Abstract

Nitrogen vacancy (NV) color centers in diamond are a leading modality for both superresolution optical imaging and nanoscale magnetic field sensing. In this work, we address the key challenge of performing optical magnetic imaging and spectroscopy selectively on multiple NV centers that are located within a diffraction-limited field-of-view. We use spin-RESOLFT microscopy to enable precision nanoscale mapping of magnetic field patterns with resolution down to ~20 nm, while employing a low power optical depletion beam. Moreover, we use a shallow NV to demonstrate the detection of proton nuclear magnetic resonance (NMR) signals exterior to the diamond, with 50 nm lateral imaging resolution and without degrading the proton NMR linewidth.

© 2017 Optical Society of America

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2016 (4)

I. Lovchinsky, A. O. Sushkov, E. Urbach, N. P. de Leon, S. Choi, K. De Greve, R. Evans, R. Gertner, E. Bersin, C. Müller, L. McGuinness, F. Jelezko, R. L. Walsworth, H. Park, and M. D. Lukin, “Nuclear magnetic resonance detection and spectroscopy of single proteins using quantum logic,” Science 351(6275), 836–841 (2016).
[Crossref] [PubMed]

J. F. Barry, M. J. Turner, J. M. Schloss, D. R. Glenn, Y. Song, M. D. Lukin, H. Park, and R. L. Walsworth, “Optical magnetic detection of single-neuron action potentials using quantum defects in diamond,” Proc. Natl. Acad. Sci. U.S.A. 113(49), 14133–14138 (2016).
[Crossref] [PubMed]

V. Zablotskii, T. Polyakova, O. Lunov, and A. Dejneka, “How a high-gradient magnetic field could affect cell life,” Sci. Rep. 6(1), 37407 (2016).
[Crossref] [PubMed]

L. M. Pham, S. J. DeVience, F. Casola, I. Lovchinsky, A. O. Sushkov, E. Bersin, J. Lee, E. Urbach, P. Cappellaro, H. Park, A. Yacoby, M. Lukin, and R. L. Walsworth, “NMR technique for determining the depth of shallow nitrogen-vacancy centers in diamond,” Phys. Rev. B 93(4), 045425 (2016).
[Crossref]

2015 (5)

M. Kim, H. J. Mamin, M. H. Sherwood, K. Ohno, D. D. Awschalom, and D. Rugar, “Decoherence of near-surface nitrogen-vacancy centers due to electric field noise,” Phys. Rev. Lett. 115(8), 087602 (2015).
[Crossref] [PubMed]

S. J. DeVience, L. M. Pham, I. Lovchinsky, A. O. Sushkov, N. Bar-Gill, C. Belthangady, F. Casola, M. Corbett, H. Zhang, M. Lukin, H. Park, A. Yacoby, and R. L. Walsworth, “Nanoscale NMR spectroscopy and imaging of multiple nuclear species,” Nat. Nanotechnol. 10(2), 129–134 (2015).
[Crossref] [PubMed]

K. Arai, C. Belthangady, H. Zhang, N. Bar-Gill, S. J. DeVience, P. Cappellaro, A. Yacoby, and R. L. Walsworth, “Fourier magnetic imaging with nanoscale resolution and compressed sensing speed-up using electronic spins in diamond,” Nat. Nanotechnol. 10(10), 859–864 (2015).
[Crossref] [PubMed]

T. van der Sar, F. Casola, R. Walsworth, and A. Yacoby, “Nanometre-scale probing of spin waves using single-electron spins,” Nat. Commun. 6, 7886 (2015).
[Crossref] [PubMed]

D. R. Glenn, K. Lee, H. Park, R. Weissleder, A. Yacoby, M. D. Lukin, H. Lee, R. L. Walsworth, and C. B. Connolly, “Single-cell magnetic imaging using a quantum diamond microscope,” Nat. Methods 12(8), 736–738 (2015).
[Crossref] [PubMed]

2014 (7)

R. R. Fu, B. P. Weiss, E. A. Lima, R. J. Harrison, X.-N. Bai, S. J. Desch, D. S. Ebel, C. Suavet, H. Wang, D. Glenn, D. Le Sage, T. Kasama, R. L. Walsworth, and A. T. Kuan, “Solar nebula magnetic fields recorded in the Semarkona meteorite,” Science 346(6213), 1089–1092 (2014).
[Crossref] [PubMed]

A. O. Sushkov, I. Lovchinsky, N. Chisholm, R. L. Walsworth, H. Park, and M. D. Lukin, “Magnetic resonance detection of individual proton spins using quantum reporters,” Phys. Rev. Lett. 113(19), 197601 (2014).
[Crossref] [PubMed]

M. S. Grinolds, M. Warner, K. De Greve, Y. Dovzhenko, L. Thiel, R. L. Walsworth, S. Hong, P. Maletinsky, and A. Yacoby, “Subnanometre resolution in three-dimensional magnetic resonance imaging of individual dark spins,” Nat. Nanotechnol. 9(4), 279–284 (2014).
[Crossref] [PubMed]

M. Pfender, N. Aslam, G. Waldherr, P. Neumann, and J. Wrachtrup, “Single-spin stochastic optical reconstruction microscopy,” Proc. Natl. Acad. Sci. U.S.A. 111(41), 14669–14674 (2014).
[Crossref] [PubMed]

S. Arroyo-Camejo, A. Lazariev, S. W. Hell, and G. Balasubramanian, “Room temperature high-fidelity holonomic single-qubit gate on a solid-state spin,” Nat. Commun. 5, 4870 (2014).
[Crossref] [PubMed]

F. Dolde, M. W. Doherty, J. Michl, I. Jakobi, B. Naydenov, S. Pezzagna, J. Meijer, P. Neumann, F. Jelezko, N. B. Manson, and J. Wrachtrup, “Nanoscale detection of a single fundamental charge in ambient conditions using the NV- center in diamond,” Phys. Rev. Lett. 112(9), 097603 (2014).
[Crossref] [PubMed]

C. Grezes, B. Julsgaard, Y. Kubo, M. Stern, T. Umeda, J. Isoya, H. Sumiya, H. Abe, S. Onoda, T. Ohshima, V. Jacques, J. Esteve, D. Vion, D. Esteve, K. Mølmer, and P. Bertet, “Multimode storage and retrieval of microwave fields in a spin ensemble,” Phys. Rev. X 4(2), 021049 (2014).
[Crossref]

2013 (10)

M. S. Grinolds, S. Hong, P. Maletinsky, L. Luan, M. D. Lukin, R. L. Walsworth, and A. Yacoby, “Nanoscale magnetic imaging of a single electron spin under ambient conditions,” Nat. Phys. 9(4), 215–219 (2013).
[Crossref]

T. Staudacher, F. Shi, S. Pezzagna, J. Meijer, J. Du, C. A. Meriles, F. Reinhard, and J. Wrachtrup, “Nuclear magnetic resonance spectroscopy on a (5-nanometer)3 sample volume,” Science 339(6119), 561–563 (2013).
[Crossref] [PubMed]

H. J. Mamin, M. Kim, M. H. Sherwood, C. T. Rettner, K. Ohno, D. D. Awschalom, and D. Rugar, “Nanoscale nuclear magnetic resonance with a nitrogen-vacancy spin sensor,” Science 339(6119), 557–560 (2013).
[Crossref] [PubMed]

S. Arroyo-Camejo, M.-P. Adam, M. Besbes, J.-P. Hugonin, V. Jacques, J.-J. Greffet, J.-F. Roch, S. W. Hell, and F. Treussart, “Stimulated emission depletion microscopy resolves individual nitrogen vacancy centers in diamond nanocrystals,” ACS Nano 7(12), 10912–10919 (2013).
[Crossref] [PubMed]

E. H. Chen, O. Gaathon, M. E. Trusheim, and D. Englund, “Wide-field multispectral super-resolution imaging using spin-dependent fluorescence in nanodiamonds,” Nano Lett. 13(5), 2073–2077 (2013).
[Crossref] [PubMed]

D. Le Sage, K. Arai, D. R. Glenn, S. J. DeVience, L. M. Pham, L. Rahn-Lee, M. D. Lukin, A. Yacoby, A. Komeili, and R. L. Walsworth, “Optical magnetic imaging of living cells,” Nature 496(7446), 486–489 (2013).
[Crossref] [PubMed]

M. W. Doherty, N. B. Manson, P. Delaney, F. Jelezko, J. Wrachtrup, and L. C. L. Hollenberg, “The nitrogen-vacancy colour centre in diamond,” Phys. Rep. 528(1), 1–45 (2013).
[Crossref]

L. Rondin, J.-P. Tetienne, S. Rohart, A. Thiaville, T. Hingant, P. Spinicelli, J.-F. Roch, and V. Jacques, “Stray-field imaging of magnetic vortices with a single diamond spin,” Nat. Commun. 4, 2279 (2013).
[Crossref] [PubMed]

F. Dolde, I. Jakobi, B. Naydenov, N. Zhao, S. Pezzagna, C. Trautmann, J. Meijer, P. Neumann, F. Jelezko, and J. Wrachtrup, “Room-temperature entanglement between single defect spins in diamond,” Nat. Phys. 9(3), 139–143 (2013).
[Crossref]

J. Cai, A. Retzker, F. Jelezko, and M. B. Plenio, “A large-scale quantum simulator on a diamond surface at room temperature,” Nat. Phys. 9(3), 168–173 (2013).
[Crossref]

2012 (1)

N. Bar-Gill, L. M. Pham, C. Belthangady, D. Le Sage, P. Cappellaro, J. R. Maze, M. D. Lukin, A. Yacoby, and R. Walsworth, “Suppression of spin-bath dynamics for improved coherence of multi-spin-qubit systems,” Nat. Commun. 3, 858 (2012).
[Crossref] [PubMed]

2011 (4)

D. Wildanger, J. R. Maze, and S. W. Hell, “Diffraction unlimited all-optical recording of electron spin resonances,” Phys. Rev. Lett. 107(1), 017601 (2011).
[Crossref] [PubMed]

F. Dolde, H. Fedder, M. W. Doherty, T. Nöbauer, F. Rempp, G. Balasubramanian, T. Wolf, F. Reinhard, L. C. L. Hollenberg, F. Jelezko, and J. Wrachtrup, “Electric-field sensing using single diamond spins,” Nat. Phys. 7(6), 459–463 (2011).
[Crossref]

M. S. Grinolds, P. Maletinsky, S. Hong, M. D. Lukin, R. L. Walsworth, and A. Yacoby, “Quantum control of proximal spins using nanoscale magnetic resonance imaging,” Nat. Phys. 7(9), 687–692 (2011).
[Crossref]

L. Robledo, H. Bernien, T. Van der Sar, and R. Hanson, “Spin dynamics in the optical cycle of single nitrogen-vacancy centres in diamond,” New J. Phys. 13(2), 025013 (2011).
[Crossref]

2010 (4)

V. M. Acosta, E. Bauch, M. P. Ledbetter, A. Waxman, L.-S. Bouchard, and D. Budker, “Temperature dependence of the nitrogen-vacancy magnetic resonance in diamond,” Phys. Rev. Lett. 104(7), 070801 (2010).
[Crossref] [PubMed]

G. de Lange, Z. H. Wang, D. Ristè, V. V. Dobrovitski, and R. Hanson, “Universal dynamical decoupling of a single solid-state spin from a spin bath,” Science 330(6000), 60–63 (2010).
[Crossref] [PubMed]

K. Y. Han, S. K. Kim, C. Eggeling, and S. W. Hell, “Metastable dark States enable ground state depletion microscopy of nitrogen vacancy centers in diamond with diffraction-unlimited resolution,” Nano Lett. 10(8), 3199–3203 (2010).
[Crossref] [PubMed]

P. C. Maurer, J. R. Maze, P. L. Stanwix, L. Jiang, A. V. Gorshkov, A. A. Zibrov, B. Harke, J. S. Hodges, A. S. Zibrov, A. Yacoby, D. Twitchen, S. W. Hell, R. L. Walsworth, and M. D. Lukin, “Far-field optical imaging and manipulation of individual spins with nanoscale resolution,” Nat. Phys. 6(11), 912–918 (2010).
[Crossref]

2009 (1)

E. Rittweger, K. Y. Han, S. E. Irvine, C. Eggeling, and S. W. Hell, “STED microscopy reveals crystal colour centres with nanometric resolution,” Nat. Photonics 3(3), 144–147 (2009).
[Crossref]

2008 (3)

J. R. Maze, P. L. Stanwix, J. S. Hodges, S. Hong, J. M. Taylor, P. Cappellaro, L. Jiang, M. V. G. Dutt, E. Togan, A. S. Zibrov, A. Yacoby, R. L. Walsworth, and M. D. Lukin, “Nanoscale magnetic sensing with an individual electronic spin in diamond,” Nature 455(7213), 644–647 (2008).
[Crossref] [PubMed]

J. M. Taylor, P. Cappellaro, L. Childress, L. Jiang, D. Budker, P. R. Hemmer, A. Yacoby, R. Walsworth, and M. D. Lukin, “High-sensitivity diamond magnetometer with nanoscale resolution,” Nat. Phys. 4(10), 810–816 (2008).
[Crossref]

G. Balasubramanian, I. Y. Chan, R. Kolesov, M. Al-Hmoud, J. Tisler, C. Shin, C. Kim, A. Wojcik, P. R. Hemmer, A. Krueger, T. Hanke, A. Leitenstorfer, R. Bratschitsch, F. Jelezko, and J. Wrachtrup, “Nanoscale imaging magnetometry with diamond spins under ambient conditions,” Nature 455(7213), 648–651 (2008).
[Crossref] [PubMed]

Abe, H.

C. Grezes, B. Julsgaard, Y. Kubo, M. Stern, T. Umeda, J. Isoya, H. Sumiya, H. Abe, S. Onoda, T. Ohshima, V. Jacques, J. Esteve, D. Vion, D. Esteve, K. Mølmer, and P. Bertet, “Multimode storage and retrieval of microwave fields in a spin ensemble,” Phys. Rev. X 4(2), 021049 (2014).
[Crossref]

Acosta, V. M.

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L. M. Pham, S. J. DeVience, F. Casola, I. Lovchinsky, A. O. Sushkov, E. Bersin, J. Lee, E. Urbach, P. Cappellaro, H. Park, A. Yacoby, M. Lukin, and R. L. Walsworth, “NMR technique for determining the depth of shallow nitrogen-vacancy centers in diamond,” Phys. Rev. B 93(4), 045425 (2016).
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K. Arai, C. Belthangady, H. Zhang, N. Bar-Gill, S. J. DeVience, P. Cappellaro, A. Yacoby, and R. L. Walsworth, “Fourier magnetic imaging with nanoscale resolution and compressed sensing speed-up using electronic spins in diamond,” Nat. Nanotechnol. 10(10), 859–864 (2015).
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M. S. Grinolds, P. Maletinsky, S. Hong, M. D. Lukin, R. L. Walsworth, and A. Yacoby, “Quantum control of proximal spins using nanoscale magnetic resonance imaging,” Nat. Phys. 7(9), 687–692 (2011).
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K. Y. Han, S. K. Kim, C. Eggeling, and S. W. Hell, “Metastable dark States enable ground state depletion microscopy of nitrogen vacancy centers in diamond with diffraction-unlimited resolution,” Nano Lett. 10(8), 3199–3203 (2010).
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M. S. Grinolds, P. Maletinsky, S. Hong, M. D. Lukin, R. L. Walsworth, and A. Yacoby, “Quantum control of proximal spins using nanoscale magnetic resonance imaging,” Nat. Phys. 7(9), 687–692 (2011).
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E. Rittweger, K. Y. Han, S. E. Irvine, C. Eggeling, and S. W. Hell, “STED microscopy reveals crystal colour centres with nanometric resolution,” Nat. Photonics 3(3), 144–147 (2009).
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S. Arroyo-Camejo, M.-P. Adam, M. Besbes, J.-P. Hugonin, V. Jacques, J.-J. Greffet, J.-F. Roch, S. W. Hell, and F. Treussart, “Stimulated emission depletion microscopy resolves individual nitrogen vacancy centers in diamond nanocrystals,” ACS Nano 7(12), 10912–10919 (2013).
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F. Dolde, M. W. Doherty, J. Michl, I. Jakobi, B. Naydenov, S. Pezzagna, J. Meijer, P. Neumann, F. Jelezko, N. B. Manson, and J. Wrachtrup, “Nanoscale detection of a single fundamental charge in ambient conditions using the NV- center in diamond,” Phys. Rev. Lett. 112(9), 097603 (2014).
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I. Lovchinsky, A. O. Sushkov, E. Urbach, N. P. de Leon, S. Choi, K. De Greve, R. Evans, R. Gertner, E. Bersin, C. Müller, L. McGuinness, F. Jelezko, R. L. Walsworth, H. Park, and M. D. Lukin, “Nuclear magnetic resonance detection and spectroscopy of single proteins using quantum logic,” Science 351(6275), 836–841 (2016).
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F. Dolde, M. W. Doherty, J. Michl, I. Jakobi, B. Naydenov, S. Pezzagna, J. Meijer, P. Neumann, F. Jelezko, N. B. Manson, and J. Wrachtrup, “Nanoscale detection of a single fundamental charge in ambient conditions using the NV- center in diamond,” Phys. Rev. Lett. 112(9), 097603 (2014).
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F. Dolde, I. Jakobi, B. Naydenov, N. Zhao, S. Pezzagna, C. Trautmann, J. Meijer, P. Neumann, F. Jelezko, and J. Wrachtrup, “Room-temperature entanglement between single defect spins in diamond,” Nat. Phys. 9(3), 139–143 (2013).
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M. W. Doherty, N. B. Manson, P. Delaney, F. Jelezko, J. Wrachtrup, and L. C. L. Hollenberg, “The nitrogen-vacancy colour centre in diamond,” Phys. Rep. 528(1), 1–45 (2013).
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F. Dolde, H. Fedder, M. W. Doherty, T. Nöbauer, F. Rempp, G. Balasubramanian, T. Wolf, F. Reinhard, L. C. L. Hollenberg, F. Jelezko, and J. Wrachtrup, “Electric-field sensing using single diamond spins,” Nat. Phys. 7(6), 459–463 (2011).
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G. Balasubramanian, I. Y. Chan, R. Kolesov, M. Al-Hmoud, J. Tisler, C. Shin, C. Kim, A. Wojcik, P. R. Hemmer, A. Krueger, T. Hanke, A. Leitenstorfer, R. Bratschitsch, F. Jelezko, and J. Wrachtrup, “Nanoscale imaging magnetometry with diamond spins under ambient conditions,” Nature 455(7213), 648–651 (2008).
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P. C. Maurer, J. R. Maze, P. L. Stanwix, L. Jiang, A. V. Gorshkov, A. A. Zibrov, B. Harke, J. S. Hodges, A. S. Zibrov, A. Yacoby, D. Twitchen, S. W. Hell, R. L. Walsworth, and M. D. Lukin, “Far-field optical imaging and manipulation of individual spins with nanoscale resolution,” Nat. Phys. 6(11), 912–918 (2010).
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J. R. Maze, P. L. Stanwix, J. S. Hodges, S. Hong, J. M. Taylor, P. Cappellaro, L. Jiang, M. V. G. Dutt, E. Togan, A. S. Zibrov, A. Yacoby, R. L. Walsworth, and M. D. Lukin, “Nanoscale magnetic sensing with an individual electronic spin in diamond,” Nature 455(7213), 644–647 (2008).
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J. M. Taylor, P. Cappellaro, L. Childress, L. Jiang, D. Budker, P. R. Hemmer, A. Yacoby, R. Walsworth, and M. D. Lukin, “High-sensitivity diamond magnetometer with nanoscale resolution,” Nat. Phys. 4(10), 810–816 (2008).
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R. R. Fu, B. P. Weiss, E. A. Lima, R. J. Harrison, X.-N. Bai, S. J. Desch, D. S. Ebel, C. Suavet, H. Wang, D. Glenn, D. Le Sage, T. Kasama, R. L. Walsworth, and A. T. Kuan, “Solar nebula magnetic fields recorded in the Semarkona meteorite,” Science 346(6213), 1089–1092 (2014).
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G. Balasubramanian, I. Y. Chan, R. Kolesov, M. Al-Hmoud, J. Tisler, C. Shin, C. Kim, A. Wojcik, P. R. Hemmer, A. Krueger, T. Hanke, A. Leitenstorfer, R. Bratschitsch, F. Jelezko, and J. Wrachtrup, “Nanoscale imaging magnetometry with diamond spins under ambient conditions,” Nature 455(7213), 648–651 (2008).
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K. Y. Han, S. K. Kim, C. Eggeling, and S. W. Hell, “Metastable dark States enable ground state depletion microscopy of nitrogen vacancy centers in diamond with diffraction-unlimited resolution,” Nano Lett. 10(8), 3199–3203 (2010).
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D. Le Sage, K. Arai, D. R. Glenn, S. J. DeVience, L. M. Pham, L. Rahn-Lee, M. D. Lukin, A. Yacoby, A. Komeili, and R. L. Walsworth, “Optical magnetic imaging of living cells,” Nature 496(7446), 486–489 (2013).
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G. Balasubramanian, I. Y. Chan, R. Kolesov, M. Al-Hmoud, J. Tisler, C. Shin, C. Kim, A. Wojcik, P. R. Hemmer, A. Krueger, T. Hanke, A. Leitenstorfer, R. Bratschitsch, F. Jelezko, and J. Wrachtrup, “Nanoscale imaging magnetometry with diamond spins under ambient conditions,” Nature 455(7213), 648–651 (2008).
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R. R. Fu, B. P. Weiss, E. A. Lima, R. J. Harrison, X.-N. Bai, S. J. Desch, D. S. Ebel, C. Suavet, H. Wang, D. Glenn, D. Le Sage, T. Kasama, R. L. Walsworth, and A. T. Kuan, “Solar nebula magnetic fields recorded in the Semarkona meteorite,” Science 346(6213), 1089–1092 (2014).
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C. Grezes, B. Julsgaard, Y. Kubo, M. Stern, T. Umeda, J. Isoya, H. Sumiya, H. Abe, S. Onoda, T. Ohshima, V. Jacques, J. Esteve, D. Vion, D. Esteve, K. Mølmer, and P. Bertet, “Multimode storage and retrieval of microwave fields in a spin ensemble,” Phys. Rev. X 4(2), 021049 (2014).
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S. J. DeVience, L. M. Pham, I. Lovchinsky, A. O. Sushkov, N. Bar-Gill, C. Belthangady, F. Casola, M. Corbett, H. Zhang, M. Lukin, H. Park, A. Yacoby, and R. L. Walsworth, “Nanoscale NMR spectroscopy and imaging of multiple nuclear species,” Nat. Nanotechnol. 10(2), 129–134 (2015).
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[Crossref] [PubMed]

J. F. Barry, M. J. Turner, J. M. Schloss, D. R. Glenn, Y. Song, M. D. Lukin, H. Park, and R. L. Walsworth, “Optical magnetic detection of single-neuron action potentials using quantum defects in diamond,” Proc. Natl. Acad. Sci. U.S.A. 113(49), 14133–14138 (2016).
[Crossref] [PubMed]

L. M. Pham, S. J. DeVience, F. Casola, I. Lovchinsky, A. O. Sushkov, E. Bersin, J. Lee, E. Urbach, P. Cappellaro, H. Park, A. Yacoby, M. Lukin, and R. L. Walsworth, “NMR technique for determining the depth of shallow nitrogen-vacancy centers in diamond,” Phys. Rev. B 93(4), 045425 (2016).
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S. J. DeVience, L. M. Pham, I. Lovchinsky, A. O. Sushkov, N. Bar-Gill, C. Belthangady, F. Casola, M. Corbett, H. Zhang, M. Lukin, H. Park, A. Yacoby, and R. L. Walsworth, “Nanoscale NMR spectroscopy and imaging of multiple nuclear species,” Nat. Nanotechnol. 10(2), 129–134 (2015).
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D. R. Glenn, K. Lee, H. Park, R. Weissleder, A. Yacoby, M. D. Lukin, H. Lee, R. L. Walsworth, and C. B. Connolly, “Single-cell magnetic imaging using a quantum diamond microscope,” Nat. Methods 12(8), 736–738 (2015).
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A. O. Sushkov, I. Lovchinsky, N. Chisholm, R. L. Walsworth, H. Park, and M. D. Lukin, “Magnetic resonance detection of individual proton spins using quantum reporters,” Phys. Rev. Lett. 113(19), 197601 (2014).
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F. Dolde, M. W. Doherty, J. Michl, I. Jakobi, B. Naydenov, S. Pezzagna, J. Meijer, P. Neumann, F. Jelezko, N. B. Manson, and J. Wrachtrup, “Nanoscale detection of a single fundamental charge in ambient conditions using the NV- center in diamond,” Phys. Rev. Lett. 112(9), 097603 (2014).
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T. Staudacher, F. Shi, S. Pezzagna, J. Meijer, J. Du, C. A. Meriles, F. Reinhard, and J. Wrachtrup, “Nuclear magnetic resonance spectroscopy on a (5-nanometer)3 sample volume,” Science 339(6119), 561–563 (2013).
[Crossref] [PubMed]

F. Dolde, I. Jakobi, B. Naydenov, N. Zhao, S. Pezzagna, C. Trautmann, J. Meijer, P. Neumann, F. Jelezko, and J. Wrachtrup, “Room-temperature entanglement between single defect spins in diamond,” Nat. Phys. 9(3), 139–143 (2013).
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D. Le Sage, K. Arai, D. R. Glenn, S. J. DeVience, L. M. Pham, L. Rahn-Lee, M. D. Lukin, A. Yacoby, A. Komeili, and R. L. Walsworth, “Optical magnetic imaging of living cells,” Nature 496(7446), 486–489 (2013).
[Crossref] [PubMed]

N. Bar-Gill, L. M. Pham, C. Belthangady, D. Le Sage, P. Cappellaro, J. R. Maze, M. D. Lukin, A. Yacoby, and R. Walsworth, “Suppression of spin-bath dynamics for improved coherence of multi-spin-qubit systems,” Nat. Commun. 3, 858 (2012).
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T. Staudacher, F. Shi, S. Pezzagna, J. Meijer, J. Du, C. A. Meriles, F. Reinhard, and J. Wrachtrup, “Nuclear magnetic resonance spectroscopy on a (5-nanometer)3 sample volume,” Science 339(6119), 561–563 (2013).
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Yacoby, A.

L. M. Pham, S. J. DeVience, F. Casola, I. Lovchinsky, A. O. Sushkov, E. Bersin, J. Lee, E. Urbach, P. Cappellaro, H. Park, A. Yacoby, M. Lukin, and R. L. Walsworth, “NMR technique for determining the depth of shallow nitrogen-vacancy centers in diamond,” Phys. Rev. B 93(4), 045425 (2016).
[Crossref]

T. van der Sar, F. Casola, R. Walsworth, and A. Yacoby, “Nanometre-scale probing of spin waves using single-electron spins,” Nat. Commun. 6, 7886 (2015).
[Crossref] [PubMed]

S. J. DeVience, L. M. Pham, I. Lovchinsky, A. O. Sushkov, N. Bar-Gill, C. Belthangady, F. Casola, M. Corbett, H. Zhang, M. Lukin, H. Park, A. Yacoby, and R. L. Walsworth, “Nanoscale NMR spectroscopy and imaging of multiple nuclear species,” Nat. Nanotechnol. 10(2), 129–134 (2015).
[Crossref] [PubMed]

D. R. Glenn, K. Lee, H. Park, R. Weissleder, A. Yacoby, M. D. Lukin, H. Lee, R. L. Walsworth, and C. B. Connolly, “Single-cell magnetic imaging using a quantum diamond microscope,” Nat. Methods 12(8), 736–738 (2015).
[Crossref] [PubMed]

K. Arai, C. Belthangady, H. Zhang, N. Bar-Gill, S. J. DeVience, P. Cappellaro, A. Yacoby, and R. L. Walsworth, “Fourier magnetic imaging with nanoscale resolution and compressed sensing speed-up using electronic spins in diamond,” Nat. Nanotechnol. 10(10), 859–864 (2015).
[Crossref] [PubMed]

M. S. Grinolds, M. Warner, K. De Greve, Y. Dovzhenko, L. Thiel, R. L. Walsworth, S. Hong, P. Maletinsky, and A. Yacoby, “Subnanometre resolution in three-dimensional magnetic resonance imaging of individual dark spins,” Nat. Nanotechnol. 9(4), 279–284 (2014).
[Crossref] [PubMed]

D. Le Sage, K. Arai, D. R. Glenn, S. J. DeVience, L. M. Pham, L. Rahn-Lee, M. D. Lukin, A. Yacoby, A. Komeili, and R. L. Walsworth, “Optical magnetic imaging of living cells,” Nature 496(7446), 486–489 (2013).
[Crossref] [PubMed]

M. S. Grinolds, S. Hong, P. Maletinsky, L. Luan, M. D. Lukin, R. L. Walsworth, and A. Yacoby, “Nanoscale magnetic imaging of a single electron spin under ambient conditions,” Nat. Phys. 9(4), 215–219 (2013).
[Crossref]

N. Bar-Gill, L. M. Pham, C. Belthangady, D. Le Sage, P. Cappellaro, J. R. Maze, M. D. Lukin, A. Yacoby, and R. Walsworth, “Suppression of spin-bath dynamics for improved coherence of multi-spin-qubit systems,” Nat. Commun. 3, 858 (2012).
[Crossref] [PubMed]

M. S. Grinolds, P. Maletinsky, S. Hong, M. D. Lukin, R. L. Walsworth, and A. Yacoby, “Quantum control of proximal spins using nanoscale magnetic resonance imaging,” Nat. Phys. 7(9), 687–692 (2011).
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P. C. Maurer, J. R. Maze, P. L. Stanwix, L. Jiang, A. V. Gorshkov, A. A. Zibrov, B. Harke, J. S. Hodges, A. S. Zibrov, A. Yacoby, D. Twitchen, S. W. Hell, R. L. Walsworth, and M. D. Lukin, “Far-field optical imaging and manipulation of individual spins with nanoscale resolution,” Nat. Phys. 6(11), 912–918 (2010).
[Crossref]

J. R. Maze, P. L. Stanwix, J. S. Hodges, S. Hong, J. M. Taylor, P. Cappellaro, L. Jiang, M. V. G. Dutt, E. Togan, A. S. Zibrov, A. Yacoby, R. L. Walsworth, and M. D. Lukin, “Nanoscale magnetic sensing with an individual electronic spin in diamond,” Nature 455(7213), 644–647 (2008).
[Crossref] [PubMed]

J. M. Taylor, P. Cappellaro, L. Childress, L. Jiang, D. Budker, P. R. Hemmer, A. Yacoby, R. Walsworth, and M. D. Lukin, “High-sensitivity diamond magnetometer with nanoscale resolution,” Nat. Phys. 4(10), 810–816 (2008).
[Crossref]

Zablotskii, V.

V. Zablotskii, T. Polyakova, O. Lunov, and A. Dejneka, “How a high-gradient magnetic field could affect cell life,” Sci. Rep. 6(1), 37407 (2016).
[Crossref] [PubMed]

Zhang, H.

S. J. DeVience, L. M. Pham, I. Lovchinsky, A. O. Sushkov, N. Bar-Gill, C. Belthangady, F. Casola, M. Corbett, H. Zhang, M. Lukin, H. Park, A. Yacoby, and R. L. Walsworth, “Nanoscale NMR spectroscopy and imaging of multiple nuclear species,” Nat. Nanotechnol. 10(2), 129–134 (2015).
[Crossref] [PubMed]

K. Arai, C. Belthangady, H. Zhang, N. Bar-Gill, S. J. DeVience, P. Cappellaro, A. Yacoby, and R. L. Walsworth, “Fourier magnetic imaging with nanoscale resolution and compressed sensing speed-up using electronic spins in diamond,” Nat. Nanotechnol. 10(10), 859–864 (2015).
[Crossref] [PubMed]

Zhao, N.

F. Dolde, I. Jakobi, B. Naydenov, N. Zhao, S. Pezzagna, C. Trautmann, J. Meijer, P. Neumann, F. Jelezko, and J. Wrachtrup, “Room-temperature entanglement between single defect spins in diamond,” Nat. Phys. 9(3), 139–143 (2013).
[Crossref]

Zibrov, A. A.

P. C. Maurer, J. R. Maze, P. L. Stanwix, L. Jiang, A. V. Gorshkov, A. A. Zibrov, B. Harke, J. S. Hodges, A. S. Zibrov, A. Yacoby, D. Twitchen, S. W. Hell, R. L. Walsworth, and M. D. Lukin, “Far-field optical imaging and manipulation of individual spins with nanoscale resolution,” Nat. Phys. 6(11), 912–918 (2010).
[Crossref]

Zibrov, A. S.

P. C. Maurer, J. R. Maze, P. L. Stanwix, L. Jiang, A. V. Gorshkov, A. A. Zibrov, B. Harke, J. S. Hodges, A. S. Zibrov, A. Yacoby, D. Twitchen, S. W. Hell, R. L. Walsworth, and M. D. Lukin, “Far-field optical imaging and manipulation of individual spins with nanoscale resolution,” Nat. Phys. 6(11), 912–918 (2010).
[Crossref]

J. R. Maze, P. L. Stanwix, J. S. Hodges, S. Hong, J. M. Taylor, P. Cappellaro, L. Jiang, M. V. G. Dutt, E. Togan, A. S. Zibrov, A. Yacoby, R. L. Walsworth, and M. D. Lukin, “Nanoscale magnetic sensing with an individual electronic spin in diamond,” Nature 455(7213), 644–647 (2008).
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ACS Nano (1)

S. Arroyo-Camejo, M.-P. Adam, M. Besbes, J.-P. Hugonin, V. Jacques, J.-J. Greffet, J.-F. Roch, S. W. Hell, and F. Treussart, “Stimulated emission depletion microscopy resolves individual nitrogen vacancy centers in diamond nanocrystals,” ACS Nano 7(12), 10912–10919 (2013).
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Nano Lett. (2)

K. Y. Han, S. K. Kim, C. Eggeling, and S. W. Hell, “Metastable dark States enable ground state depletion microscopy of nitrogen vacancy centers in diamond with diffraction-unlimited resolution,” Nano Lett. 10(8), 3199–3203 (2010).
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E. H. Chen, O. Gaathon, M. E. Trusheim, and D. Englund, “Wide-field multispectral super-resolution imaging using spin-dependent fluorescence in nanodiamonds,” Nano Lett. 13(5), 2073–2077 (2013).
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Nat. Commun. (4)

L. Rondin, J.-P. Tetienne, S. Rohart, A. Thiaville, T. Hingant, P. Spinicelli, J.-F. Roch, and V. Jacques, “Stray-field imaging of magnetic vortices with a single diamond spin,” Nat. Commun. 4, 2279 (2013).
[Crossref] [PubMed]

T. van der Sar, F. Casola, R. Walsworth, and A. Yacoby, “Nanometre-scale probing of spin waves using single-electron spins,” Nat. Commun. 6, 7886 (2015).
[Crossref] [PubMed]

N. Bar-Gill, L. M. Pham, C. Belthangady, D. Le Sage, P. Cappellaro, J. R. Maze, M. D. Lukin, A. Yacoby, and R. Walsworth, “Suppression of spin-bath dynamics for improved coherence of multi-spin-qubit systems,” Nat. Commun. 3, 858 (2012).
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S. Arroyo-Camejo, A. Lazariev, S. W. Hell, and G. Balasubramanian, “Room temperature high-fidelity holonomic single-qubit gate on a solid-state spin,” Nat. Commun. 5, 4870 (2014).
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Nat. Methods (1)

D. R. Glenn, K. Lee, H. Park, R. Weissleder, A. Yacoby, M. D. Lukin, H. Lee, R. L. Walsworth, and C. B. Connolly, “Single-cell magnetic imaging using a quantum diamond microscope,” Nat. Methods 12(8), 736–738 (2015).
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Nat. Nanotechnol. (3)

M. S. Grinolds, M. Warner, K. De Greve, Y. Dovzhenko, L. Thiel, R. L. Walsworth, S. Hong, P. Maletinsky, and A. Yacoby, “Subnanometre resolution in three-dimensional magnetic resonance imaging of individual dark spins,” Nat. Nanotechnol. 9(4), 279–284 (2014).
[Crossref] [PubMed]

K. Arai, C. Belthangady, H. Zhang, N. Bar-Gill, S. J. DeVience, P. Cappellaro, A. Yacoby, and R. L. Walsworth, “Fourier magnetic imaging with nanoscale resolution and compressed sensing speed-up using electronic spins in diamond,” Nat. Nanotechnol. 10(10), 859–864 (2015).
[Crossref] [PubMed]

S. J. DeVience, L. M. Pham, I. Lovchinsky, A. O. Sushkov, N. Bar-Gill, C. Belthangady, F. Casola, M. Corbett, H. Zhang, M. Lukin, H. Park, A. Yacoby, and R. L. Walsworth, “Nanoscale NMR spectroscopy and imaging of multiple nuclear species,” Nat. Nanotechnol. 10(2), 129–134 (2015).
[Crossref] [PubMed]

Nat. Photonics (1)

E. Rittweger, K. Y. Han, S. E. Irvine, C. Eggeling, and S. W. Hell, “STED microscopy reveals crystal colour centres with nanometric resolution,” Nat. Photonics 3(3), 144–147 (2009).
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Nat. Phys. (7)

F. Dolde, H. Fedder, M. W. Doherty, T. Nöbauer, F. Rempp, G. Balasubramanian, T. Wolf, F. Reinhard, L. C. L. Hollenberg, F. Jelezko, and J. Wrachtrup, “Electric-field sensing using single diamond spins,” Nat. Phys. 7(6), 459–463 (2011).
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J. M. Taylor, P. Cappellaro, L. Childress, L. Jiang, D. Budker, P. R. Hemmer, A. Yacoby, R. Walsworth, and M. D. Lukin, “High-sensitivity diamond magnetometer with nanoscale resolution,” Nat. Phys. 4(10), 810–816 (2008).
[Crossref]

F. Dolde, I. Jakobi, B. Naydenov, N. Zhao, S. Pezzagna, C. Trautmann, J. Meijer, P. Neumann, F. Jelezko, and J. Wrachtrup, “Room-temperature entanglement between single defect spins in diamond,” Nat. Phys. 9(3), 139–143 (2013).
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J. Cai, A. Retzker, F. Jelezko, and M. B. Plenio, “A large-scale quantum simulator on a diamond surface at room temperature,” Nat. Phys. 9(3), 168–173 (2013).
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P. C. Maurer, J. R. Maze, P. L. Stanwix, L. Jiang, A. V. Gorshkov, A. A. Zibrov, B. Harke, J. S. Hodges, A. S. Zibrov, A. Yacoby, D. Twitchen, S. W. Hell, R. L. Walsworth, and M. D. Lukin, “Far-field optical imaging and manipulation of individual spins with nanoscale resolution,” Nat. Phys. 6(11), 912–918 (2010).
[Crossref]

M. S. Grinolds, S. Hong, P. Maletinsky, L. Luan, M. D. Lukin, R. L. Walsworth, and A. Yacoby, “Nanoscale magnetic imaging of a single electron spin under ambient conditions,” Nat. Phys. 9(4), 215–219 (2013).
[Crossref]

M. S. Grinolds, P. Maletinsky, S. Hong, M. D. Lukin, R. L. Walsworth, and A. Yacoby, “Quantum control of proximal spins using nanoscale magnetic resonance imaging,” Nat. Phys. 7(9), 687–692 (2011).
[Crossref]

Nature (3)

G. Balasubramanian, I. Y. Chan, R. Kolesov, M. Al-Hmoud, J. Tisler, C. Shin, C. Kim, A. Wojcik, P. R. Hemmer, A. Krueger, T. Hanke, A. Leitenstorfer, R. Bratschitsch, F. Jelezko, and J. Wrachtrup, “Nanoscale imaging magnetometry with diamond spins under ambient conditions,” Nature 455(7213), 648–651 (2008).
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D. Le Sage, K. Arai, D. R. Glenn, S. J. DeVience, L. M. Pham, L. Rahn-Lee, M. D. Lukin, A. Yacoby, A. Komeili, and R. L. Walsworth, “Optical magnetic imaging of living cells,” Nature 496(7446), 486–489 (2013).
[Crossref] [PubMed]

J. R. Maze, P. L. Stanwix, J. S. Hodges, S. Hong, J. M. Taylor, P. Cappellaro, L. Jiang, M. V. G. Dutt, E. Togan, A. S. Zibrov, A. Yacoby, R. L. Walsworth, and M. D. Lukin, “Nanoscale magnetic sensing with an individual electronic spin in diamond,” Nature 455(7213), 644–647 (2008).
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New J. Phys. (1)

L. Robledo, H. Bernien, T. Van der Sar, and R. Hanson, “Spin dynamics in the optical cycle of single nitrogen-vacancy centres in diamond,” New J. Phys. 13(2), 025013 (2011).
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Phys. Rep. (1)

M. W. Doherty, N. B. Manson, P. Delaney, F. Jelezko, J. Wrachtrup, and L. C. L. Hollenberg, “The nitrogen-vacancy colour centre in diamond,” Phys. Rep. 528(1), 1–45 (2013).
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Phys. Rev. B (1)

L. M. Pham, S. J. DeVience, F. Casola, I. Lovchinsky, A. O. Sushkov, E. Bersin, J. Lee, E. Urbach, P. Cappellaro, H. Park, A. Yacoby, M. Lukin, and R. L. Walsworth, “NMR technique for determining the depth of shallow nitrogen-vacancy centers in diamond,” Phys. Rev. B 93(4), 045425 (2016).
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Phys. Rev. Lett. (5)

V. M. Acosta, E. Bauch, M. P. Ledbetter, A. Waxman, L.-S. Bouchard, and D. Budker, “Temperature dependence of the nitrogen-vacancy magnetic resonance in diamond,” Phys. Rev. Lett. 104(7), 070801 (2010).
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F. Dolde, M. W. Doherty, J. Michl, I. Jakobi, B. Naydenov, S. Pezzagna, J. Meijer, P. Neumann, F. Jelezko, N. B. Manson, and J. Wrachtrup, “Nanoscale detection of a single fundamental charge in ambient conditions using the NV- center in diamond,” Phys. Rev. Lett. 112(9), 097603 (2014).
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M. Kim, H. J. Mamin, M. H. Sherwood, K. Ohno, D. D. Awschalom, and D. Rugar, “Decoherence of near-surface nitrogen-vacancy centers due to electric field noise,” Phys. Rev. Lett. 115(8), 087602 (2015).
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A. O. Sushkov, I. Lovchinsky, N. Chisholm, R. L. Walsworth, H. Park, and M. D. Lukin, “Magnetic resonance detection of individual proton spins using quantum reporters,” Phys. Rev. Lett. 113(19), 197601 (2014).
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D. Wildanger, J. R. Maze, and S. W. Hell, “Diffraction unlimited all-optical recording of electron spin resonances,” Phys. Rev. Lett. 107(1), 017601 (2011).
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Phys. Rev. X (1)

C. Grezes, B. Julsgaard, Y. Kubo, M. Stern, T. Umeda, J. Isoya, H. Sumiya, H. Abe, S. Onoda, T. Ohshima, V. Jacques, J. Esteve, D. Vion, D. Esteve, K. Mølmer, and P. Bertet, “Multimode storage and retrieval of microwave fields in a spin ensemble,” Phys. Rev. X 4(2), 021049 (2014).
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Proc. Natl. Acad. Sci. U.S.A. (2)

M. Pfender, N. Aslam, G. Waldherr, P. Neumann, and J. Wrachtrup, “Single-spin stochastic optical reconstruction microscopy,” Proc. Natl. Acad. Sci. U.S.A. 111(41), 14669–14674 (2014).
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J. F. Barry, M. J. Turner, J. M. Schloss, D. R. Glenn, Y. Song, M. D. Lukin, H. Park, and R. L. Walsworth, “Optical magnetic detection of single-neuron action potentials using quantum defects in diamond,” Proc. Natl. Acad. Sci. U.S.A. 113(49), 14133–14138 (2016).
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Sci. Rep. (1)

V. Zablotskii, T. Polyakova, O. Lunov, and A. Dejneka, “How a high-gradient magnetic field could affect cell life,” Sci. Rep. 6(1), 37407 (2016).
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Science (5)

R. R. Fu, B. P. Weiss, E. A. Lima, R. J. Harrison, X.-N. Bai, S. J. Desch, D. S. Ebel, C. Suavet, H. Wang, D. Glenn, D. Le Sage, T. Kasama, R. L. Walsworth, and A. T. Kuan, “Solar nebula magnetic fields recorded in the Semarkona meteorite,” Science 346(6213), 1089–1092 (2014).
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I. Lovchinsky, A. O. Sushkov, E. Urbach, N. P. de Leon, S. Choi, K. De Greve, R. Evans, R. Gertner, E. Bersin, C. Müller, L. McGuinness, F. Jelezko, R. L. Walsworth, H. Park, and M. D. Lukin, “Nuclear magnetic resonance detection and spectroscopy of single proteins using quantum logic,” Science 351(6275), 836–841 (2016).
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G. de Lange, Z. H. Wang, D. Ristè, V. V. Dobrovitski, and R. Hanson, “Universal dynamical decoupling of a single solid-state spin from a spin bath,” Science 330(6000), 60–63 (2010).
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H. J. Mamin, M. Kim, M. H. Sherwood, C. T. Rettner, K. Ohno, D. D. Awschalom, and D. Rugar, “Nanoscale nuclear magnetic resonance with a nitrogen-vacancy spin sensor,” Science 339(6119), 557–560 (2013).
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M. Fanciulli, C. E. Ascheron, and A. H. Duhm, Electron Spin Resonance and Related Phenomena in Low-dimensional Structures, vol. 115 (Springer Berlin Heidelberg, 2009).

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Figures (12)

Fig. 1
Fig. 1

spin-RESOLFT imaging of NV centers. (a) Energy levels and diamond lattice schematic for the negatively charged NV center in diamond, which has electronic spin S = 1. (b) The spin-RESOLFT experimental setup is an NV-diamond scanning confocal microscope augmented with a low power green doughnut beam. (c) Spin-RESOLFT experimental sequence for quantum sensing using NV centers in diamond, e.g., AC magnetometry with the dynamical decoupling pulse sequence shown. A spatially selective repolarisation via the pulsed green doughnut beam is inserted before the spin readout to interrogate only a specific NV center. Readout reference measurements allow calibration of photon count to spin state. (d) 1D spin-RESOLFT scans for a single NV center and different doughnut durations, with doughnut beam power of 700 µW. (e) 2D spin-RESOLFT image of the same NV as in (d) with similar resolution ≈35 nm but with a much lower doughnut beam power of 25 µW and longer duration of 50 µs. Comparison confocal data in (d) and (e) are normalized to the maximum photon counts. spin-RESOLFT profiles and images are determined by comparing the fluorescence after applying the doughnut (pulse sig) with confocal scans (pulse ref0) and normalized with respect to the maximum spin contrast (see Appendix B).

Fig. 2
Fig. 2

Spin coherence time measurement for two NV defects resolvable only via spin-RESOLFT. (a) 2D Confocal image of two unresolved NV centres with the same orientation of their spin quantization axes. Black crosses indicate the NV positions as extracted from the spin-RESOLFT image, the black square indicates the Gaussian green laser beam centre. (b) 2D spin-RESOLFT image of same field-of-view as in (a) (acquisition time of 9 s per pixel, 150 µW doughnut beam power with duration of 17 µs). A 50 nm FWHM is extracted using a numerical fit of a five-level model. (c) Selective NV spin coherence measurements and associated fits to a stretched exponential for the two NV centres shown in (a) and (b), using the same doughnut beam power and duration as in (b). Inset: spin coherence time determined for the ensemble of two NVs via a confocal measurement and associated fit. Shaded regions indicate 95% confidence interval extracted from the fits.

Fig. 3
Fig. 3

Superresolution magnetic field imaging for two NV centres via spin-RESOLFT. (a) Schematic of the AC current wire and two NV centers (same as in Fig. 2(b)). (b) spin-RESOLFT AC magnetometry measurements at ν AC = 8.3 kHz for each NV center individually and for the two NV ensemble in confocal mode. Also shown are fits of data to sinusoids with phase fixed to zero for no applied current. (c) AC magnetic field magnitude at ν AC = 8.3 kHz as a function of applied current, measured at the position of each NV center via spin-RESOLFT and for the two NV ensemble in confocal mode. (d) 2D magnetic field map created by spin-RESOLFT (at two points) and confocal (one point) measurements at a fixed AC current 7 mA and ν AC = 8.3 kHz. The size of the disc for each NV is given by the fit uncertainty (95% confidence) of the 2D position from the superresolved NV imaging. For all spin-RESOLFT measurements in this figure, the same doughnut beam power and duration were used as in Fig. 2 (150 µW and 17 µs).

Fig. 4
Fig. 4

NV spin-RESOLFT sensing of proton NMR. (a) Schematic showing nanometer-scale localization volume of a shallow NV. (b) XY8-k dynamical decoupling pulse sequence used for NMR proton sensing with sub-diffraction resolution. (c) Example use of an XY8-4 sequence for spin-RESOLFT (blue) and confocal (red) NV NMR spectroscopy of proton spins in immersion oil on the diamond surface without degradation of the measured NMR proton linewidth (with doughnut beam power of 30 µW and duration of 10 µs). Fits to an analytical model (red and blue curves) determine the NV depth to be 3.0 ± 0.3 nm [30].

Fig. 5
Fig. 5

(a) Single NV fluorescence measurements as a function of relative position (1D) acquired for the spin-RESOLFT protocol: after the application of the doughnut beam (signal, green) and after a complete repolarization with a Gaussian beam (ref0, blue). A 2-pixel running average is applied to smooth shot-noise-limited intensity fluctuations. At certain positions, the NV spin repolarization occurring from doughnut beam illumination is more efficient, leading eventually to a stronger fluorescence signal. (b) 1D spin-RESOLFT NV image (blue dots) constructed by subtracting the fluorescence curves shown in (a). Red curve is a numerical fit of data to a five level model (see next section).

Fig. 6
Fig. 6

NV level structure and decay rates. The populations are denoted by , where i refers to the following levels: 1 for ms = 0 ground state, 2 for ms = −1 ground state, 3 for ms = 0 excited state, 4 for ms = −1 excited state and 5 for the singlet states. The decay rates aij between levels are indexed by the initial level i and the final level j. All rates are given relative to the primary fluorescence decay rate γ. The singlet states are represented as a single state for the sake of simplicity, and we use previously measured room temperature rates [37].

Fig. 7
Fig. 7

Simulation of the dependence of the NV spin polarization on green excitation beam intensity. The degree of polarization displays a non-linear behaviour with light excitation. Short pulses of about 100 µs provide at most 70% polarization, due to non-zero decay rates from the singlet state to both the ground state sublevels. Longer pulses provide a higher degree of polarization but restrict the intensity to a fraction of the saturation intensity. The highest resolution is obtained for durations where the slope near the doughnut center is steeper, which leads to strong non-linear behaviour, a degradation of the spin polarization far from the doughnut center and a non-trivial PSF profile.

Fig. 8
Fig. 8

Simulated spin-RESOLFT PSF for two different residual intensities in the center of the green doughnut beam: = 0.1% (red) and = 2% (blue).

Fig. 9
Fig. 9

Measured 2D images of a pair of proximal NV centers and a reference NV center (a) confocal scan; (b) green doughnut beam scan.

Fig. 10
Fig. 10

(a) Measured relative 1D position of an example NV center and the laboratory temperature during a 5h-long confocal scan. A 1D NV fluorescence intensity profile takes about 1 minute after which the temperature and the NV center position are recorded. The laboratory temperature oscillates with a period of about 1 h and induces a correlated drift of the NV center position ~500 nm. (b) Stabilization of the laboratory temperature to a peak-to-peak variation of 0.1 °C allows data acquisition for two hours during which time the NV position is stable with a standard deviation of 11 nm.

Fig. 11
Fig. 11

(a) Magnetic field strength and (b) gradient extracted from a model that takes into account the distance from the wire and the orientation of the NV center axis. At a horizontal distance of 10 µm from the wire, the measured magnetic field strength of 9 µT and (b) measured gradient of 1 nT/nm are in good agreement with the experimental values reported in the main text.

Fig. 12
Fig. 12

(a) Calculated NV Rabi frequency as a function of the NV center horizontal position. This spatial behaviour is calculated from a model that takes into account the distance between the wire and the NV center as well as the NV orientation. The red dot corresponds to the position of the two NV centers used in the main text (NV1 and NV2). (b) Measured NV Rabi oscillations (blue dots) and a fit to an exponentially damped sinusoid (red curve). The extracted Rabi frequency of 5.5 MHz is a good agreement with the model calculation.

Tables (1)

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Table 1 Technique comparison.

Equations (9)

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1 γ dn 1 dt =I( t ) σ n 1 + n 1 + a 51 n 5
1 γ dn 2 dt =I( t ) σ n 2 + n 2 + a 52 n 5
1 γ dn 3 dt =I( t ) σ n 1 n 3 a 35 n 3
1 γ dn 4 dt =I( t ) σ n 2 n 4 a 45 n 4
1 γ dn 5 dt = a 35 n 3 + a 45 n 4 a 51 n 5 a 52 n 5 .
I( r )= I 0 ( ( r r 0 ) 2 +ϵ )exp ( r r 0 ) 2
B ||  ( r )=  B wire  ( r )NV( r ) = μ 0 2π   I x 2 + z 2 ( z sinϕcosθ+xcosϕ ).
B  ( r )=  B wire  ( r ) B wire  ( r )NV( r ).
η= 1 γ e 1 C  e τ/ T 2 t i +τ+ t R τ

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