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Register a new userNanoscale NMR Spectroscopy and Imaging of Multiple Nuclear Species
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Nuclear magnetic resonance (NMR) and magnetic resonance imaging (MRI) are well-established techniques that provide valuable information in a diverse set of disciplines but are currently limited to macroscopic sample volumes. Here we demonstrate nanoscale NMR spectroscopy and imaging under ambient conditions of samples containing multiple nuclear species, using nitrogen-vacancy (NV) colour centres in diamond as sensors. With single, shallow NV centres in a diamond chip and samples placed on the diamond surface, we perform NMR spectroscopy and one-dimensional MRI on few-nanometre-sized samples containing $^1$H and $^{19}$F nuclei. Alternatively, we employ a high-density NV layer near the surface of a diamond chip to demonstrate wide-field optical NMR spectroscopy of nanoscale samples containing $^1$H, $^{19}$F, and $^{31}$P nuclei, as well as multi-species two-dimensional optical MRI with sub-micron resolution. For all diamond samples exposed to air, we identify a ubiquitous $^1$H NMR signal, consistent with a $sim 1$ nm layer of adsorbed hydrocarbons or water on the diamond surface and below any sample placed on the diamond. This work lays the foundation for nanoscale NMR and MRI applications such as studies of single proteins and functional biological imaging with subcellular resolution, as well as characterization of thin films with sub-nanometre resolution.
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Nuclear magnetic resonance (NMR) spectroscopy has approached the limit of single molecule sensitivity, however the spectral resolution is currently insufficient to obtain detailed information on chemical structure and molecular interactions. Here we demonstrate more than two orders of magnitude improvement in spectral resolution by performing correlation spectroscopy with shallow nitrogen-vacancy (NV) magnetic sensors in diamond. In principle, the resolution is sufficient to observe chemical shifts in $sim$1 T magnetic fields, and is currently limited by molecular diffusion at the surface. We measure oil diffusion rates of $D = 0.15 - 0.2$,nm$^2/mathrm{mu}$s within (5 nm)$^3$ volumes at the diamond surface.
Considerable evidence suggests that variations in the properties of topological insulators (TIs) at the nanoscale and at interfaces can strongly affect the physics of topological materials. Therefore, a detailed understanding of surface states and interface coupling is crucial to the search for and applications of new topological phases of matter. Currently, no methods can provide depth profiling near surfaces or at interfaces of topologically inequivalent materials. Such a method could advance the study of interactions. Herein we present a non-invasive depth-profiling technique based on $beta$-NMR spectroscopy of radioactive $^8$Li$^+$ ions that can provide one-dimensional imaging in films of fixed thickness and generates nanoscale views of the electronic wavefunctions and magnetic order at topological surfaces and interfaces. By mapping the $^8$Li nuclear resonance near the surface and 10 nm deep into the bulk of pure and Cr-doped bismuth antimony telluride films, we provide signatures related to the TI properties and their topological non-trivial characteristics that affect the electron-nuclear hyperfine field, the metallic shift and magnetic order. These nanoscale variations in $beta$-NMR parameters reflect the unconventional properties of the topological materials under study, and understanding the role of heterogeneities is expected to lead to the discovery of novel phenomena involving quantum materials.
The interaction of organic molecules and molecular aggregates with electromagnetic fields that are strongly confined inside optical cavities within nanoscale volumes, has allowed the observation of exotic quantum regimes of light-matter interaction at room temperature, for a wide variety of cavity materials and geometries. Understanding the universal features of such organic cavities represents a significant challenge for theoretical modelling, as experiments show that these systems are characterized by an intricate competition between coherent and dissipative processes involving entangled nuclear, electronic and photonic degrees of freedom. In this review, we discuss a new theoretical framework that can successfully describe organic cavities under strong light-matter coupling. The theory combines standard concepts in chemical physics and quantum optics to provide a microscopic description of vibronic organic polaritons that is fully consistent with available experiments, and yet is profoundly different from the common view of organic polaritons. We show that by introducing a new class of vibronic polariton wave functions with a photonic component that is dressed by intramolecular vibrations, the new theory can offer a consistent solution to some of the long-standing puzzles in the interpretation of organic cavity photoluminescence. Throughout this review, we confront the predictions of the model with spectroscopic observations, and describe the conditions under which the theory reduces to previous approaches. We finally discuss possible extensions of the theory to account for realistic complexities of organic cavities such spatial inhomogeneities and the multi-mode nature of confined electromagnetic fields.
Nanomagnetometry using the nitrogen-vacancy (NV) centre in diamond has attracted a great deal of interest because of the combined features of room temperature operation, nanoscale resolution and high sensitivity. One of the important goals for nano-magnetometry is to be able to detect nanoscale nuclear magnetic resonance (NMR) in individual molecules. Our theoretical analysis shows how a single molecule at the surface of diamond, with characteristic NMR frequencies, can be detected using a proximate NV centre on a time scale of order seconds with nanometer precision. We perform spatio-temporal resolution optimisation and also outline paths to greater sensitivity. In addition, the method is suitable for application in low and relatively inhomogeneous background magnetic fields in contrast to both conventional liquid and solid state NMR spectroscopy.
We use multiple quantum (MQ) NMR dynamics of a gas of spin-carrying molecules in nanocavities at high and low temperatures for an investigation of many-particle entanglement. A distribution of MQ NMR intensities is obtained at high and low temperatures in a system of 201 spins 1/2. The second moment of the distribution, which provides a lower bound on the quantum Fisher information, sheds light on the many-particle entanglement in the system. The dependence of the many-particle entanglement on the temperature is investigated. Almost all spins are entangled at low temperatures.
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