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Tunable photon-induced spatial modulation of free electrons

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Abstract

Spatial modulation of electron beams is an essential tool for various applications such as nanolithography and imaging, yet its conventional implementations are severely limited and inherently non-tunable. Conversely, proposals of light-driven electron spatial modulation promise tunable electron wavefront shaping, for example, using the mechanism of photon-induced near-field electron microscopy. Here we present tunable photon-induced spatial modulation of electrons through their interaction with externally controlled surface plasmon polaritons (SPPs). Using recently developed methods of shaping SPP patterns, we demonstrate a dynamic control of the electron beam with a variety of electron distributions and verify their coherence through electron diffraction. Finally, the nonlinearity stemming from energy post-selection provides us with another avenue for controlling the electron shape, generating electron features far below the SPP wavelength. Our work paves the way to on-demand electron wavefront shaping at ultrafast timescales, with prospects for aberration correction, nanofabrication and material characterization.

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Fig. 1: Concept illustration of tunable photo-induced free-electron spatial amplitude modulation.
Fig. 2: Experimental set-up and proof of concept of photon-induced spatial modulation of free electrons.
Fig. 3: Electron diffraction from a hexagonal plasmonic vortex array.
Fig. 4: Spatial modulation of free electrons by active control of SPP boundary conditions.
Fig. 5: Nonlinear control over the electron distribution using a plasmonic pattern and electron post-selection.

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Data availability

Due to the large size of the raw data files (over 16.5 GB), the data supporting the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

Samples were prepared at Technion’s Micro and Nano Fabrication Unit, with the help of G. Ankonina and L. Popilevsky. Measurements were conducted in I.K.’s UTEM laboratory in the electron microscopy centre (MIKA) in the Department of Materials Science and Engineering of the Technion. We acknowledge the Russell Berrie Nanotechnology Institute and the Hellen Diller Quantum Center for their support of this research. S.T. acknowledges support by the Adams Fellowship Program of the Israel Academy of Science and Humanities and thanks A. Karnieli, A. Arie, Y. Kauffmann and M. Krueger for helpful conversations. R.D. thanks G. M. Vanacore for helpful discussions on performing electron diffraction. We are especially grateful to the Q-SORT consortium for inspiring this work. I.K. acknowledges the support of the Azrieli Faculty Fellowship. This research was supported by the European Research Council starting grant NanoEP 851780, the European Union’s Horizon 2020 research and innovation programme grant SMART-electron 964591 and the Israel Science Foundation grants 3334/19 and 831/19.

Author information

Author notes

  1. These authors contributed equally: Shai Tsesses, Raphael Dahan.

Authors and Affiliations

  1. Andrew and Erna Viterbi Department of Electrical Engineering, Technion, Israel Institute of Technology, Haifa, Israel

    Shai Tsesses, Raphael Dahan, Kangpeng Wang, Tomer Bucher, Kobi Cohen, Ori Reinhardt, Guy Bartal & Ido Kaminer

  2. Solid State Institute, Technion, Israel Institute of Technology, Haifa, Israel

    Raphael Dahan, Kangpeng Wang, Tomer Bucher, Ori Reinhardt & Ido Kaminer

  3. Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai, China

    Kangpeng Wang

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  1. Shai Tsesses
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Contributions

S.T. and I.K. conceived the project. S.T. and K.C. designed and fabricated the samples. R.D., S.T. and K.W. conducted the measurements. O.R., S.T. and T.B. performed simulations and theoretical calculations. G.B. and I.K. supervised the project. All authors participated in writing the manuscript and analysing the experimental results.

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Correspondence to Ido Kaminer.

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Nature Materials thanks Benjamin McMorran and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Extended data

Extended Data Fig. 1 Sample design and fabrication.

(a) Illustration of the sample used in the experiments, overlaid with the cross-section of the long-range surface plasmon polariton (SPP), showing its electric field amplitude in the direction of electron propagation (|Ez|). The vertical arrow provides an axis for the SPP amplitude profile. (b) A SEM micrograph of the various plasmonic coupling slits used in our experiments, which were optimized for broadband operation around an excitation wavelength of 730 nm and milled into the gold layer of the sample (scale bar is 10 microns). The coordinate system of the experiment appears in both (a) and (b), rotated to fit the observation direction in each case.

Extended Data Fig. 2 Electron energy filtering schemes used in the experiment.

The figure shows a representative measurement of the electron energy loss spectrum (EELS) measured in our experiment (blue area), with visible peaks at integer multiples of the laser pulse (~1.7 eV). The measured EELS without laser pulse excitation is given by the dotted gold curve. For the measurements performed in Figs. 2–3, we filter electrons that gained energy, as marked by the dashed black frame, effectively adding up all positive free-electron–light interaction orders. For the measurements performed in Fig. 4, we filter electrons that underwent interactions of specific orders, as marked by the light orange rectangles (each with a ~1 eV energy width). The energy dispersion of our EELS measurement was 0.1 eV per pixel.

Extended Data Fig. 3 Theory of photon-induced amplitude and phase modulation.

(a),(b) Calculated amplitude and phase of the out-of-plane electric field for a 1st order plasmonic Bessel vortex, created by a circular coupling slit as in Fig. 2b. The field is calculated via the Huygens principle method. (c),(d) Calculated amplitude and phase of the transverse electron wavefunction, after interaction with the SPP vortex presented in (a),(b), in the low-intensity interaction regime. The wavefunction distribution is calculated via the expression given in Methods section, by summing over the first 10 interaction orders. The fine match between the electron and electric field distributions suggests that light shapes both the electron amplitude and phase, as was also verified by the diffraction measurement in Fig. 3. A specific consequence of shaping both the amplitude and the phase is that angular momentum can indeed be transferred from the SPP vortex field to the electrons interacting with it.

Extended Data Fig. 4 Image processing of the electron distribution measurements.

The figure illustrates the process of creating the electron distribution images presented throughout the manuscript. (a) The raw data without any manipulation. Random pixel flaring greatly reduces image contrast, making it seem as though there is no signal. (b) Mitigation of random pixel flaring by contrast manipulation, as described in Methods section. (c) Equalization of the image after contrast manipulation enables the visualization of more detailed features. (d) The image generated automatically from the detector software, qualitatively similar to the image that we extracted. The white scale bar in (d) is relevant for all images and corresponds to 5 microns.

Supplementary information

Supplementary Video 1

Spatial modulation of free electrons by active control of SPP boundary conditions at high magnification.

Supplementary Video 2

Spatial modulation of free electrons by active control of SPP boundary conditions at low magnification.

Supplementary Video 3

Sample tilt influence on photon-induced spatial modulation of free electrons.

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Tsesses, S., Dahan, R., Wang, K. et al. Tunable photon-induced spatial modulation of free electrons. Nat. Mater. 22, 345–352 (2023). https://doi.org/10.1038/s41563-022-01449-1

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