bits. We have implemented the scheme in a three- qubit nuclear magnetic resonance (NMR) quantum computer. The experimental results show a good agreement between theory and experiment.
A qubit chosen from equatorial or polar great circles on a Bloch sphere can be remotely prepared with an Einstain-Podolsky-Rosen (EPR) state shared and a cbit communication. We generalize this protocal into an arbitrary longitudinal qubit on the Bloch sphere in which the azimuthal angle phi can be an arbitrary value instead of only being zero. The generalized scheme was experimentally realized using liquid-state nuclear magnetic resonance (NMR) techniques. Also, we have experimentally demonstrated remote state measurement (RSM) on an arbitary qubit proposed by Pati.
We demonstrate the use of an NMR quantum computer based on the pyrimidine base cytosine, and the implementation of a quantum algorithm to solve Deutsch's problem.
We have tested complementarity for the ensemble-averaged spin states of nuclei $^{13}$C in the molecule of $^{13}$CHCl$_{3}$ by the use of the spin states of another nuclei $^{1}$H as the path marker. It turns out that the wave-particle duality holds when one merely measures the probability density of quantum states, and that the wave- and particle-like behavior is simultaneously observed with the help of measuring populations and coherence in a single nuclear magnetic resonance(NMR) experiment. Effects of path-marking schemes and causes of the appearance and disappearance of the wave behavior…
We report the detection and polarization of nuclear spins in diamond at room temperature by using a single nitrogen-vacancy (NV) center. We use Hartmann-Hahn double resonance to coherently enhance the signal from a single nuclear spin while decoupling from the noisy spin-bath, which otherwise limits the detection sensitivity. As a proof-of-principle we: (I) observe coherent oscillations between the NV center and a weakly coupled nuclear spin, (II) demonstrate nuclear bath cooling which prolongs the coherence time of the NV sensor by more than a factor of five. Our results provide a route to na…
Shifts from the expected nuclear magnetic resonance frequencies of antimony and bismuth donors in silicon of greater than a megahertz are observed in electrically detected magnetic resonance spectra. Defects created by ion implantation of the donors are discussed as the source of effective electric field gradients generating these shifts via quadrupole interaction with the nuclear spins. The experimental results are modeled quantitatively by molecular orbital theory for a coupled pair consisting of a donor and a spin-dependent recombination readout center.
We demonstrate a method to quantify and manipulate nuclear spin decoherence mechanisms that are active in zero to ultralow magnetic fields. These include: (i) non-adiabatic switching of spin quantization axis, due to residual background fields; (ii) scalar pathways due to through-bond couplings between $^1$H and heteronuclear spin species, such as $^2$H used partially as an isotopic substitute for $^1$H. Under conditions of free evolution, scalar relaxation due to $^2$H can significantly limit nuclear spin polarization lifetimes and thus the scope of magnetic resonance procedures near zero fie…
We show that, under an appropriate out-of-plane static magnetic field, nuclear spins in a thin specimen on a surface acoustic wave (SAW) cavity can be resonantly excited and detected through spin-rotation coupling. Since such a SAW cavity can have the quality factor as high as $10^{4}$ and the mode volume as small as $10^{-2}$ mm$^{3}$ the signal-to-noise ratio in detecting the resonance is estimated to be quite high. We argue that detecting nuclear spin resonance of a single flake of an atomically-thin layer of two-dimensional semiconductor, which has so far been beyond hope with the conventi…
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…
Density functional theory within the two-component quasi-relativistic zeroth-order regular approximation (ZORA) is used to predict parity violation shifts in 183W nuclear magnetic resonance shielding tensors of chiral, tetrahedrally bonded tungsten complexes of the form NWXYZ (X, Y, Z = H, F, Cl, Br or I). The calculations reveal that sub-mHz accuracy is required to detect such tiny effects in this class of compounds, and that parity violation effects are very sensitive to the choice of ligands.
The adiabatic condition governing cyclic adiabatic inversion of proton spins in a micron-sized ammonium chloride crystal was studied using room temperature nuclear magnetic resonance force microscopy. A systematic degradation of signal-to-noise was observed as the adiabatic condition became violated. A theory of adiabatic following applicable to cyclic adiabatic inversion is reviewed and implemented to quantitatively determine an adiabaticity threshold $(γH_1)^2/(ω_{osc}Ω) = 6.0$ from our experimental results.
The error-robust and short composite operations named ConCatenated Composite Pulses (CCCPs), developed as high-precision unitary operations in quantum information processing (QIP), are derived from composite pulses widely employed in nuclear magnetic resonance (NMR). CCCPs simultaneously compensate for two types of systematic errors, which was not possible with the known composite pulses in NMR. Our experiments demonstrate that CCCPs are powerful and versatile tools not only in QIP but also in NMR.
