Prospects for nuclear spin hyperpolarization of molecular samples using nitrogen-vacancy centers in diamond

Tetienne, J.‐P.; Hall, Liam T.; Healey, A. J.; White, Gregory A. L.; Sani, Marc‐Antoine; Separovic, Frances; Hollenberg, Lloyd C. L.

doi:10.1103/physrevb.103.014434

Cited by 31 publications

(38 citation statements)

References 79 publications

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“…We assume that, for each spinlock duration used in the experiment, such an excess of depolarization observed in the matched case versus the nonmatched one is due to spin polarization transfer to the nuclear target. Thus, the contribution due to relaxation mechanisms can be distinguished from the polarization transfer by simply subtracting the two curves ( [8]) (Fig. 4 b), d) and f)).…”

Section: Resultsmentioning

confidence: 99%

“…To each of these, specific rate constants are associated and in particular: k SI = k IS and k T 1ρ are the rates for the polarization transfer and the NV T 1ρ relaxation, respectively and have been measured experimentally as reported above. The nuclear relaxation k T1n and the spin diffusion k SD rates are both estimated based on data reported in the literature [8,16,37] (see Appendix 4). Simulations have been performed calculating for each repetition of the sequence the change of the nuclear and electron spin polarizations obtained by the solution of the system of equations reported in Appendix 4.…”

Section: Discussionmentioning

confidence: 99%

“…To overcome the issue, hyperpolarization methods, such as Dynamic Nuclear Polarization (DNP), have emerged consisting of well-suited microwave (MW) irradiation schemes that allow to transfer the higher thermal polarization of the electron spins to the target nuclei [1][2][3][4]. In contrast, the electronic spin of the NV-center in diamond can be highly polarized by optical excitation at room temperature and coherently manipulated, forming a promising hyperpolarization platform [5][6][7][8]. Although direct detection of spin polarization build-up has not been demonstrated yet for nuclei external to the diamond, the polarization transfer from NV centers to nuclear spins has been accomplished either within the (nano)diamond lattice [9][10][11][12][13] or from single NV centers to small external nuclear ensembles.…”

Section: Introductionmentioning

confidence: 99%

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Polarization transfer from optically-pumped NV center ensembles to multinuclear spin baths

Rizzato¹,

Bruckmaier²,

Liu³

et al. 2021

Preprint

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NV-diamonds have attracted keen interest for nanoscale sensing and spin manipulation. In particular, the non-equilibrium electron spin polarization after optical excitation of single NV centers has successfully been transferred to nuclear spin baths in the surrounding of the defects. However, these experiments need to be extended to NV-ensembles which have promising practical applications in the hyperpolarization of bulk sample volumes for NMR signal enhancement. Here, we use a dense, shallow ensemble of NV-centers to demonstrate polarization transfer to nuclear spins in a well-defined composite diamond sample system. This allows us to address three different types of nuclear spins in different positions with respect to the NV polarization source: from the close proximity of 13 C inside the diamond lattice to the self-assembled molecular system consisting of 1 H and 19 F spins outside the diamond and over multiple interfaces. We show that ensemble NV experiments face problems different from single NV experiments. In particular, using spinlock pulses, the inhomogeneously broadened ESR line of the NV ensemble limits the minimal resonance linewidth with which the transfer protocol can occur. Furthermore, we compare the NV spin-polarization losses and polarization transfer rates to the different nuclear baths and discuss the role of spin-diffusion as detrimentally affecting the direct observation of nuclear polarization build-up within the detection volume of nanoscale NV-NMR experiments.

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Section: Resultsmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Polarization transfer from optically-pumped NV center ensembles to multinuclear spin baths

Rizzato¹,

Bruckmaier²,

Liu³

et al. 2021

Preprint

View full text Add to dashboard Cite

show abstract

“…Under appropriate dynamical decoupling the rotating frame lifetimes can be extended further T 1q > 1s. It is attractive to consider these coherent nuclei, especially when enriched, as a relay medium to transfer polarization to external molecules tethered to the diamond surface [7,11,15].…”

Section: Introductionmentioning

confidence: 99%

Low-field microwave-mediated optical hyperpolarization in optically pumped diamond

Ajoy

Adrisha

Druga

et al. 2021

Journal of Magnetic Resonance

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The emergence of a new class of optically polarizable electronic spins in diamond, nitrogen vacancy (NV) defect centers, has opened interesting new avenues for dynamic nuclear polarization. Here we review methods for the room-temperature hyperpolarization of lattice 13 C nuclei using optically pumped NV centers, focusing particular attention to a polarization transfer via rotating-frame level anti-crossings. We describe special features of this optical DNP mechanism at low-field, in particular, its deployability to randomly oriented diamond nanoparticles. In addition, we detail methods for indirectly obtaining high-resolution NV ESR spectra via hyperpolarization readout. These mechanistic features provide perspectives for interesting new applications exploiting the optically generated 13 C hyperpolarization.

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“…The pioneering studies have been reported on target nuclear spin hyperpolarization using nonequilibrium electron spin polarization in the nitrogen-vacancy (NV) center of diamonds. [18][19][20][21][22][23] However, since the polarization is directly transferred from the electron spins of the NV center to the target nuclear spins by the solid effect, the polarizable region is limited to a small scale near the diamond surface and the polarizable target is limited to solids or highly-viscous liquids. Therefore, how to transfer the polarization from non-equilibrium electron spins in solids to the nuclear spins in bulk liquid water is an extremely important but unsolved problem.…”

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confidence: 99%

Proton Hyperpolarization Relay from Nanocrystals to Liquid Water

Matsumoto

Nishimura

Kimizuka

et al. 2022

Preprint

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Dynamic nuclear polarization (DNP) using transient electron spin polarization generated by photoexcitation can improve nuclear magnetic resonance (NMR) sensitivity far beyond the thermal equilibrium limit for analysis in life science and drug discovery. However, DNP of liquid water at room temperature remains an important challenge. In previous studies, polarization has been transferred directly from the electron spins in the solid to the nuclear spins of the target, and this has been limited to near-surface solid or highly-viscous targets. Here, we propose a new method called hyperpolarization relay, in which the polarization of electron spins is transferred to proton spins in the nanocrystals and then to proton spins in bulk water by the nuclear Overhauser effect (NOE). Molecular nanocrystals doped with a polarizing agent that generates a highly-polarized photoexcited triplet were synthesized by a reprecipitation method while controlling the size of the nanocrystals. As the size of the nanocrystals decreases, the efficiency of polarization transfer from nanocrystals to water was improved due to the increase in the surface area.

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Prospects for nuclear spin hyperpolarization of molecular samples using nitrogen-vacancy centers in diamond

Cited by 31 publications

References 79 publications

Polarization transfer from optically-pumped NV center ensembles to multinuclear spin baths

Polarization transfer from optically-pumped NV center ensembles to multinuclear spin baths

Low-field microwave-mediated optical hyperpolarization in optically pumped diamond

Proton Hyperpolarization Relay from Nanocrystals to Liquid Water

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