Understanding the magnetic resonance spectrum of nitrogen vacancy centers in an ensemble of randomly-oriented nanodiamonds

Nanodiamonds containing nitrogen vacancy (NV-) centers show promise for a number of emerging applications including targeted in vivo imaging and generating nuclear spin hyperpolarization for enhanced NMR spectroscopy and imaging. Here, we develop a detailed understanding of the magnetic resonance behavior of NV- centers in an ensemble of nanodiamonds with random crystal orientations. Two-dimensional optically detected magnetic resonance spectroscopy reveals the distribution of energy levels, spin populations, and transition probabilities that give rise to a complex spectrum. We identify overtone transitions that are inherently insensitive to crystal orientation and give well-defined transition frequencies that access the entire nanodiamond ensemble. These transitions may be harnessed for high-resolution imaging and generation of nuclear spin hyperpolarization. The data are well described by numerical simulations from the zero- to high-field regimes, including the intermediate regime of maximum complexity. We evaluate the prospects of nanodiamond ensembles specifically for nuclear hyperpolarization and show that frequency-swept dynamic nuclear polarization may transfer a large amount of the NV- center's hyperpolarization to nuclear spins by sweeping over a small region of its spectrum.Comment: 6 pages, 5 figure

A subradiant optical mirror formed by a single structured atomic layer

Efficient and versatile interfaces for the interaction of light with matter are an essential cornerstone for quantum science. A fundamentally new avenue of controlling light-matter interactions has been recently proposed based on the rich interplay of photon-mediated dipole-dipole interactions in structured subwavelength arrays of quantum emitters. Here we report on the direct observation of the cooperative subradiant response of a two-dimensional (2d) square array of atoms in an optical lattice. We observe a spectral narrowing of the collective atomic response well below the quantum-limited decay of individual atoms into free space. Through spatially resolved spectroscopic measurements, we show that the array acts as an efficient mirror formed by only a single monolayer of a few hundred atoms. By tuning the atom density in the array and by changing the ordering of the particles, we are able to control the cooperative response of the array and elucidate the interplay of spatial order and dipolar interactions for the collective properties of the ensemble. Bloch oscillations of the atoms out of the array enable us to dynamically control the reflectivity of the atomic mirror. Our work demonstrates efficient optical metamaterial engineering based on structured ensembles of atoms and paves the way towards the controlled many-body physics with light and novel light-matter interfaces at the single quantum level.Comment: 8 pages, 5 figures + 12 pages Supplementary Infomatio

meV resolution in laser-assisted energy-filtered transmission electron microscopy

The electronic, optical, and magnetic properties of quantum solids are determined by their low-energy (< 100 meV) many-body excitations. Dynamical characterization and manipulation of such excitations relies on tools that combine nm-spatial, fs-temporal, and meV-spectral resolution. Currently, phonons and collective plasmon resonances can be imaged in nanostructures with sub-nm and 10s meV space/energy resolution using state-of-the-art energy-filtered transmission electron microscopy (TEM), but only under static conditions, while fs-resolved measurements are common but lack spatial or energy resolution. Here, we demonstrate a new method of spectrally resolved photon-induced near-field electron microscopy (SRPINEM) that allows us to obtain nm-fs-resolved maps of nanoparticle plasmons with an energy resolution determined by the laser linewidth (20 meV in this work), and not limited by electron beam and spectrometer energy spreading. This technique can be extended to any optically-accessible low-energy mode, thus pushing TEM to a previously inaccessible spectral domain with an unprecedented combination of space, energy and temporal resolution.Comment: 19 pages, 7 figure

Study of the properties of hyperpolarized xenon-129 for magnetic resonance imaging

Produkce hyperpolarizovaných plynů, především helia (3He) nebo xenonu (129Xe), nachází stále rostoucí rozsah aplikací v zobrazování magnetickou rezonancí (MRI). Helium ani xenon nejsou obyčejně obsaženy v těle a experimenty tedy nejsou ovlivněny nechtěným signálem z okolních tkání. Ukázalo se, že několika hyperpolarizačními technikami může být magnetická polarizace (magnetizace) jader vzácných plynů zvýšena na hladinu, se kterou jsou praktické aplikace proveditelné. Hyperpolarizované plyny mohou tedy být užitečným nástrojem pro neinvazivní zkoumání lidského dýchání, dovolující statické zobrazování během zadržení dechu nebo zkoumání dynamiky výdechu nebo nádechu, nebo funkčního zobrazování. V neživé přírodě, mohou být hyperpolarizovaný plyny využity jako kontrastní látka při studiu mikroporézních materiálů, jako jsou zeolity, stavební látky a hmoty, atd. V této doktorské práci je popsán vývoj a konstrukce aparatury pro hyperpolarizaci xenonu (izotopu 129Xe). Nákup hyperpolarizovaného xenonu od jiných výzkumných center v zahraničí a jeho dovážení by ovšem nebylo efektivní a to zejména z důvodu náročnosti zajištění potřebných fyzikálních podmínek pro přepravu hyperpolarizovaného plynu. Toto bylo hlavní motivací k vývoji vlastní technologie pro přípravu hyperpolarizovaného xenonu. Se zvládnutou technologií by bylo možné navázat spolupráci s medicínskými zařízeními, nebo s týmy zabývající se živou nebo neživou přírodou (např. při studiu mikroporézních materiálů, gelů, v zemědělských aplikacích nebo při výzkumu využívajících zvířat, atd.). Cílem této práce je studium teorie hyperpolarizovaných vzácných plynů se zaměřením na 129Xe a experimentální ověření a změření relaxačních časů pomocí jaderné magnetické rezonance. Vzhledem k tomu, že je možné hyperpolarizované vzácné plyny skladovat pro pozdější využití, se tato práce také zabývá možnostmi zásobníku hyperpolarizovaného vzácného plynu a jeho teoretickým a experimentálním řešením. V této práci jsou popsány především dva základní typy experimentů přípravy hyperpolarizovaného xenonu. V obou jsou využity zatavené válcové skleněné vzorky naplněné xenonem a doplňujícím plynem – dusíkem, heliem. První z experimentů se zabývá měřením vlastností termálně polarizovaného xenonu a druhý měřením vlastností hyperpolarizovaného xenonu. Pro hyperpolarizaci 129Xe bylo použito výkonového laseru a experimentálně byla zkoumána jednak míra polarizace na základě změny spektrální hustoty čerpacího laserového svazku a dále pak optimální doba optického čerpání 129Xe a relaxační časy xenonu.The production of hyperpolarized gases (HpG), predominantly helium (3He) or xenon (129Xe), have found a steadily increasing range of applications in magnetic resonance imaging (MRI). Neither helium nor xenon are normally present in the body, thus the magnetic resonance experiments do not suffer from unwanted background signals. It has been demonstrated by several techniques of hyperpolarization that the magnetic polarization (magnetization) of the noble gas nuclei can be increased to levels that make practical application feasible. Hence, hyperpolarized gases may become a useful tool for non-invasive investigation of human lung ventilation, permitting static imaging during breathhold or probing the dynamics of inhalation/exhalation, or functional imaging. In inanimate nature, hyperpolarized gas can be used as a contrast medium for microporous materials, such zeolites, constructive materials in civil engineering, etc. This thesis describes the development and construction of a xenon (129Xe) hyperpolarization (Hp) device. Buying hyperpolarized xenon from other research centres abroad is inefficient mainly because of a need of a fast transport of HpXe under specific conditions. That was the main motivation for developing of our own technology for production of HpXe. Well-handled technology could allow a medical cooperation or cooperation with teams dealing with in/animate nature (microporous material, gels, agriculture, animals, etc.). The aim of this work is to study the hyperpolarized noble gases theory with concern to 129Xe and to experimentally prove and measure xenon relaxation times by the NMR. Since it is possible to store hyperpolarized noble gases for later use, this doctoral thesis also explores the potentials of hyperpolarized noble gas storage system and its theoretical and experimental solution. Mainly two types of experiments are described in the thesis. In both experiments, sealed cylindrical Simax sample filled with xenon and supplement gas – nitrogen, helium were used. The first type of experiment is based on thermally polarized xenon and the second on hyperpolarized xenon. For hyperpolarization of 129Xe a high-power laser was used. In this experiment, the relation between power spectral density of optical pumping beam and efficiency of HpXe production process was investigated. The optimal duration of optical pumping and relaxation times of HpXe were investigated too.

Fast Fiber Orientation Estimation in Diffusion MRI from kq-Space Sampling and Anatomical Priors

High spatio-angular resolution diffusion MRI (dMRI) has been shown to provide accurate identification of complex fiber configurations, albeit at the cost of long acquisition times. We propose a method to recover intra-voxel fiber configurations at high spatio-angular resolution relying on a kq-space under-sampling scheme to enable accelerated acquisitions. The inverse problem for reconstruction of the fiber orientation distribution (FOD) is regularized by a structured sparsity prior promoting simultaneously voxelwise sparsity and spatial smoothness of fiber orientation. Prior knowledge of the spatial distribution of white matter, gray matter and cerebrospinal fluid is also assumed. A minimization problem is formulated and solved via a forward-backward convex optimization algorithmic structure. Simulations and real data analysis suggest that accurate FOD mapping can be achieved from severe kq-space under-sampling regimes, potentially enabling high spatio-angular dMRI in the clinical setting.Comment: 10 pages, 5 figures, Supplementary Material

Comparison of imaging with sub-wavelength resolution in the canalization and resonant tunnelling regimes

We compare the properties of subwavelength imaging in the visible wavelength range for metal-dielectric multilayers operating in the canalization and the resonant tunnelling regimes. The analysis is based on the transfer matrix method and time domain simulations. We show that Point Spread Functions for the first two resonances in the canalization regime are approximately Gaussian in shape. Material losses suppress transmission for higher resonances, regularise the PSF but do not compromise the resolution. In the resonant tunnelling regime, the MTF may dramatically vary in their phase dependence. Resulting PSF may have a sub-wavelength thickness as well as may be broad with multiple maxima and a rapid phase modulation. We show that the width of PSF may be reduced by further propagation in free space, and we provide arguments to explain this surprising observation.Comment: 17 pages,12 figure