PULSEE: A software for the quantum simulation of an extensive set of magnetic resonance observables

We present an open-source software for the simulation of observables in magnetic resonance experiments, including nuclear magnetic/quadrupole resonance NMR/NQR and electron spin resonance (ESR), developed to assist experimental research in the design of new strategies for the investigation of fundamental quantum properties of materials, as inspired by magnetic resonance protocols that emerged in the context of quantum information science (QIS). The package introduced here enables the simulation of both standard NMR spectroscopic observables and the time-evolution of an interacting single-spin system subject to complex pulse sequences, i.e. quantum gates. The main purpose of this software is to facilitate in the development of much needed novel NMR-based probes of emergent quantum orders, which can be elusive to standard experimental probes. The software is based on a quantum mechanical description of nuclear spin dynamics in NMR/NQR experiments and has been widely tested on available theoretical and experimental results. Moreover, the structure of the software allows for basic experiments to easily be generalized to more sophisticated ones, as it includes all the libraries required for the numerical simulation of generic spin systems. In order to make the program easily accessible to a large user base, we developed a user-friendly graphical interface, Jupyter notebooks, and fully-detailed documentation. Lastly, we portray several examples of the execution of the code that illustrate the potential of a novel NMR paradigm, inspired by QIS, for efficient investigation of emergent phases in strongly correlated materials.Comment: 51 page

Exploring quantum chaos with a single nuclear spin

Most classical dynamical systems are chaotic. The trajectories of two identical systems prepared in infinitesimally different initial conditions diverge exponentially with time. Quantum systems, instead, exhibit quasi-periodicity due to their discrete spectrum. Nonetheless, the dynamics of quantum systems whose classical counterparts are chaotic are expected to show some features that resemble chaotic motion. Among the many controversial aspects of the quantum-classical boundary, the emergence of chaos remains among the least experimentally verified. Time-resolved observations of quantum chaotic dynamics are particularly rare, and as yet unachieved in a single particle, where the subtle interplay between chaos and quantum measurement could be explored at its deepest levels. We present here a realistic proposal to construct a chaotic driven top from the nuclear spin of a single donor atom in silicon, in the presence of a nuclear quadrupole interaction. This system is exquisitely measurable and controllable, and possesses extremely long intrinsic quantum coherence times, allowing for the observation of subtle dynamical behavior over extended periods. We show that signatures of chaos are expected to arise for experimentally realizable parameters of the system, allowing the study of the relation between quantum decoherence and classical chaos, and the observation of dynamical tunneling.Comment: revised and published versio

Atomic interferometer measurements of Berry's and Aharonov-Anandan's phases for isolated spins S > 1/2 non-linearly coupled to external fields

The aim of the present paper is to propose experiments for observing the significant features of Berry's phases for S>1, generated by spin-Hamiltonians endowed with two couplings, a magnetic dipole and an electric quadrupole one with external B and E fields, as theoretically studied in our previous work. The fields are assumed orthogonal, this mild restriction leading to geometric and algebraic simplifications. Alkali atoms appear as good candidates for interferometric measurements but there are challenges to be overcome. The only practical way to generate a suitable E-field is to use the ac Stark effect which induces an instability of the dressed atom. Besides atom loss, this might invalidate Berry's phase derivation but this latter problem can be solved by an appropriate detuning. The former puts an upper limit to the cycle duration, which is bounded below by the adiabatic condition. By relying upon our previous analysis of the non-adiabatic corrections, we have been able to reach a compromise for the $^{87}$Rb hf level F=2, m=0 state, which is our candidate for an interferometric measurement of the exotic Berry's phase generated by a rotation of the E-field around the fixed B-field. By a numerical simulation we have shown that the non-adiabatic corrections can be kept below the 0.1% level. As an alternative candidate, we discuss the chromium ground state J=S=3, where the instability problem is easily solved. We make a proposal to extend the measurement of Aharonov-Anandan's phase beyond S=1/2 to the $^{87}$Rb hf level F=m=1, by constructing, with the help of light-shifts, a Hamiltonian able to perform a parallel transport along a closed circuit upon the density matrix space, without any adiabatic constraint. In Appendix A, Berry's phase difference for S=3/2 and 1/2, m=1/2 states is used to perform an entanglement of 3 Qbits.Comment: 23 pages, 6 figures, modifications in the introduction, two paragraphs adde

Quantum information processing by nuclear magnetic resonance on quadrupolar nuclei

Nuclear magnetic resonance is viewed as an important technique for the implementation of many quantum information algorithms and protocols. Although the most straightforward approach is to use the two-level system composed of spin 1/2 nuclei as qubits, quadrupolar nuclei, which possess a spin greater than 1/2, are being used as an alternative. In this study, we show some unique features of quadrupolar systems for quantum information processing, with an emphasis on the ability to execute efficient quantum state tomography (QST) using only global rotations of the spin system, whose performance is shown in detail. By preparing suitable states and implementing logical operations by numerically optimized pulses together with the QST method, we follow the stepwise execution of Grover's algorithm. We also review some work in the literature concerning the relaxation of pseudo-pure states in spin 3/2 systems as well as its modelling in both the Redfield and Kraus formalisms. These data are used to discuss differences in the behaviour of the quantum correlations observed for two-qubit systems implemented by spin 1/2 and quadrupolar spin 3/2 systems, also presented in the literature. The possibilities and advantages of using nuclear quadrupole resonance experiments for quantum information processing are also discussed.CNPqCAPESFAPES

Dark-state suppression and optimization of laser cooling and fluorescence in a trapped alkaline-earth-metal single ion

We study the formation and destabilization of dark states in a single trapped 88Sr+ ion caused by the cooling and repumping laser fields required for Doppler cooling and fluorescence detection of the ion. By numerically solving the time-dependent density matrix equations for the eight-level system consisting of the sublevels of the 5s 2S1/2, 5p 2P1/2, and 4d 2D3/2 states, we analyze the different types of dark states and how to prevent them in order to maximize the scattering rate, which is crucial for both the cooling and the detection of the ion. The influence of the laser linewidths and ion motion on the scattering rate and the dark resonances is studied. The calculations are then compared with experimental results obtained with an endcap ion trap system located at the National Research Council of Canada and found to be in good agreement. The results are applicable also to other alkaline earth ions and isotopes without hyperfine structure

Quantum manipulation of a single trapped molecular ion

The controlled manipulation of quantum states of single trapped atomic ions forms the basis of some of the most precise measurements preformed to date with proven applications in fundamental physics, time keeping and quantum computing. In this thesis, we extend the toolbox of coherent manipulation of single trapped ions to molecular ions with potential applications including measuring a possible time variation of the proton-to-electron mass ratio, $m_p/m_e$, the implementation of new frequency standards in the mid-infrared regime and the realization of noise-insensitive qubits. We describe in detail the theoretical modeling of molecular energy levels, systematic shifts and transition strengths for the identification of molecular transitions which are useful as a new clock standard and as a molecular qubit. The homonuclear diatomic molecule N$_2^+$ is found to form a noise-insensitive system with clock transitions suitable for precision measurements over a wide range of frequencies. We further describe the experimental implementation of a single-molecule trapped-ion experiment for precision measurements including the design, manufacturing and characterization of a new ion trap and the electronic circuits required for stable operation. We describe several techniques used for laser stabilization and present the techniques developed for cooling the molecular ion from an initial temperature of over 1000 K to the motional ground state of the trap below 10 µK. A new state readout technique is presented which relies on phase-sensitive forces to non-destructively read out and prepare the internal state of the molecule from a large number of possible states. The demonstration of state readout and state preparation of a single ground-state-cooled N$_2^+$ ion signifies the successful implementation of all necessary prerequisites for precision measurements and coherent manipulations of single molecular ions

Investigation of Local Structures in Cation-Ordered Microwave Dielectric a Solid-State Nmr and First Principle Calculation Study

Solid-state Nuclear Magnetic Resonance (ssNMR) spectroscopy has proven to be a powerful method to probe the local structure and dynamics of a system. In powdered solids, the nuclear spins experience various anisotropic interactions which depend on the molecular orientation. These anisotropic interactions make ssNMR very useful as they give a specific appearance to the resonance lines of the spectra. The position and shape of these resonance lines can be related to local structure and dynamics of the system under study. My research interest has focused around studying local structures and dynamics of quadrupolar nuclei in materials using ssNMR spectroscopy. $^7$Li and $^{93}$Nb ssNMR magic angle spinning (MAS) spectra, acquired at 17.6 and 7.06 T, have been used to evaluate the structural and dynamical properties of cation-ordered microwave dielectric materials. Microwave dielectric materials are essential in the application of wireless telecommunication, biomedical engineering, and other scientific and industrial implementations that use radio and microwave signals. The study of the local environment with respect to average structure, such as X-ray diffraction study, is essential for the better understanding of the correlations between structures and properties of these materials. The investigation for short and medium range can be performed with the use of ssNMR techniques. Even though XRD results show cationic ordering at the B-site (third coordination spehere), NMR spectra show a presence of disorder materials. This was indicated by the observation of a distribution in NMR parameters derived from experimental $^{93}$Nb NMR spectra and supported by theoretical calculations

Long-Range Interactions in One- and Two-Electron Rydberg Atoms

We present calculations of long-range interactions in Rydberg atoms, with a focus on the dipole-dipole interactions of strontium Rydberg states. The growing use of Rydberg states in the field of cold atoms necessitates a more detailed understanding of the effects of dipole-dipole interactions, which are currently being investigated in a number of research groups worldwide. Calculations of long-range interactions in Rydberg states of caesium, cal- cium, rubidium, strontium and ytterbium are presented. By taking the one active electron approximation we develop consistent models of these long- range interactions, and construct a survey of the Rydberg state dipole-dipole interactions and quadrupole-quadrupole interactions. We compare the inter- actions between series and between atoms, highlighting the importance of certain series for applications suggested in previous works. In order to include two-electron effects in the description of dipole-dipole interactions in divalent atoms, we use multichannel quantum defect theory (MQDT) to develop models of the Rydberg series of strontium. We use an empirical reactance matrix formalism, where the reactance matrix is fitted to reproduce experimentally measured values of the bound state energy levels. Models are found for all series of strontium with L ≤ 3. We extend the MQDT formalism to the description of the natural radiative lifetimes of strontium, where the perturbers are found to have a large quenching effect on these lifetimes. By incorporating the MQDT description of the Rydberg states of strontium into the calculation of dipole-dipole interactions, we find a spin-forbidden two-atom resonance in the 3D2 states of strontium. We consider a one- dimensional lattice of strontium atoms, and find that the internal dynamics of the Rydberg atoms demonstrates spin transport for large lattice spacings and a separation of the spin and total angular momentum dynamics for small lattice spacings. Spin-angular momentum separation (analogous to spin-charge separation in condensed matter) in strontium Rydberg atoms may have uses in the investigation of one-dimensional Fermi gases and their description using Luttinger liquid theory