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 distinction between constant and balanced functions.
Algorithmic Cooling is a method that uses novel data compression techniques and simplecquantum computing devices to improve NMR spectroscopy, and to offer scalable NMR quantum computers. The algorithm recursively employs two steps. A reversible entropy compression of the computation quantum-bits (qubits) of the system and an irreversible heat transfer from the system to the environment through a set of reset qubits that reach thermal relaxation rapidly. Is it possible to experimentally demonstrate algorithmic cooling using existing technology? To allow experimental algorithmic cooling, the the…
We theoretically investigate thermalization and spin diffusion driven by a quantum spin bath for a realistic solid-state NMR experiment. We consider polycrystalline L-alanine, and investigate how the spin polarization spreads among several $^{13}$C nuclear spins, which interact via dipole-dipole coupling with the bath of strongly dipolar-coupled $^1$H nuclear (proton) spins. We do this by using direct numerical simulation of the many-spin time-dependent Schrödinger equation. We find that, although the proton spins located near the carbon sites interact most strongly with the $^{13}$C spins, th…
The role of mixed state entanglement in liquid-state nuclear magnetic resonance (NMR) quantum computation is not yet well-understood. In particular, despite the success of quantum information processing with NMR, recent work has shown that quantum states used in most of those experiments were not entangled. This is because these states, derived by unitary transforms from the thermal equilibrium state, were too close to the maximally mixed state. We are thus motivated to determine whether a given NMR state is entanglable - that is, does there exist a unitary transform that entangles the state? …
An ensemble of nuclear spin-pairs under certain conditions is known to exhibit singlet state life-times much longer than other non-equilibrium states. This property of singlet state can be exploited in quantum information processing for efficient initialization of quantum registers. Here we describe a general method of initialization and experimentally demonstrate it with two-, three-, and four-qubit nuclear spin registers.
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 …
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…
Experimental implementation of a quantum algorithm requires unitary operator decomposition. Here we treat the unitary operator decomposition as an optimization problem and use Genetic Algorithm, a global optimization method inspired by nature's evolutionary process for operator decomposition. As an application, we apply this to NMR Quantum Information Processing and find a probabilistic way of doing universal quantum computation using global hard pulses. We also demonstrate efficient creation of singlet state (as a special case of Bell state) directly from thermal equilibrium using an optimum …
We present here algorithmic cooling (via polarization-heat-bath)- a powerful method for obtaining a large number of highly polarized spins in liquid nuclear-spin systems at finite temperature. Given that spin-half states represent (quantum) bits, algorithmic cooling cleans dirty bits beyond the Shannon's bound on data compression, by employing a set of rapidly thermal-relaxing bits. Such auxiliary bits could be implemented using spins that rapidly get into thermal equilibrium with the environment, e.g., electron spins. Cooling spins to a very low temperature without cooling the environment cou…
Dymanics of spin dimers in multiple quantum NMR experiment is studied on the 5-qubit superconducting quantum processor of IBM {Quantum Experience} for the both {pure} ground and thermodynamic equilibrium (mixed) initial states. The work can be considered as a first step towards an application of quantum computers to solving problems of magnetic resonance. This article is dedicated to Prof. Klaus Möbius and Prof. Kev Salikhov on the occasion of their 85th birthdays.
In conventional NMR experiments, the Zeeman energy gaps of the nuclear spin ensembles are much lower than their thermal energies, and accordingly exhibit tiny polarizations. Generally such low-purity quantum states are devoid of quantum entanglement. However, there exist certain nonclassical correlations which can be observed even in such systems. In this chapter, we discuss three such quantum correlations, namely, quantum contextuality, Leggett-Garg temporal correlations, and quantum discord. In each case, we provide a brief theoretical background and then describe some results from NMR exper…
Algorithmic cooling is a method that employs thermalization to increase qubit purification level, namely it reduces the qubit-system's entropy. We utilized gradient ascent pulse engineering (GRAPE), an optimal control algorithm, to implement algorithmic cooling in liquid state nuclear magnetic resonance. Various cooling algorithms were applied onto the three qubits of $^{13}$C$_2$-trichloroethylene, cooling the system beyond Shannon's entropy bound in several different ways. In particular, in one experiment a carbon qubit was cooled by a factor of 4.61. This work is a step towards potentially …
We implemented the refined Deutsch-Jozsa algorithm on a 3-bit nuclear magnetic resonance quantum computer, which is the meaningful test of quantum parallelism because qubits are entangled. All of the balanced and constant functions were realized exactly. The results agree well with theoretical predictions and clearly distinguish the balanced functions from constant functions. Efficient refocusing schemes were proposed for the soft z-pulse and J-coupling and it is proved that the thermal equilibrium state gives the same results as the pure state for this algorithm.
Superradiant phase transition (SPT) in thermal equilibrium, as a fundamental concept bridging the statistical physics and electrodynamics, can offer the key resources for quantum information science. Notwithstanding its fundamental and practical significances, equilibrium SPT has never been observed in experiments since the first proposal in the 1970s. Furthermore, the existence of equilibrium SPT in the cavity quantum electrodynamics (QED) systems is still subject of ongoing debates, due to the no-go theorem induced by the so-called A2 term. Based on the platform of nuclear magnetic resonance…
The nitrogen-vacancy (NV) center in diamond is supposed to be a building block for quantum computing and nanometer scale metrology at ambient conditions. Therefore, precise knowledge of its quantum states is crucial. Here, we experimentally show that under usual operating conditions the NV exists in an equilibrium of two charge states (70% in the expected negative (NV-) and 30% in the neutral one (NV0)). Projective quantum non-demolition measurement of the nitrogen nuclear spin enables the detection even of the additional, optically inactive state. The nuclear spin can be coherently driven als…
Physical potentials are routinely approximated to harmonic potentials so as to analytically solve the system dynamics. Often it is important to know when a quantum harmonic oscillator (QHO) behaves quantum mechanically and when classically. Recently Su et. al. [Phys. Rev. A {\bf 85}, 052126 (2012)] have theoretically shown that QHO exhibits quantum contextuality (QC) for a certain set of pseudospin observables. In this work, we encode the four eigenstates of a QHO onto four Zeeman product states of a pair of spin-1/2 nuclei. Using the techniques of NMR quantum information processing, we then d…
The electron and nuclear spins of the shallow donor 31P are promising qubit candidates invoked in many proposed Si-based quantum computing schemes. We have recently shown that the near-elimination of inhomogeneous broadening in highly isotopically enriched 28Si enables an optical readout of both the donor electron and nuclear spins by resolving the donor hyperfine splitting in the near-gap donor bound exciton transitions. We have also shown that pumping these same transitions can very quickly produce large electron and nuclear hyperpolarizations at low magnetic fields, where the equilibrium el…
The multiple quantum (MQ) NMR dynamics in the system of equivalent spins with the dipolar ordered initial state is considered. The high symmetry of the MQ Hamiltonian is used in order to develop the analytical and numerical methods for an investigation of the MQ NMR dynamics in the systems consisting of hundreds of spins from "the first principles". We obtain the dependence of the intensities of the MQ NMR coherences on their orders (profiles of the MQ NMR coherences) for the systems of $200 - 600$ spins. It is shown that these profiles may be well approximated by the exponential distribution …
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…
Recently, Yu, Brown, and Chuang [Phys. Rev. A {\bf 71}, 032341 (2005)] investigated the entanglement attainable from unitary transformed thermal states in liquid-state nuclear magnetic resonance (NMR). Their research gave an insight into the role of the entanglement in a liquid-state NMR quantum computer. Moreover, they attempted to reveal the role of mixed-state entanglement in quantum computing. However, they assumed that the Zeeman energy of each nuclear spin which corresponds to a qubit takes a common value for all; there is no chemical shift. In this paper, we research a model with the ch…
NMR quantum information processing studies rely on the reconstruction of the density matrix representing the so-called pseudo-pure states (PPS). An initially pure part of a PPS state undergoes unitary and non-unitary (relaxation) transformations during a computation process, causing a "loss of purity" until the equilibrium is reached. Besides, upon relaxation, the nuclear polarization varies in time, a fact which must be taken into account when comparing density matrices at different instants. Attempting to use time-fixed normalization procedures when relaxation is present, leads to various an…
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 offer an improved method for using a nuclear-magnetic-resonance quantum computer (NMRQC) to solve the Deutsch-Jozsa problem. Two known obstacles to the application of the NMRQC are exponential diminishment of density-matrix elements with the number of bits, threatening weak signal levels, and the high cost of preparing a suitable starting state. A third obstacle is a heretofore unnoticed restriction on measurement operators available for use by an NMRQC. Variations on the function classes of the Deutsch-Jozsa problem are introduced, both to extend the range of problems advantageous for quan…
An open quantum system refers to a system, which is in turn coupled to an environment that can describe time irreversible dynamics through which the system evolves toward the thermal equilibrium state. We present a quantum mechanically rigorous theory in order to help an analysis of spectra obtained from the advanced nuclear magnetic resonance (NMR) and muon spin rotation, relaxation or resonance ($μ$SR) techniques. Our approach is based on the numerically "exact" hierarchical equations of motion (HEOM) approach, which allows us to study the reduced system dynamics for non-perturbative and non…
Among initialization schemes for ensemble quantum computation beginning at thermal equilibrium, the scheme proposed by Schulman and Vazirani [L. J. Schulman and U. V. Vazirani, in Proceedings of the 31st ACM Symposium on Theory of Computing (STOC'99) (ACM Press, New York, 1999), pp. 322-329] is known for the simple quantum circuit to redistribute the biases (polarizations) of qubits and small time complexity. However, our numerical simulation shows that the number of qubits initialized by the scheme is rather smaller than expected from the von Neumann entropy because of an increase in the sum …
We revisist the issue of entanglement of thermal equilibrium states in composite quantum systems. The possible scenarios are exemplified in bipartite qubit/qubit and qubit/qutrit systems.
We critically discuss the common belief that the thermal Casimir-Polder force can always be represented as a Matsubara sum, as it is true for the Casimir force. On the contrary, an exact treatment of the atom-field coupling reveals that for a ground-state atom, terms associated with virtual-photon absorption contribute to the force which are identified as a signature of non-equilibrium dynamics. Even the equilibrium force on a thermalized atom or molecule may be overestimated when using the ground-state polarizability instead of its thermal counterpart.
Quantum thermodynamics seeks to extend non-equilibrium stochastic thermodynamics to small quantum systems where non-classical features are essential to its description. Such a research area has recently provided meaningful theoretical and experimental advances by exploring the wealth and the power of quantum features along with informational aspects of a system's thermodynamics. The relevance of such investigations is related to the fact that quantum technological devices are currently at the forefront of science and engineering applications. This short review article provides an overview of s…
The loss of coherence in quantum mechanical superposition states limits the time for which quantum information remains useful. Similarly, it limits the distance over which quantum information can be transmitted, resembling Anderson localization, where disorder causes quantum mechanical states to become localized. Here, we investigate in a nuclear spin-based quantum simulator, the localization of the size of spin clusters that are generated by a Hamiltonian driving the transmission of information, while a variable-strength perturbation counteracts the spreading. We find that the system reaches …
We provide an explicit analytical calculation that shows the asymptotic approach of the one dimensional Caldeira-Leggett model to thermal equilibrium in the high temperature and weak coupling limit. We investigate a free particle and a harmonic oscillator system, using both the Lindblad and the non-Lindblad type master equations for each case, and show that thermal equilibrium is reached exactly for the free particle and aproximately for the harmonic oscillator, irrespective of the initial preparation of the system. We also generalize our calculation to higher dimensions.
We characterize all Gaussian dynamical semigroups in continuous variables quantum systems of n-bosonic modes which have a thermal Gibbs state as a stationary solution. This is performed through an explicit relation between the diffusion and dissipation matrices, which characterize the semigroup dynamic, and the covariance matrix of the thermal equilibrium state. We also show that Alicki's quantum detailed-balance condition, based on a Gelfand-Naimark-Segal inner product, allows the determination of the temperature dependence of the diffusion and dissipation matrices, and the identification of …
To understand under which conditions thermodynamics emerges from the microscopic dynamics is the ultimate goal of statistical mechanics. Despite the fact that the theory is more than 100 years old, we are still discussing its foundations and its regime of applicability. A point of crucial importance is the definition of the notion of thermal equilibrium, which is given as the state that maximises the von Neumann entropy. Here we argue that it is necessary to propose a new way of describing thermal equilibrium, focused on observables rather than on the full state of the quantum system. We chara…
We investigate evolution of quantum correlations in ensembles of two-qubit nuclear spin systems via nuclear magnetic resonance techniques. We use discord as a measure of quantum correlations and the Werner state as an explicit example. We first introduce different ways of measuring discord and geometric discord in two-qubit systems and then describe the following experimental studies: (a) We quantitatively measure discord for Werner-like states prepared using an entangling pulse sequence. An initial thermal state with zero discord is gradually and periodically transformed into a mixed state wi…
We study two two-level atomic quantum systems (qubits) placed close to a body held at a temperature different from that of the surrounding walls. While at thermal equilibrium the two-qubit dynamics is characterized by not entangled steady thermal states, we show that absence of thermal equilibrium may bring to the generation of entangled steady states. Remarkably, this entanglement emerges from the two-qubit dissipative dynamic itself, without any further external action on the two qubits, suggesting a new protocol to produce and protect entanglement which is intrinsically robust to environmen…
Current experiments in liquid-state nuclear magnetic resonance quantum computing are limited by low initial polarization. To address this problem, we have investigated the use of optical pumping techniques to enhance the polarization of a 2-qubit NMR quantum computer (13C and 1H in 13CHCl3). To efficiently use the increased polarization, we have generalized the procedure for effective pure state preparation. With this new, more flexible scheme, an effective pure state was prepared with polarization-enhancement of a factor of 10 compared to the thermal state. An implementation of Grover's quant…
We study the energy shift and the Casimir-Polder force of an atom out of thermal equilibrium near the surface of a dielectric substrate. We first generalize, adopting the local source hypothesis, the formalism proposed by Dalibard, Dupont-Roc and Cohen-Tannoudji, which separates the contributions of thermal fluctuations and radiation reaction to the energy shift and allows a distinct treatment to atoms in the ground and excited states, to the case out of thermal equilibrium, and then use the generalized formalism to calculate the energy shift and the Casimir-Polder force of an isotropically po…
Low thermal polarization of nuclear spins is a primary sensitivity limitation for nuclear magnetic resonance. Here we demonstrate optically pumped (microwave-free) nuclear spin polarization of $^{13}\mathrm{C}$ and $^{15}\mathrm{N}$ in $^{15}\mathrm{N}$-doped diamond. $^{15}\mathrm{N}$ polarization enhancements up to $-2000$ above thermal equilibrium are observed in the paramagnetic system $\mathrm{N_s}^{0}$. Nuclear spin polarization is shown to diffuse to bulk $^{13}\mathrm{C}$ with NMR enhancements of $-200$ at room temperature and $-500$ at $\mathrm{240~K}$, enabling a route to microwave-f…
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 report bulk, room-temperature hyperpolarization of 13C nuclear spins observed via high-field nuclear magnetic resonance (NMR). The hyperpolarization is achieved by optical pumping (OP) of nitrogen vacancy defect centers in diamond accompanied by dynamic nuclear polarization (DNP). The technique harnesses the large optically-induced spin polarization of NV- centers at room temperature, which is many orders of magnitude greater than thermal equilibrium polarization and typically achievable only at sub-Kelvin temperatures. Transfer of the spin polarization to the 13C nuclear spins is accomplis…
The thermal Casimir-Lifshitz force among two bodies held at different temperatures displays striking features that are absent in systems in thermal equilibrium. The manifestation of this force has been observed so far only in Bose-Einstein condensates close to a heated substrate, but never between two macroscopic bodies. Observation of the thermal Casimir-Lifhitz force out of thermal equilibrium with conventional Casimir setups is very difficult, because for experimentally accessible separations the thermal force is small compared to the zero-temperature quantum Casimir force, unless prohibiti…
Thermalization is the dynamical process by which a many-body system evolves toward a thermal equilibrium state that maximizes its entropy. In certain cases, however, the establishment of thermal equilibrium is significantly slowed down and a phenomenon of pre-thermalization can emerge. It describes the initial relaxation toward a quasi-steady state after a perturbation. While having similar properties to their thermal counterparts, pre-thermal states exhibit a partial memory of initial conditions. Here, we observe the dynamical formation of a pre-thermal state in a non-equilibrium, two-dimensi…
We develop an exact method for computing Casimir forces and the power of radiative heat transfer between two arbitrary nanostructured surfaces out of thermal equilibrium. The method is based on a generalization of the scattering approach recently used in investigations on the Casimir effect. Analogously to the equilibrium case, we find that also out of thermal equilibrium the shape and composition of the surfaces enter only through their scattering matrices. The expressions derived provide exact results in terms of the scattering matrices of the intervening surfaces.
We study the thermalization of an elementary quantum system modeled by a two-level atom interacting with stationary electromagnetic fields out of thermal equilibrium near a dielectric slab. The slab is held at a temperature different from that of the region where the atom is located. We find that when the slab is a nonabsorbing and nondispersive dielectric of a finite thickness $ d$, no out of thermal equilibrium effects appear as far as the thermalization of the atom is concerned, and a finite thick dielectric slab with a tiny imaginary part in the relative permittivity $\operatorname{Im} ε$ …
A framework for the investigation of disordered quantum systems in thermal equilibrium is proposed. The approach is based on a dynamical model--which consists of a combination of a double-bracket gradient flow and a uniform Brownian fluctuation--that `equilibrates' the Hamiltonian into a canonical distribution. The resulting equilibrium state is used to calculate quenched and annealed averages of quantum observables.
Quantum computation is a subject of much theoretical promise, but has not been realized in large scale, despite the discovery of fault-tolerant procedures to overcome decoherence. Part of the reason is that the theoretically modest requirements still present daunting experimental challenges. The goal of this Dissertation is to reduce various resources required for robust quantum computation, focusing on quantum error correcting codes and solution NMR quantum computation. A variety of techniques have been developed, including high rate quantum codes for amplitude damping, relaxed criteria for q…
The circumstances under which a system reaches thermal equilibrium, and how to derive this from basic dynamical laws, has been a major question from the very beginning of thermodynamics and statistical mechanics. Despite considerable progress, it remains an open problem. Motivated by this issue, we address the more general question of equilibration. We prove, with virtually full generality, that reaching equilibrium is a universal property of quantum systems: Almost any subsystem in interaction with a large enough bath will reach an equilibrium state and remain close to it for almost all times…
