Ultrafast generation and control of an electron vortex beam via chiral plasmonic near fields

Abstract

Vortex-carrying matter waves, such as chiral electron beams, are of significant interest in both applied and fundamental science. Continuous-wave electron vortex beams are commonly prepared via passive phase masks imprinting a transverse phase modulation on the electron’s wavefunction. Here, we show that femtosecond chiral plasmonic near fields enable the generation and dynamic control on the ultrafast timescale of an electron vortex beam. The vortex structure of the resulting electron wavepacket is probed in both real and reciprocal space using ultrafast transmission electron microscopy. This method offers a high degree of scalability to small length scales and a highly efficient manipulation of the electron vorticity with attosecond precision. Besides the direct implications in the investigation of nanoscale ultrafast processes in which chirality plays a major role, we further discuss the perspectives of using this technique to shape the wavefunction of charged composite particles, such as protons, and how it can be used to probe their internal structure.

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Fig. 1: Generation and detection of chiral SPPs.
Fig. 2: One-to-one correspondence between the complex SPP optical field and the transverse distribution of the electron wavefunction.
Fig. 3: Generation and detection of an ultrafast electron vortex beam via interaction with a chiral plasmonic near field.
Fig. 4: Dynamic phase control of the electron/chiral-plasmon interactions.

Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

References

  1. 1.

    Rubinsztein-Dunlop, H. et al. Roadmap on structured light. J. Opt. 19, 013001 (2017).

    Article  Google Scholar 

  2. 2.

    Yao, A. M. & Padgett, M. J. Orbital angular momentum: origins, behavior and applications. Adv. Opt. Photon. 3, 161–204 (2011).

    CAS  Article  Google Scholar 

  3. 3.

    Gibson, G. et al. Free-space information transfer using light beams carrying orbital angular momentum. Opt. Express 12, 5448–5456 (2004).

    Article  Google Scholar 

  4. 4.

    Bozinovic, N. et al. Terabit-scale orbital angular momentum mode division multiplexing in fibers. Science 340, 1545–1548 (2013).

    CAS  Article  Google Scholar 

  5. 5.

    Sit, A. et al. High-dimensional intracity quantum cryptography with structured photons. Optica 4, 1006–1010 (2017).

    Article  Google Scholar 

  6. 6.

    Grier, D. G. A revolution in optical manipulation. Nature 424, 810–816 (2003).

    CAS  Article  Google Scholar 

  7. 7.

    Padgett, M. J. & Bowman, R. Tweezers with a twist. Nat. Photon. 5, 343–348 (2011).

    CAS  Article  Google Scholar 

  8. 8.

    Mair, A., Vaziri, A., Weihs, G. & Zeilinger, A. Entanglement of the orbital angular momentum states of photons. Nature 412, 313–316 (2001).

    CAS  Article  Google Scholar 

  9. 9.

    Leach, J. et al. Quantum correlations in optical angle–orbital angular momentum variables. Science 329, 662–665 (2010).

    CAS  Article  Google Scholar 

  10. 10.

    Zilio, P., Mari, E., Parisi, G., Tamburini, F. & Romanato, F. Angular momentum properties of electromagnetic field transmitted through holey plasmonic vortex lenses. Opt. Lett. 37, 3234–3236 (2012).

    Article  Google Scholar 

  11. 11.

    Bliokh, K. Y., Bliokh, Y. P., Savel’ev, S. & Nori, F. Semiclassical dynamics of electron wave packet states with phase vortices. Phys. Rev. Lett. 99, 190404 (2007).

    Article  Google Scholar 

  12. 12.

    Bliokh, K. Y. et al. Theory and applications of free-electron vortex states. Phys. Rep. 690, 1–70 (2017).

    CAS  Article  Google Scholar 

  13. 13.

    Lloyd, S. M., Babiker, M., Thirunavukkarasu, G. & Yuan, J. Electron vortices: beams with orbital angular momentum. Rev. Mod. Phys. 89, 035004 (2017).

    Article  Google Scholar 

  14. 14.

    Larocque, H. et al. ‘Twisted’ electrons. Contemp. Phys. 59, 126–144 (2018).

    Article  Google Scholar 

  15. 15.

    Edström, A., Lubk, A. & Rusz, J. Elastic scattering of electron vortex beams in magnetic matter. Phys. Rev. Lett. 116, 127203 (2016).

    Article  Google Scholar 

  16. 16.

    Grillo, V. et al. Observation of nanoscale magnetic fields using twisted electron beams. Nat. Commun. 8, 689 (2017).

    Article  Google Scholar 

  17. 17.

    Uchida, M. & Tonomura, A. Generation of electron beams carrying orbital angular momentum. Nature 464, 737–739 (2010).

    CAS  Article  Google Scholar 

  18. 18.

    Verbeeck, J., Tian, H. & Schattschneider, P. Production and application of electron vortex beams. Nature 467, 301–304 (2010).

    CAS  Article  Google Scholar 

  19. 19.

    McMorran, B. J. et al. Electron vortex beams with high quanta of orbital angular momentum. Science 331, 192–195 (2011).

    CAS  Article  Google Scholar 

  20. 20.

    Mafakheri, E. et al. Realization of electron vortices with large orbital angular momentum using miniature holograms fabricated by electron beam lithography. Appl. Phys. Lett. 110, 093113 (2017).

    Article  Google Scholar 

  21. 21.

    Béché, A., Van Boxem, R., Van Tendeloo, G. & Verbeeck, J. J. Magnetic monopole field exposed by electrons. Nat. Phys. 10, 26–29 (2014).

    Article  Google Scholar 

  22. 22.

    Verbeeck, J. et al. Demonstration of a 2×2 programmable phase plate for electrons. Ultramicroscopy 190, 58–65 (2018).

    CAS  Article  Google Scholar 

  23. 23.

    Pozzi, G., Lub, P.-H., Tavabi, A. H., Duchamp, M. & Dunin-Borkowski, R. E. Generation of electron vortex beams using line charges via the electrostatic Aharonov–Bohm effect. Ultramicroscopy 181, 191–196 (2017).

    CAS  Article  Google Scholar 

  24. 24.

    Handali, J., Shakya, P. & Barwick, B. Creating electron vortex beams with light. Opt. Express 23, 5236–5243 (2015).

    CAS  Article  Google Scholar 

  25. 25.

    Cai, W., Reinhardt, O., Kaminer, I. & García de Abajo, F. J. Efficient orbital angular momentum transfer between plasmons and free electrons. Phys. Rev. B 98, 045424 (2018).

    CAS  Article  Google Scholar 

  26. 26.

    Piazza, L. et al. Design and implementation of a fs-resolved transmission electron microscope based on thermionic gun technology. Chem. Phys. 423, 79–84 (2015).

    Article  Google Scholar 

  27. 27.

    Vanacore, G. M., Fitzpatrick, A. W. P. & Zewail, A. H. Four-dimensional electron microscopy: ultrafast imaging, diffraction and spectroscopy in materials science and biology. Nano Today 11, 228–249 (2016).

    CAS  Article  Google Scholar 

  28. 28.

    Aidala, C. A., Bass, S. D., Hasch, D. & Mallot, G. K. The spin structure of the nucleon. Rev. Mod. Phys. 85, 655–691 (2013).

    CAS  Article  Google Scholar 

  29. 29.

    Priebe, K. E. et al. Attosecond electron pulse trains and quantum state reconstruction in ultrafast transmission electron microscopy. Nat. Photon. 11, 793–797 (2017).

    CAS  Article  Google Scholar 

  30. 30.

    Morimoto, Y. & Baum, P. Diffraction and microscopy with attosecond electron pulse trains. Nat. Phys. 14, 252–256 (2018).

    CAS  Article  Google Scholar 

  31. 31.

    Vanacore, G. M. et al. Attosecond coherent control of free-electron wave functions using semi-infinite light fields. Nat. Commun. 9, 2694 (2018).

    CAS  Article  Google Scholar 

  32. 32.

    Spektor, G. et al. Revealing the subfemtosecond dynamics of orbital angular momentum in nanoplasmonic vortices. Science 355, 1187–1191 (2017).

    CAS  Article  Google Scholar 

  33. 33.

    Gorodetski, Y., Niv, A., Kleiner, V. & Hasman, E. Observation of the spin-based plasmonic effect in nanoscale structures. Phys. Rev. Lett. 101, 043903 (2008).

    CAS  Article  Google Scholar 

  34. 34.

    Bliokh, K. Y., Rodríguez-Fortuño, F. J., Nori, F. & Zayats, A. V. Spin–orbit interactions of light. Nat. Photon. 9, 796–808 (2015).

    CAS  Article  Google Scholar 

  35. 35.

    Madan, I. et al. Holographic imaging of electromagnetic fields via electron-light quantum interference. Sci. Adv. 5, eaav8358 (2019).

    CAS  Article  Google Scholar 

  36. 36.

    Ohno, T. & Miyanishi, S. Study of surface plasmon chirality induced by Archimedes’ spiral grooves. Opt. Express 14, 6285 (2006).

    Article  Google Scholar 

  37. 37.

    Cho, S.-W., Park, J., Lee, S.-Y., Kim, H. & Lee, B. Coupling of spin and angular momentum of light in plasmonic vortex. Opt. Express 20, 10083 (2012).

    Article  Google Scholar 

  38. 38.

    Guzzinati, G. et al. Probing the symmetry of the potential of localized surface plasmon resonances with phase-shaped electron beams. Nat. Commun. 8, 14999 (2017).

    CAS  Article  Google Scholar 

  39. 39.

    Larocque, H., Kaminer, I., Grillo, V., Boyd, R. W. & Karimi, E. Twisting neutrons may reveal their internal structure. Nat. Phys. 14, 1–2 (2018).

    Article  Google Scholar 

  40. 40.

    Bliokh, K. Y., Dennis, M. R. & Nori, F. Relativistic electron vortex beams: angular momentum and spin–orbit interaction. Phys. Rev. Lett. 107, 174802 (2011).

    Article  Google Scholar 

  41. 41.

    Harvey, T. R., Grillo, V. & McMorran, B. J. Stern–Gerlach-like approach to electron orbital angular momentum measurement. Phys. Rev. A 95, 021801 (2017).

    Article  Google Scholar 

  42. 42.

    Karimi, E., Marrucci, L., Grillo, V. & Santamato, E. Spin-to-orbital angular momentum conversion and spin-polarization filtering in electron beams. Phys. Rev. Lett. 108, 044801 (2012).

    Article  Google Scholar 

  43. 43.

    Grillo, V. et al. Measuring the orbital angular momentum spectrum of an electron beam. Nat. Commun. 8, 15536 (2017).

    CAS  Article  Google Scholar 

  44. 44.

    Pomarico, E. et al. meV resolution in laser-assisted energy-filtered transmission electron microscopy. ACS Photon. 5, 759–764 (2018).

    CAS  Article  Google Scholar 

Download references

Acknowledgements

The LUMES laboratory acknowledges support from the NCCR MUST. G.M.V. is partially supported by the EPFL-Fellows-MSCA international fellowship (grant agreement no. 665667). R.J.L. and D.M. acknowledge funding support of R.J.L. by an EPSRC DTG studentship. I.K. is supported by the Azrieli Foundation and partially supported by the FP7-Marie Curie IOF under grant no. 328853-MC-BSiCS. V.G. is supported by the European project Q-SORT, which has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 766970. H.L. and E.K. acknowledge support from the Canada Research Chair (CRC) and Early Researcher Award (ERA). F.J.G.d.A. acknowledges support from the ERC (advanced grant 789104-eNANO), the Spanish MINECO (MAT2017-88492-R and SEV2015-0522) and the Catalan CERCA and Fundació Privada Cellex. B.B. acknowledges support with this material by the NSF under grant no. 1759847.

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Contributions

G.M.V., G.B., I.M., F.C., F.J.G.d.A. and E.K. conceived and designed the research. G.M.V., G.B., I.M. and E.P. conducted the experiments and analysed the data. R.J.L., D.M., I.M. and G.M.V. fabricated the samples. F.J.G.d.A. developed the semi-analytical theory and performed the calculations. P.B. performed the FDTD simulations. V.G. performed the electron vortex beam calculations. H.L. and E.K. performed the proton vortex beam calculations. G.M.V., G.B., I.M., O.R., I.K., B.B., V.G., E.K., F.J.G.d.A. and F.C. interpreted the results. All authors contributed to writing the article, and read and approved the final manuscript.

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Correspondence to G. M. Vanacore.

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Supplementary information

Supplementary Information

Supplementary Sections 1–5, Supplementary Figs. 1–11, Supplementary refs. 1–8

Supplementary Video 1

Coherent modulation of the intensity and of the spatial periodicity of the plasmonic fringes with a temporal 223 period given by the optical cycle of ~2.67 fs.

Supplementary Video 2

Experimentally measured spatial maps of the inelastically scattered electrons when using two elliptically polarized light pulses.

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Vanacore, G.M., Berruto, G., Madan, I. et al. Ultrafast generation and control of an electron vortex beam via chiral plasmonic near fields. Nat. Mater. 18, 573–579 (2019). https://doi.org/10.1038/s41563-019-0336-1

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