- Physical Review Journals
All JournalsPhysics Magazine

Physical Review Research

Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Letter
  • Open Access

Quantum sensing of magnetic fields with molecular color centers

Kathleen R. Mullin1, Daniel W. Laorenza2, Danna E. Freedman2, and James M. Rondinelli1,*

  • 1Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA
  • 2Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA

  • *jrondinelli@northwestern.edu
PDF

Phys. Rev. Research 5, L042023 – Published 8 November, 2023

DOI: https://doi.org/10.1103/PhysRevResearch.5.L042023

Abstract

Molecular color centers, such as S=1 Cr(o−tolyl)4, show promise as an adaptable platform for magnetic quantum sensing. Their intrinsically small size, i.e., 1–2 nm, enables them to sense fields at short distances and in various geometries. This feature, in conjunction with tunable optical read-out of spin information, offers the potential for molecular color centers to be a paradigm shifting materials class beyond diamond-NV centers by accessing a distance scale opaque to NVs. This capability could, for example, address ambiguity in the reported magnetic fields arising from two-dimensional magnets by allowing for a single sensing technique to be used over a wider range of distances. Yet, so far, these abilities have only been hypothesized with theoretical validation absent. We show through simulation that Cr(o−tolyl)4 can spatially resolve proximity-exchange versus direct magnetic-field effects from monolayer CrI3 by quantifying how these interactions impact the excited states of the molecule. At short distances, proximity exchange dominates through molecule-substrate interactions, but at further distances the molecule behaves as a typical magnetic sensor, with magnetostatic effects dominating changes to the energy of the excited state. Our models effectively demonstrate how a molecular color center could be used to measure the magnetic field of a two-dimensional magnet and the role different distance-dependent interactions contribute to the measured field.

View figure in article

Physics Subject Headings (PhySH)

Article Text

References (58)

  1. M. J. H. Ku, T. X. Zhou, Q. Li, Y. J. Shin, J. K. Shi, C. Burch, L. E. Anderson, A. T. Pierce, Y. Xie, A. Hamo, U. Vool, H. Zhang, F. Casola, T. Taniguchi, K. Watanabe, M. M. Fogler, P. Kim, A. Yacoby, and R. L. Walsworth, Imaging viscous flow of the Dirac fluid in graphene, Nature (London) 583, 537 (2020).
  2. U. Vool, A. Hamo, G. Varnavides, Y. Wang, T. X. Zhou, N. Kumar, Y. Dovzhenko, Z. Qiu, C. A. C. Garcia, A. T. Pierce, J. Gooth, P. Anikeeva, C. Felser, P. Narang, and A. Yacoby, Imaging phonon-mediated hydrodynamic flow in WTe2, Nat. Phys. 17, 1216 (2021).
  3. E. Marchiori, L. Ceccarelli, N. Rossi, L. Lorenzelli, C. L. Degen, and M. Poggio, Nanoscale magnetic field imaging for 2D materials, Nat. Rev. Phys. 4, 49 (2022).
  4. P. Ripka, New directions in fluxgate sensors, J. Magn. Magn. Mater. 215, 735 (2000).
  5. Y. Zheng, L. Huang, Z. Zhang, J. Jiang, K. Wang, L.-M. Peng, and G. Yu, Sensitivity enhancement of graphene Hall sensors modified by single-molecule magnets at room temperature, RSC Adv. 7, 1776 (2017).
  6. R. Li, S. Zhang, S. Luo, Z. Guo, Y. Xu, J. Ouyang, M. Song, Q. Zou, L. Xi, X. Yang, J. Hong, and L. You, A spin–orbit torque device for sensing three-dimensional magnetic fields, Nat. Electron. 4, 179 (2021).
  7. 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, 810 (2008).
  8. C. L. Degen, F. Reinhard, and P. Cappellaro, Quantum sensing, Rev. Mod. Phys. 89, 035002 (2017).
  9. S. Hong, M. S. Grinolds, L. M. Pham, D. Le Sage, L. Luan, R. L. Walsworth, and A. Yacoby, Nanoscale magnetometry with NV centers in diamond, MRS Bull. 38, 155 (2013).
  10. M. Radtke, E. Bernardi, A. Slablab, R. Nelz, and E. Neu, Nanoscale sensing based on nitrogen vacancy centers in single crystal diamond and nanodiamonds: Achievements and challenges, Nano Futures 3, 042004 (2019).
  11. M. Xie, X. Yu, L. V. H. Rodgers, D. Xu, I. Chi-Durán, A. Toros, N. Quack, N. P. de Leon, and P. C. Maurer, Biocompatible surface functionalization architecture for a diamond quantum sensor, Proc. Natl. Acad. Sci. USA 119, e2114186119 (2022).
  12. L. Tesi, F. Stemmler, M. Winkler, S. S. Y. Liu, S. Das, X. Sun, M. Zharnikov, S. Ludwigs, and J. van Slageren, Modular approach to creating functionalized surface arrays of molecular qubits, Adv. Mater. 35, 2208998 (2023).
  13. S. L. Bayliss, D. W. Laorenza, P. J. Mintun, B. D. Kovos, D. E. Freedman, and D. D. Awschalom, Optically addressable molecular spins for quantum information processing, Science 370, 1309 (2020).
  14. D. W. Laorenza, A. Kairalapova, S. L. Bayliss, T. Goldzak, S. M. Greene, L. R. Weiss, P. Deb, P. J. Mintun, K. A. Collins, D. D. Awschalom, T. C. Berkelbach, and D. E. Freedman, Tunable Cr4+ molecular color centers, J. Am. Chem. Soc. 143, 21350 (2021).
  15. W. F. Koehl, B. Diler, S. J. Whiteley, A. Bourassa, N. T. Son, E. Janzén, and D. D. Awschalom, Resonant optical spectroscopy and coherent control of Cr4+ spin ensembles in SiC and GaN, Phys. Rev. B 95, 035207 (2017).
  16. B. Diler, S. J. Whiteley, C. P. Anderson, G. Wolfowicz, M. E. Wesson, E. S. Bielejec, F. Joseph Heremans, and D. D. Awschalom, Coherent control and high-fidelity readout of chromium ions in commercial silicon carbide, npj Quantum Inf. 6, 11 (2020).
  17. 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 (London) 455, 644 (2008).
  18. L. Rondin, J.-P. Tetienne, P. Spinicelli, C. Dal Savio, K. Karrai, G. Dantelle, A. Thiaville, S. Rohart, J.-F. Roch, and V. Jacques, Nanoscale magnetic field mapping with a single spin scanning probe magnetometer, Appl. Phys. Lett. 100, 153118 (2012).
  19. A. Kubica, J. Kowalewski, D. Kruk, and M. Odelius, Zero-field splitting in nickel(II) complexes: A comparison of DFT and multi-configurational wavefunction calculations, J. Chem. Phys. 138, 064304 (2013).
  20. M. Gibertini, M. Koperski, A. F. Morpurgo, and K. S. Novoselov, Magnetic 2D materials and heterostructures, Nat. Nanotechnol. 14, 408 (2019).
  21. Q. H. Wang, A. Bedoya-Pinto, M. Blei, A. H. Dismukes, A. Hamo, S. Jenkins, M. Koperski, Y. Liu, Q.-C. Sun, E. J. Telford, H. H. Kim, M. Augustin, U. Vool, J.-X. Yin, L. H. Li, A. Falin, C. R. Dean, F. Casanova, R. F. L. Evans, M. Chshiev et al., The magnetic genome of two-dimensional van der Waals materials, ACS Nano 16, 6960 (2022).
  22. D. Zhong, K. L. Seyler, X. Linpeng, R. Cheng, N. Sivadas, B. Huang, E. Schmidgall, T. Taniguchi, K. Watanabe, M. A. McGuire, W. Yao, D. Xiao, K.-M. C. Fu, and X. Xu, Van der Waals engineering of ferromagnetic semiconductor heterostructures for spin and valleytronics, Sci. Adv. 3, e1603113 (2017).
  23. L. Thiel, Z. Wang, M. A. Tschudin, D. Rohner, I. Gutiérrez-Lezama, N. Ubrig, M. Gibertini, E. Giannini, A. F. Morpurgo, and P. Maletinsky, Probing magnetism in 2D materials at the nanoscale with single-spin microscopy, Science 364, 973 (2019).
  24. K. Zollner, P. E. Faria Junior, and J. Fabian, Giant proximity exchange and valley splitting in transition metal dichalcogenide/hBN/(Co, Ni) heterostructures, Phys. Rev. B 101, 085112 (2020).
  25. K. Zollner, P. E. Faria Junior, and J. Fabian, Proximity exchange effects in MoSe2 and WSe2 heterostructures with CrI3: Twist angle, layer, and gate dependence, Phys. Rev. B 100, 085128 (2019).
  26. E. C. Ahn, 2D materials for spintronic devices, npj 2D Mater. Appl. 4, 17 (2020).
  27. K. Zollner and J. Fabian, Proximity effects in graphene on monolayers of transition-metal phosphorus trichalcogenides MPX3(M:Mn,Fe,Ni,Co, and X:S,Se), Phys. Rev. B 106, 035137 (2022).
  28. G. Kresse and J. Hafner, Ab initio molecular dynamics for liquid metals, Phys. Rev. B 47, 558 (1993).
  29. G. Kresse and J. Hafner, Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium, Phys. Rev. B 49, 14251 (1994).
  30. G. Kresse and J. Furthmüller, Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set, Comput. Mater. Sci. 6, 15 (1996).
  31. G. Kresse and J. Furthmüller, Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set, Phys. Rev. B 54, 11169 (1996).
  32. G. Kresse and D. Joubert, From ultrasoft pseudopotentials to the projector augmented-wave method, Phys. Rev. B 59, 1758 (1999).
  33. P. E. Blöchl, Projector augmented-wave method, Phys. Rev. B 50, 17953 (1994).
  34. J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple [Phys. Rev. Lett. 77, 3865 (1996)], Phys. Rev. Lett. 78, 1396 (1997).
  35. J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
  36. A. Hellman, B. Razaznejad, and B. I. Lundqvist, Potential-energy surfaces for excited states in extended systems, J. Chem. Phys. 120, 4593 (2004).
  37. J. Gavnholt, T. Olsen, M. Engelund, and J. Schiøtz, Δ self-consistent field method to obtain potential energy surfaces of excited molecules on surfaces, Phys. Rev. B 78, 075441 (2008).
  38. D. Wang and B. Sanyal, Systematic study of monolayer to trilayer CrI3: Stacking sequence dependence of electronic structure and magnetism, J. Phys. Chem. C 125, 18467 (2021).
  39. S. Grimme, J. Antony, S. Ehrlich, and H. Krieg, A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu, J. Chem. Phys. 132, 154104 (2010).
  40. S. Grimme, S. Ehrlich, and L. Goerigk, Effect of the damping function in dispersion corrected density functional theory, J. Comput. Chem. 32, 1456 (2011).
  41. A. Okuniewski, D. Rosiak, J. Chojnacki, and B. Becker, Coordination polymers and molecular structures among complexes of mercury(II) halides with selected 1-benzoylthioureas, Polyhedron 90, 47 (2015).
  42. M. J. Amdur, K. R. Mullin, M. J. Waters, D. Puggioni, M. K. Wojnar, M. Gu, L. Sun, P. H. Oyala, J. M. Rondinelli, and D. E. Freedman, Chemical control of spin-lattice relaxation to discover a room temperature molecular qubit, Chem. Sci. 13, 7034 (2022).
  43. J. F. Barry, J. M. Schloss, E. Bauch, M. J. Turner, C. A. Hart, L. M. Pham, and R. L. Walsworth, Sensitivity optimization for NV-diamond magnetometry, Rev. Mod. Phys. 92, 015004 (2020).
  44. S. L. Bayliss, P. Deb, D. W. Laorenza, M. Onizhuk, G. Galli, D. E. Freedman, and D. D. Awschalom, Enhancing spin coherence in optically addressable molecular qubits through host-matrix control, Phys. Rev. X 12, 031028 (2022).
  45. K. Xiao, W. Deng, J. K. Keum, M. Yoon, I. V. Vlassiouk, K. W. Clark, A.-P. Li, I. I. Kravchenko, G. Gu, E. A. Payzant, B. G. Sumpter, S. C. Smith, J. F. Browning, and D. B. Geohegan, Surface-induced orientation control of CuPc molecules for the epitaxial growth of highly ordered organic crystals on graphene, J. Am. Chem. Soc. 135, 3680 (2013).
  46. M. Stöhr, M. Gabriel, and R. Möller, Investigation of the growth of PTCDA on Cu(110): An STM study, Surf. Sci. 507-510, 330 (2002).
  47. S. Tiwari, M. L. Van de Put, B. Sorée, and W. G. Vandenberghe, Magnetic order and critical temperature of substitutionally doped transition metal dichalcogenide monolayers, npj 2D Mater. Appl. 5, 54 (2021).
  48. K. S. Burch, D. Mandrus, and J.-G. Park, Magnetism in two-dimensional van der Waals materials, Nature (London) 563, 47 (2018).
  49. A. B. Georgescu, A. J. Millis, and J. M. Rondinelli, Trigonal symmetry breaking and its electronic effects in the two-dimensional dihalides MX2 and trihalides MX3, Phys. Rev. B 105, 245153 (2022).
  50. S. Trebst and C. Hickey, Kitaev materials, Phys. Rep. 950, 1 (2022).
  51. J. A. Sears, M. Songvilay, K. W. Plumb, J. P. Clancy, Y. Qiu, Y. Zhao, D. Parshall, and Y.-J. Kim, Magnetic order in α−RuCl3: A honeycomb-lattice quantum magnet with strong spin-orbit coupling, Phys. Rev. B 91, 144420 (2015).
  52. Y. Wang, M. E. Ziebel, L. Sun, J. T. Gish, T. J. Pearson, X.-Z. Lu, A. E. Thorarinsdottir, M. C. Hersam, J. R. Long, D. E. Freedman, J. M. Rondinelli, D. Puggioni, and T. D. Harris, Strong magnetocrystalline anisotropy arising from metal–ligand covalency in a metal–organic candidate for 2D magnetic order, Chem. Mater. 33, 8712 (2021).
  53. A. E. Thorarinsdottir and T. D. Harris, Metal–organic framework magnets, Chem. Rev. (Washington, DC, US) 120, 8716 (2020).
  54. C. M. Fang, M. A. van Huis, Q. Xu, R. J. Cava, and H. W. Zandbergen, Unexpected origin of magnetism in monoclinic Nb12O29 from first-principles calculations, J. Mater. Chem. C 3, 651 (2015).
  55. E. Sheridan, T. F. Harrelson, E. Sivonxay, K. A. Persson, M. V. P. Altoé, I. Siddiqi, D. F. Ogletree, D. I. Santiago, and S. M. Griffin, Microscopic theory of magnetic disorder-induced decoherence in superconducting Nb films, arXiv:2111.11684.
  56. A. J. Fielding, S. Fox, G. L. Millhauser, M. Chattopadhyay, P. M. Kroneck, G. Fritz, G. R. Eaton, and S. S. Eaton, Electron spin relaxation of copper(II) complexes in glassy solution between 10 and 120 K, J. Magn. Reson. 179, 92 (2006).
  57. M. Atzori, S. Benci, E. Morra, L. Tesi, M. Chiesa, R. Torre, L. Sorace, and R. Sessoli, Structural effects on the spin dynamics of potential molecular qubits, Inorg. Chem. (Washington, DC, US) 57, 731 (2018).
  58. https://github.com/MTD-group/Magnetostatic-Model-CrI3.

Outline

Information

Phys. Rev. Research 5, L042023– Published 8 November, 2023
  • Received 7 February 2023
  • Revised 13 June 2023
  • Accepted 10 October 2023
Crossmark - Check for updates button
Creative Commons Logo

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

Published by the American Physical Society

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation