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arXiv:2502.13821

Electron-Enabled Nanoparticle Diffraction

Stefan Nimmrichter, Dennis Rätzel, Isobel Claire Bicket, Michael Stanislaus Seifner, Philipp Haslinger

Published Feb 19, 2025• 0 citations
arXivHTMLPDF

Abstract

Matter-wave interferometry is a phenomenon which has been utilized and studied in electron microscopy since the early days of electron optics, with the development of phase contrast imaging, electron diffraction, electron holography, etc. When an electron diffracts off of a crystal lattice, it enters a superposition state of eligible Bragg diffraction components; due to momentum conservation, the crystalline sample must receive an equal and opposite superposition of momentum transfers. In theory, this results in an entangled electron-sample state. Typically, however, the sample is extremely large relative to the electron and is held fast in a sample holder, and this reciprocal momentum transfer is unobservable [1]. We present a proposal [2] to establish a system where such momentum kicks would be resolvable, to enable probing of the matter-wave properties of the sample as well as the free electron. A crystalline silicon nanoparticle is levitated in the sample plane, then released from its trap to enter free-fall. A single electron impacts the nanoparticle and undergoes Bragg diffraction. The nanoparticle receives a momentum transfer from the diffraction and is allowed to continue free-falling for a fixed amount of time before recapture and measurement of its position, X. In synchrony, the position of the electron, x, is measured. Assuming perfect measurement resolution, we calculate the resulting interference pattern for a quantum interaction, where the nanoparticle can behave as a quantum wave (Fig. 1a), or for the case where it behaves as a classical grating aperture (Fig. 1b) for different recapture times, t. The quantum scenario presents additional fringes visible at specific recapture times. Such an experiment provides a test of the matter-wave behaviour of high mass nanoparticles, with an efficient duty cycle and a short interference time, and would allow access to electron-sample entanglement in a transmission electron microscope.

DOI
10.34726/12104

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Matter-wave interferometry is a phenomenon which has been utilized and studied in electron microscopy since the early days of electron optics, with the development of phase contrast imaging, electron diffraction, electron holography, etc. When an electron diffracts off of a crystal lattice, it enters a superposition state of eligible Bragg diffraction components; due to momentum conservation, the crystalline sample must receive an equal and opposite superposition of momentum transfers. In theory, this results in an entangled electron-sample state. Typically, however, the sample is extremely large relative to the electron and is held fast in a sample holder, and this reciprocal momentum transfer is unobservable [1]. We present a proposal [2] to establish a system where such momentum kicks would be resolvable, to enable probing of the matter-wave properties of the sample as well as the free electron. A crystalline silicon nanoparticle is levitated in the sample plane, then released from its trap to enter free-fall. A single electron impacts the nanoparticle and undergoes Bragg diffraction. The nanoparticle receives a momentum transfer from the diffraction and is allowed to continue free-falling for a fixed amount of time before recapture and measurement of its position, X. In synchrony, the position of the electron, x, is measured. Assuming perfect measurement resolution, we calculate the resulting interference pattern for a quantum interaction, where the nanoparticle can behave as a quantum wave (Fig. 1a), or for the case where it behaves as a classical grating aperture (Fig. 1b) for different recapture times, t. The quantum scenario presents additional fringes visible at specific recapture times. Such an experiment provides a test of the matter-wave behaviour of high mass nanoparticles, with an efficient duty cycle and a short interference time, and would allow access to electron-sample entanglement in a transmission electron microscope.
We propose a scheme for generating high-mass quantum superposition states of an optically precooled, levitated nanoparticle through electron diffraction at its subnanometer crystal lattice. When a single electron undergoes Bragg diffraction at a free-falling nanoparticle, momentum conservation implies that the superposition of Bragg momenta is imprinted onto the relative coordinate between electron and nanoparticle, which entangles their wave functions. By imaging the electron interferogram, one maps the nanoparticle state onto a superposition of Bragg momenta, as if it was diffracted by its own lattice. This results in a coherent momentum splitting approximately 1000 times greater than what is achievable with two-photon recoils in conventional standing-wave gratings. Self-interference of the nanoparticle can thus be observed within drastically shorter free-fall times in a time-domain Talbot interferometer configuration, significantly relaxing source requirements and alleviating decoherence from environmental factors such as residual gas and thermal radiation. Shorter interference times also allow for a recapture of the nanoparticle within its initial trapping volume, facilitating its reuse in many rapid experimental duty cycles. This opens new possibilities for experimental tests of macroscopic quantum effects within a transmission electron microscope.
Although interferometry's earliest and most familiar use is with photons, the discovery of matter-wave (deBroglie-wave) interference for electrons demanded the development of quantum mechanics. Since then, matter-wave interferometry has been performed with neutrons, Cooper electron-pairs, and most recently, with whole atoms and diatomic molecules. This talk describes our recent high-flux atom interferometry experiments using the generalized Talbot-vonLau effect. Our interferometer consists of a sequence of three planar vacuum-slit diffraction gratings, microfabricated from silicon nitride membranes. DeBroglie-wave interference fringes are sensed by measuring the transmission of potassium atoms on a hot- wire as a function of grating relative position. Different spatial Fourier components (up to sixth) in the diffraction pattern are resonant in the interferometer at different atomic velocities (i.e., at different wavelengths). When a laser cooled slow atomic beam is incident, various different diffraction patterns are observed as a function of atomic velocity. In an alternative `Heisenberg Microscope' configuration an incident thermal beam produces a velocity average over different fringe Fourier components. AC modulated weak laser light passing through the interferometer interacts selectively with atoms at a specific velocity. The associated fringe pattern is then ac modulated and revealed by its selective destruction.
Electron beams are a formidable tool for probing nanophotonic systems [1]. Combining electron microscopy with external optical excitation in ultrafast transmission electron microscopes has enabled the mapping of optical near-fields [2] and the bunching of electrons in attosecond pulses [3, 4]. These developments are based on the stimulated inelastic scattering between electrons and light [5, 6], in which the electrons gain energy from or lose energy to the optical field. Recently, the underlying interaction strength of this process has been increased significantly by harnessing resonant enhancement of the optical field and velocity phase matching [7]. Such an increased interaction strength also benefits the spontaneous scattering of electrons with light, thus promising applications like generating complex quantum states of light [8]. In this presentation, we discuss a set of experiments on free electron quantum optics that investigate single-electron-single-photon interactions and probe the resulting entanglement. Specifically, we consider scenarios in which optical waveguide structures are placed inside a transmission electron microscope (TEM) facilitating the interaction. Electrons passing by, for example, an integrated photonic structure (cf. Fig. 1a) can inelastically scatter with the optical mode, leading to the emergence of electron-photon pair states [9]. The resulting correlation between energy-loss electrons and photons, illustrated in Fig. 1b, can be probed employing time- and energy-resolved detection of both particles, revealing a pronounced coincidence peak between their arrival times, schematically shown in Fig. 1c. Extending the photon detection setup by a second detector to allow for Hanbury Brown and Twiss (HBT) measurements, the photon statistics heralded by such energy-loss electrons can be studied [10]. The observed anti-bunching behavior indicates a nonclassical optical state with single-photon properties. The inelastic electron-light scattering underlying the electron-photon pair generation is further expected to induce entanglement in the particle energies [11], however, direct observation of quantum entanglement would be exceedingly difficult given the large number of independent quantum states available in these degrees of freedom. Therefore, we propose experiments based on the quantum eraser scheme to demonstrate this free-electron-photon entanglement in different degrees of freedom [12,13]. Specifically, we consider a double-slit geometry coherently illuminated by an electron beam such that an interference pattern can be observed on a distant screen (cf. Fig. 2a). If electrons passing through the left or right (denoted |Land |R⁠, respectively) slit generate distinct marker photons with vertical (|V)or horizontal (|H) polarization, this interference pattern would disappear due to the entanglement of electron path and photon polarisation (cf. Fig. 2b). However, if this which-path information carried by the marker photon is erased, e.g. by mixing the polarisation states, the interference pattern can be recovered when detecting electrons and photons in coincidence. We describe an extension of this idea to an entanglement test, before discussing possible realistic implementations and presenting preliminary results on several experimental key aspects. In summary, we discuss the inelastic electron-light scattering at integrated photonic structures with applications ranging from coherent electron beam modulation using continuous-wave optical fields to the electron-driven generation of quantum optical states of light. Delving deeper into single electron-single photon interactions, we outline feasible experiments to generate and verify electron-photon entanglement with a potential extension to electron pairs based on entanglement swapping. All this adds to the toolbox of free electron quantum optics, potentially enabling novel sources of quantum light as well as quantum-enhanced sensing in electron microscopy. Generation of correlated electron-photon pairs. (a) Electrons pass over a photonic integrated circuit placed in the sample plane of a TEM, generating photons in the optical waveguides via inelastic scattering. Energy-loss electrons are detected and time-tagged behind an imaging spectrometer in coincidence with photons exiting the waveguide. (b) Inelastic scattering links the electron energy loss (green, right ladder) to the generation of photons (red, left ladder), creating correlations in energy and time. (c) A strong temporal correlation between the loss electrons and detected photons, indicated by the red dot, is observed relative to the uncorrelated zero-loss background electrons (blue line). Free-electron-photon quantum eraser. (a) Coherent electron illumination of a double-slit structure results in interference between the two pathways |Land |R.(b) If the electrons generate distinguishable marker photons, e.g. of orthogonal polarizations |Vand |H⁠, no interference pattern can be observed due to the electron-photon entanglement. (c) Collecting these marker photons and erasing the which-path information, e.g. using a half-wave plate (⁠λ/2⁠), the electron interference can be recovered using electron-photon coincidence detection with single-photon detectors (SPDs) placed behind a polarizing beam splitter (PBS).
Electron microscopes provide a powerful platform for exploring physical phenomena with nanoscale resolution, based on the interaction of free electrons with the excitations of a sample such as phonons, excitons, bulk plasmons, and surface plasmons. The interaction usually results in the absorption or emission of such excitations, which can be detected directly through cathodoluminescence or indirectly through electron energy loss spectroscopy (EELS). However, as we show here, the underlying interaction of a free electron and an arbitrary optical excitation goes beyond what was predicted or measured so far, due to the interplay of entanglement and decoherence of the electron-excitation system. The entanglement of electrons and optical excitations can provide new analytical tools in electron microscopy. For example, it can enable measurements of optical coherence, plasmonic lifetimes, and electronic length scales in matter (such as the Bohr radius of an exciton). We show how these can be achieved using common configurations in electron diffraction and EELS, revealing significant changes in the electron’s coherence, as well as in other quantum information theoretic measures such as purity. Specifically, we find that the purity after interaction with nanoparticles can only take discrete values, versus a continuum of values for interactions with surface plasmons. We quantify the post-interaction density matrix of the combined electron-excitation system by developing a framework based on macroscopic quantum electrodynamics. The framework enables a quantitative account of decoherence due to excitations in any general polarizable material (optical environment). This framework is thus applicable beyond electron microscopy. Particularly in electron microscopy, our work enriches analytical capabilities and informs the design of quantum information experiments with free electrons, allowing control over their quantum states and their decoherence by the optical environment.
Matter wave interferometry with increasingly larger masses could pave the way to understanding the nature of wavefunction collapse, the quantum to classical transition, or even how an object in a spatial superposition interacts with its gravitational field. In order to improve upon the current mass record, it is necessary to move into the nanoparticle regime. In this paper, we provide a design for a nanoparticle Talbot–Lau matter wave interferometer that circumvents the practical challenges of previously proposed designs. We present numerical estimates of the expected fringe patterns that such an interferometer would produce, considering all major sources of decoherence. We discuss the practical challenges involved in building such an experiment, as well as some preliminary experimental results to illustrate the proposed measurement scheme. We show that such a design is suitable for seeing interference fringes with 106 amu SiO2 particles and that this design can be extended to even 108 amu particles by using flight times below the typical Talbot time of the system.
Quantum theory is often cited as being one of the most empirically validated theories in terms of its predictive power and precision. These attributes have led to numerous scientific discoveries and technological advancements. However, the precise relationship between quantum and classical physics remains obscure. The prevailing description is known as decoherence theory, where classical physics emerges from a more general quantum theory through environmental interaction. Sometimes referred to as the decoherence program, it does not solve the quantum measurement problem. We believe experiments performed between the microscopic and macroscopic world may help finish the program. The following considers a free electron that interacts with a surface (the environment), providing a controlled decoherence mechanism. There are non-decohering interactions to be examined and quantified before the weaker decohering effects are filtered out. In the first experiment, an electron beam passes over a surface that’s illuminated by low-power laser light. This induces a surface charge redistribution causing the electron deflection. This phenomenon’s parameters are investigated. This system can be well understood in terms of classical electrodynamics, A second experiment tests decoherence theory by introducing a nanofabricated diffraction grating before the surface. The electron undergoes diffraction through the grating, but as the electron passes over the surface it’s predicted by various physical models that the electron will lose its wave interference property. Image charge based models, which predict a larger loss of contrast than what is observed, are falsified (despite experiencing an image charge force). A theoretical study demonstrates how a loss of contrast may not be due to the irreversible process decoherence, but dephasing (a reversible process due to randomization of the wavefunction’s phase). To resolve this ambiguity, a correlation function on an ensemble of diffraction patterns is analyzed after an electron undergoes either process in a path integral calculation. The diffraction pattern is successfully recovered for dephasing, but not for decoherence, thus verifying it as a potential tool in experimental studies to determine the nature of the observed process.