Implementation of Liouville space search algorithm on strongly dipolar coupled nuclear spins
T. Gopinath, Anil Kumar
备注：
25 pages, 7 figures. "Future Directions of Magnetic Resonance" Special issue to commemorate the Platinum Jubilee of the Indian National Science Academy, Springer, (in press)
Liouville space search algorithm [Bruschweiler, Phys. Rev. Lett. {\bf 85}, 4815(2000).] utilizes mixed initial states of the ensemble, and has been successfully implemented earlier in weakly coupled spins, in which a spin can be identified as a qubit. It has recently been demonstrated that n-strongly coupled spins can be collectively treated as an n-qubit system. Application of algorithms in such systems, requires new approaches using transition selective pulses rather than qubit selective pulses. This work develops a modified version of Liouville space search algorithm, which is applicable for strongly as well as weakly coupled spins. All the steps of the algorithm, can be implemented by using transition selective pulses. Experimental implementation is carried out on a strongly dipolar coupled four qubit system.
Dipolar coupled homonuclear spins present challenging, yet useful systems for quantum information processing. In such systems, eigenbasis of the system Hamiltonian is the appropriate computational basis and coherent control can be achieved by specially designed strongly modulating pulses. In this letter we describe the first experimental implementation of the quantum algorithm for numerical gradient estimation on the eigenbasis of a four spin system.
A model cluster, with a resonant electron spin surrounded with identical nuclear spins occupying the sites of a cubic lattice, and with dipolar coupling between the spins, is used for a theoretical investigation of the transient nutations induced by a strong oscillating field but disturbed by these local dipolar fields. An effective Hamiltonian valid at the time scale of the nutations is first established. An analytical expression for the Dipolar Coherence time tDC is derived by adapting Van Vleck's perturbative approach to the present situation, with weak rather than intermediate dipolar coup…
We implement an iterative quantum state transfer exploiting the natural dipolar couplings in a spin chain of a liquid crystal NMR system. During each iteration a finite part of the amplitude of the state is transferred and by applying an external operation on only the last two spins the transferred state is made to accumulate on the spin at the end point. The transfer fidelity reaches one asymptotically through increasing the number of iterations. We also implement the inverted version of the scheme which can transfer an arbitrary state from the end point to any other position of the chain and…
Geometric phases have been used in NMR, to implement controlled phase shift gates for quantum information processing, only in weakly coupled systems in which the individual spins can be identified as qubits. In this work, we implement controlled phase shift gates in strongly coupled systems, by using non-adiabatic geometric phases, obtained by evolving the magnetization of fictitious spin-1/2 subspaces, over a closed loop on the Bloch sphere. The dynamical phase accumulated during the evolution of the subspaces, is refocused by a spin echo pulse sequence and by setting the delay of transition …
We consider the adiabatic demagnetization in the rotating reference frame (ADRF) of a system of dipolar coupled nuclear spins $s=1/2$ in the external magnetic field. The demagnetization starts with the offset of the external magnetic field (in frequency units) from the Larmor frequency being several times greater than the local dipolar field. For different subsystem sizes, we have found from numerical simulations the temperatures at which subsystems of a one-dimensional nine-spin chain and a plane nine-spin cluster become entangled. These temperatures are of the order of microkelvins and are a…
The thesis is centred on the theory of experimental methods in solid-state Nuclear Magnetic Resonance (ssNMR) spectroscopy, which deals with the interaction of electromagnetic radiation with nuclei in a magnetic field and possessing a fundamental quantum mechanical property called spin. Orientation-dependent interactions in ssNMR, while offering a wealth of information, lead to broad indistinct signal and therefore are averaged out, predominantly by Magic-Angle Spinning (MAS). Reintroduction of the coupling interactions is achieved through radio frequency recoupling pulse sequences. NMR experi…
The interaction between a central qubit spin and a surrounding bath of spins is critical to spin-based solid state quantum sensing and quantum information processing. Spin-bath interactions are typically strongly anisotropic, and rapid physical rotation has long been used in solid-state nuclear magnetic resonance to simulate motional averaging of anisotropic interactions, such as dipolar coupling between nuclear spins. Here, we show that the interaction between electron spins of nitrogen-vacancy centers and a bath of $^{13}$C nuclear spins in a diamond rotated at up to 300,000rpm introduces de…
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.
Continuously tracked, stable, large excursion trajectories of dipolar coupled nuclear spins
University of California, Berkeley（加州大学伯克利分校）；Max Planck Institute for the Physics of Complex Systems（马克斯·普朗克复杂系统物理研究所）；Element Six Innovation（Element Six 创新公司）；Tabor Electronics, Inc.（塔博电子公司）；KTH Royal Institute of Technology（皇家理工学院）；St. Kliment Ohridski University of Sofia（索非亚圣克利门特奥赫里德斯基大学）
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 demonstrate that CPMG and XYXY decoupling sequences with non-ideal $π$ pulses can reduce dipolar interactions between spins of the same species in solids. Our simulations of pulsed electron spin resonance (ESR) experiments show that $π$ rotations with small ($<$~10\%) imperfections refocus instantaneous diffusion. Here, the intractable N-body problem of interacting dipoles is approximated by the average evolution of a single spin in a changing mean field. These calculations agree well with experiments and do not require powerful hardware. Our results add to past attempts to explain similar …
Non-equilibrium dynamics of many-body systems is important in many branches of science, such as condensed matter, quantum chemistry, and ultracold atoms. Here we report the experimental observation of a phase transition of the quantum coherent dynamics of a 3D many-spin system with dipolar interactions, and determine its critical exponents. Using nuclear magnetic resonance (NMR) on a solid-state system of spins at room-temperature, we quench the interaction Hamiltonian to drive the evolution of the system. The resulting dynamics of the system coherence can be localized or extended, depending o…
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…
At the magnetic fields of common NMR instruments, electron Zeeman frequencies are too high for efficient electron-nuclear dipolar cross-relaxation to occur in solution. The rate of that process fades with the electron Zeeman frequency as omega^{-2} - in the absence of isotropic hyperfine couplings, liquid state dynamic nuclear polarisation (DNP) in high-field magnets is therefore impractical. However, contact coupling and dipolar cross-relaxation are not the only mechanisms that can move electron magnetisation to nuclei in liquids: multiple cross-correlated (CC) relaxation processes also exist…
Mapping the physical dipolar Hamiltonian of a solid-state network of nuclear spins onto a system of nearest-neighbor couplings would be extremely useful for a variety of quantum information processing applications, as well as NMR structural studies. We demonstrate such a mapping for a system consisting of an ensemble of spin pairs, where the coupling between spins in the same pair is significantly stronger than the coupling between spins on different pairs. An amplitude modulated RF field is applied on resonance with the Larmor frequency of the spins, with the frequency of the modulation match…
We present a protocol to selectively decouple, recouple, and engineer effective couplings in mesoscopic dipolar spin networks. In particular, we develop a versatile protocol that relies upon magic angle spinning to perform Hamiltonian engineering. By using global control fields in conjunction with a local actuator, such as a diamond Nitrogen Vacancy center located in the vicinity of a nuclear spin network, both global and local control over the effective couplings can be achieved. We show that the resulting effective Hamiltonian can be well understood within a simple, intuitive geometric pictu…
The polarisation dynamics of nuclear spins weakly coupled to an NV center is highly sensitive to the parameters of the microwave control and the nuclear Larmor frequency. What is commonly regarded as a challenge, we propose here as a resource for quantum sensing. By varying a single experimental parameter in a suitable set-up, i.e., the Rabi frequency of a continual microwave driving or the nuclear Larmor frequency, we predict periodic reversals of the steady-state polarisation of the nuclear spin. Crucially, interference between the transverse and longitudinal dipolar interaction of electron …
Quantum information processing often uses systems with dipolar interactions. We use a nuclear spin-based quantum simulator, to study the spreading of information in such a dipolar-coupled system and how perturbations to the dipolar couplings limit the spreading, leading to localization. In [Phys. Rev. Lett. 104, 230403 (2010)], we found that the system reaches a dynamic equilibrium size, which decreases with the square of the perturbation strength. Here, we study the impact of a disordered Hamiltonian with dipolar 1/r^3 interactions. We show that the expansion of the coherence length of the cl…
We propose a two-qubit gate based on dipolar exchange interactions between individually addressable ultracold polar molecules in an array of optical dipole traps. Our proposal treats the full Hamiltonian of the $^1Σ^+$ molecule NaCs, utilizing a pair of nuclear spin states as storage qubits. A third rotationally excited state with rotation-hyperfine coupling enables switchable dipolar exchange interactions between two molecules to generate an iSWAP gate. All three states are insensitive to external magnetic and electric fields. Impacts on gate fidelity due to coupling to other molecular states…
The central spin decoherence problem has been researched for over 50 years in the context of both nuclear magnetic resonance and electron spin resonance. Until recently, theoretical models have employed phenomenological stochastic descriptions of the bath-induced noise. During the last few years, cluster expansion methods have provided a microscopic, quantum theory to study the spectral diffusion of a central spin. These methods have proven to be very accurate and efficient for problems of nuclear-induced electron spin decoherence in which hyperfine interactions with the central electron spin …
A proposal for a scalable, solid-state implementation of a quantum computer is presented. Qubits are fluorine nuclear spins in a solid crystal of fluorapatite [Ca_5 F(PO_4)_3] with resonant frequencies separated by a large field gradient. Quantum logic is accomplished using nuclear-nuclear dipolar couplings with decoupling and selective recoupling RF pulse sequences. Magnetic resonance force microscopy is used for readout. As many as 300 qubits can be implemented in the laboratory extremes of T=10 mK and B_0=20 T with the existing sensitivity of force microscopy.
We experimentally demonstrate an approach to scale up quantum devices by harnessing spin defects in the environment of a quantum probe. We follow this approach to identify, locate, and control two electron-nuclear spin defects in the environment of a single nitrogen-vacancy center in diamond. By performing spectroscopy at various orientations of the magnetic field, we extract the unknown parameters of the hyperfine and dipolar interaction tensors, which we use to locate the two spin defects and design control sequences to initialize, manipulate, and readout their quantum state. We finally crea…
The dynamics of single electron and nuclear spins in a diamond lattice with different 13C nuclear spin concentration is investigated. It is shown that coherent control of up to three individual nuclei in a dense nuclear spin cluster is feasible. The free induction decays of nuclear spin Bell states and single nuclear coherences among 13C nuclear spins are compared and analyzed. Reduction of a free induction decay time T2* and a coherence time T2 upon increase of nuclear spin concentration has been found. For diamond material with depleted concentration of nuclear spin, T2* as long as 30 micros…
We report on the measurement of the contribution of the magnetic-dipole hyperfine interaction to the tensor polarizability of the electronic ground-state in $^{87}$Rb. This contribution was isolated by measuring the differential shift of the clock transition frequency in $^{87}$Rb atoms that were optically trapped in the focus of an intense CO$_2$ laser beam. By comparing to previous tensor polarizability measurements in $^{87}$Rb, the contribution of the interaction with the nuclear electric-quadrupole moment was isolated as well. Our measurement will enable better estimation of black-body sh…
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…
In a closed quantum system of N coupled spins with magnetic quantum number I, there are about (2I + 1)^N constants of motion. However, the possibility of observing such quasi-invariant (QI) states in solid-like spin systems in Nuclear Magnetic Resonance (NMR) is not a strictly exact prediction. The aim of this work is to provide experimental evidence of several QI, in the proton NMR of small spin clusters, besides those already known Zeeman, and dipolar orders (strong and weak). We explore the spin states prepared with the Jeener-Broekaert pulse sequence by analyzing the time-domain signals yi…
Dipolar interaction between the magnetic moments of electrons is studied as a source for electron spin decay in quantum dots or arrays of quantum dots. This magnetic interaction will govern spin decay, after other sources, such as the coupling to nuclear spins or spin orbit coupling, have been eliminated by a suitable sample design. Electron-electron (Coulomb) interactions, important for magnetic properties, are included. Decomposing the dipolar operator according to the symmetric group of electron permutations allows one to deduce vanishing decay channels as a function of electron number and …
Recently, it has been observed that the effective dipolar interactions between nuclear spins of spin-carrying molecules of a gas in a closed nano-cavities are independent of the spacing between all spins. We derive exact time-dependent polarization for all spins in spin-1/2 ensemble with spatially independent effective dipolar interactions. If the initial polarization is on a single (first) spin,$P_1(0)= 1$ then the exact spin dynamics of the model is shown to exhibit a periodical short pulses of the polarization of the first spin, the effect being typical of the systems having a large number,…
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…
We consider the decoherence of a single localized electron spin due to its coupling to the lattice nuclear spin bath in a semiconductor quantum computer architecture. In the presence of an external magnetic field and at low temperatures, the dominant decoherence mechanism is the spectral diffusion of the electron spin resonance frequency due to the temporally fluctuating random magnetic field associated with the dipolar interaction induced flip-flops of nuclear spin pairs. The electron spin dephasing due to this random magnetic field depends intricately on the quantum dynamics of the nuclear s…
Entanglement and quantum discord for a pair of nuclear spins $s=1/2$ in a nanopore filled with a gas of spin-carrying molecules (atoms) are studied. The correlation functions describing dynamics of dipolar coupled spins in a nanopore are found. The dependence of spin-pair entanglement on the temperature and the number of spins is obtained from the reduced density matrix, which is centrosymmetric (CS). An analytic expression for the concurrence is obtained for an arbitrary CS density matrix. It is shown that the quantum discord as a measure of quantum correlations attains a significant value at…
We investigate pure dephasing decoherence (free induction decay and spin echo) of a spin qubit interacting with a nuclear spin bath. While for infinite magnetic field B the only decoherence mechanism is spectral diffusion due to dipolar flip-flops of nuclear spins, with decreasing B the hyperfine-mediated interactions between the nuclear spins become important. We give a theory of decoherence due to these interactions which takes advantage of their long-range nature. For a thermal uncorrelated bath we show that our theory is applicable down to B~10 mT, allowing for comparison with recent exper…
We report NMR experiments using high-power, RF decoupling techniques to show that a 29-Si nuclear spin qubit in a solid silicon crystal at room temperature can preserve quantum phase for 10^9 precessional periods. The coherence times we report are longer than for any other observed solid-state qubit by more than four orders of magnitude. In high quality crystals, these times are limited by residual dipolar couplings and can be further improved by isotopic depletion. In defect-heavy samples, we provide evidence for decoherence limited by 1/f noise. These results provide insight toward proposals…
Distance measurements via the dipolar interaction are fundamental to the application of nuclear magnetic resonance (NMR) to molecular structure determination, but they only provide information on the absolute distance $r$ and polar angle $θ$ between spins. In this Letter, we present a protocol to also retrieve the azimuth angle $ϕ$. Our method relies on measuring the nuclear precession phase after application of a control pulse with a calibrated external radio-frequency coil. We experimentally demonstrate three-dimensional positioning of individual carbon-13 nuclear spins in a diamond host cry…
We propose a model for spectral diffusion of localized spins in semiconductors due to the dipolar fluctuations of lattice nuclear spins. Each nuclear spin flip-flop is assumed to be independent, the rate for this process being calculated by a method of moments. Our calculated spin decoherence time $T_{M}=0.64$ ms for donor electron spins in Si:P is a factor of two longer than spin echo decay measurements. For $^{31}$P nuclear spins we show that spectral diffusion is well into the motional narrowing regime. The calculation for GaAs quantum dots gives $T_{M}=10-50$ $μ$s depending on the quantum …
Electron spin qubits in molecular systems offer high reproducibility and the ability to self assemble into larger architectures. However, interactions between neighbouring qubits are 'always-on' and although the electron spin coherence times can be several hundred microseconds, these are still much shorter than typical times for nuclear spins. Here we implement an electron-nuclear hybrid scheme which uses coherent transfer between electron and nuclear spin degrees of freedom in order to both controllably turn on/off dipolar interactions between neighbouring spins and benefit from the long nucl…
The enormous theoretical potential of Quantum Information Processing (QIP) is driving the pursuit for its practical realization by various physical techniques. Currently Nuclear Magnetic Resonance (NMR) has been the forerunner by demonstrating a majority of quantum algorithms. In NMR, spin systems consisting of coupled nuclear spins are utilized as qubits. In order to carry out QIP, a spin system has to meet two major requirements: (i) qubit addressability and (ii) mutual coupling among the qubits. It has been demonstrated that the magnitude of the mutual coupling among qubits can be increased…
This work introduces the so-called synchrosqueezed wavelet transform, to shed light on the dipolar fluctuations of a thermal ensemble of nuclear spins in a diamond crystal structure, hyperfine-coupled to a central spin. The raw time series of the nuclear spin bath coherent dynamics is acquired through the two-point correlation function computed using the cluster correlation expansion method. The dynamics can be conveniently analyzed according to zero-, single-, and double-quantum transitions derived from the dipolar pairwise spin flips. We show that in the early-time behavior when the coherenc…
The coupled-channels density-matrix technique for nuclear reaction dynamics, which is based on the Liouville-von Neumann equation with Lindblad dissipative terms, is developed with the inclusion of full angular momentum couplings. It allows a quantitative study of the role and importance of quantum decoherence in nuclear scattering. Formulae of asymptotic observables that can reveal effects of quantum decoherence are given. A method for extracting energy-resolved scattering information from the time-dependent density matrix is introduced. As an example, model calculations are carried out for t…
We investigate the dynamic nuclear polarization process by frequently injecting polarized electron spins into a quantum dot. Due to the suppression of the direct dipolar and indirect electron-mediated nuclear spin interactions, by the frequently injected electron spins, the analytical predictions under the independent spin approximation agree well with quantum numerical simulations. Our results show that the acquired nuclear polarization is highly inhomogeneous, proportional to the square of the local electron-nuclear hyperfine interaction constant, if the injection frequency is high. Utilizin…
An experiment demonstrating the quantum simulation of a spin-lattice Hamiltonian is proposed. Dipolar interactions between nuclear spins in a solid state lattice can be modulated by rapid radio-frequency pulses. In this way, the effective Hamiltonian of the system can be brought to the form of an antiferromagnetic Heisenberg model with long range interactions. Using a semiconducting material with strong optical properties such as InP, cooling of nuclear spins could be achieved by means of optical pumping. An additional cooling stage is provided by adiabatic demagnetization in the rotating fram…
Evaluating the role of perturbations versus the intrinsic coherent dynamics in driving to equilibrium is of fundamental interest to understand quantum many-body thermalization, in the quest to build ever complex quantum devices. Here we introduce a protocol that scales down the coupling strength in a quantum simulator based on a solid-state nuclear spin system, leading to a longer decay time T2, while keeping perturbations associated to control error constant. We can monitor quantum information scrambling by measuring two powerful metrics, out-of-time-ordered correlators (OTOCs) and Loschmidt …
Periodically driven Floquet quantum systems provide a promising platform to investigate novel physics out of equilibrium. Unfortunately, the drive generically heats up the system to a featureless infinite temperature state. For large driving frequency, the heat absorption rate is predicted to be exponentially small, giving rise to a long-lived prethermal regime which exhibits all the intriguing properties of Floquet systems. Here we experimentally observe Floquet prethermalization using nuclear magnetic resonance techniques. We first show the relaxation of a far-from-equilibrium initial state …
Direct Observation of Dipolar-Driven Anisotropic Quantum Projection Noise in a Solid-State Spin Ensemble
Massachusetts Institute of Technology（麻省理工学院）；Harvard University（哈佛大学）；University of California, Santa Barbara（加州大学圣塔芭芭拉分校）；California Institute of Technology（加州理工学院）；Boston University（波士顿大学）
Magnetic Resonance Imaging (MRI) can characterize and discriminate among tissues using their diverse physical and biochemical properties. Unfortunately, submicrometer screening of biological specimens is presently not possible, mainly due to lack of detection sensitivity. Here we analyze the use of a nitrogen-vacancy center in diamond as a magnetic sensor for nanoscale nuclear spin imaging and spectroscopy. We examine the ability of such a sensor to probe the fluctuations of the "classical" dipolar field due to a large number of neighboring nuclear spins in a densely protonated sample. We iden…
Nuclear spins in semiconductors are leading candidates for quantum technologies, including quantum computation, communication, and sensing. Nuclear spins in diamond are particularly attractive due to their extremely long coherence lifetime. With the nitrogen-vacancy (NV) centre, such nuclear qubits benefit from an auxiliary electronic qubit, which has enabled entanglement mediated by photonic links. The transport of quantum information by the electron itself, via controlled transfer to an adjacent centre or via the dipolar interaction, would enable even faster and smaller processors, but optic…
A scheme for decoupling and selectively recoupling large networks of dipolar-coupled spins is proposed. The scheme relies on a combination of broadband, decoupling pulse sequences applied to all the nuclear spins with a band-selective pulse sequence for single spin rotations or recoupling. The evolution-time overhead required for selective coupling is independent of the number of spins, subject to time-scale constraints, for which we discuss the feasibility. This scheme may improve the scalability of solid-state-NMR quantum computing architectures.
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.
Van der Waals layered materials are a focus of materials research as they support strong quantum effects and can easily form heterostructures. Electron spins in van der Waals materials played crucial roles in many recent breakthroughs, including topological insulators, two-dimensional (2D) magnets, and spin liquids. However, nuclear spins in van der Waals materials remain an unexplored quantum resource. Here we report the first demonstration of optical polarization and coherent control of nuclear spins in a van der Waals material at room temperature. We use negatively-charged boron vacancy ($V…
