Interaction of the probe with the specimen in an electron microscope inevitably leads to entanglement between the probe and the scatterer. In spite of the importance of entanglement in many areas of modern physics, this subject has not been touched in the literature. Here, we develop some ideas about entanglement in electron microscopy for a number of scattering mechanisms. The relationship between entropy, density matrices, and coherence is discussed. In addition, we explore the questions “Why is Bragg scattering coherent and energy loss incoherent?” and “When does decoherence play a role?” It seems to be possible to measure decoherence on extremely short timescales of ∼10−8s. This is especially important in view of recent developments in ultrafast electron microscopy.
Interaction of the probe with the specimen in an electron microscope inevitably leads to entanglement between the probe and the scatterer. In spite of the importance of entanglement in many areas of modern physics, this subject has not been touched in the literature. Here, we develop some ideas about entanglement in electron microscopy for a number of scattering mechanisms. The relationship between entropy, density matrices, and coherence is discussed. In addition, we explore the questions “Why is Bragg scattering coherent and energy loss incoherent?” and “When does decoherence play a role?” It seems to be possible to measure decoherence on extremely short timescales of ∼10−8s. This is especially important in view of recent developments in ultrafast electron microscopy.
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.
The major resolution-limiting factor in cryoelectron microscopy of unstained biological specimens is radiation damage by the very electrons that are used to probe the specimen structure. To address this problem, an electron microscopy scheme that employs quantum entanglement to enable phase measurement precision beyond the standard quantum limit has recently been proposed [H. Okamoto, Phys. Rev. A 85, 043810 (2012)]. Here we identify and examine in detail measurement errors that will arise in the scheme. Emphasis is given to considerations concerning inelastic scattering events because, in general, schemes assisted with quantum entanglement are known to be highly vulnerable to lossy processes. We find that the amount of error due to both elastic and inelastic scattering processes is acceptable provided that the electron beam geometry is properly designed and the specimen is sufficiently thin.
Free electrons provide a powerful tool for probing material properties at atomic resolution. Recent advances in ultrafast electron microscopy enable the manipulation of free-electron wave functions using laser pulses. It would be of great importance if one could combine the spatial resolution of electron microscopes with the ability of laser pulses to probe coherent phenomena in quantum systems. To this end, we propose a novel concept that leverages free electrons that are coherently shaped by laser pulses to measure quantum coherence in materials. We develop the quantum theory of interactions between shaped electrons and arbitrary qubit states in materials, and show how the postinteraction electron energy spectrum enables measuring the qubit state (on the Bloch sphere) and the decoherence or relaxation times (T_{2}/T_{1}). Finally, we describe how such electrons can detect and quantify superradiance from multiple qubits. Our scheme can be implemented in ultrafast transmission electron microscopes (UTEM), opening the way toward the full characterization of the state of quantum systems at atomic resolution.
One of the astounding consequences of quantum mechanics is that it allows the detection of a target using an incident probe, with only a low probability of interaction of the probe and the target. This 'quantum weirdness' could be applied in the field of electron microscopy to generate images of beam-sensitive specimens with substantially reduced damage to the specimen. A reduction of beam-induced damage to specimens is especially of great importance if it can enable imaging of biological specimens with atomic resolution. Following a recent suggestion that interaction-free measurements are possible with electrons, we now analyze the difficulties of actually building an atomic resolution interaction-free electron microscope, or "quantum electron microscope". A quantum electron microscope would require a number of unique components not found in conventional transmission electron microscopes. These components include a coherent electron beam-splitter or two-state-coupler, and a resonator structure to allow each electron to interrogate the specimen multiple times, thus supporting high success probabilities for interaction-free detection of the specimen. Different system designs are presented here, which are based on four different choices of two-state-couplers: a thin crystal, a grating mirror, a standing light wave and an electro-dynamical pseudopotential. Challenges for the detailed electron optical design are identified as future directions for development. While it is concluded that it should be possible to build an atomic resolution quantum electron microscope, we have also identified a number of hurdles to the development of such a microscope and further theoretical investigations that will be required to enable a complete interpretation of the images produced by such a microscope.
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).
Atomic resolution transmission electron microscopy (TEM) is an indispensable tool for interdisciplinary investigations of radiation soft or hard materials that evolves rapidly because emerging technologies enable remarkable new experiments [1, 2]. Nowadays, many of them embrace the time domain [2-4]. Beyond materials research, electron microscopy is uniquely suited to study fundamental quantum-mechanical aspects. In fact, it remains concerning that aspects addressing the wave-particle duality, time-dependent measurements, or the entanglement of wave functions and their collapse at a detector still require detailed investigations to guide progress. Certainly, this is no academic matter because such aspects become the bottleneck for the deployment of microscopes that enable studying dynamic processes at high spatiotemporal resolution. It is established practice to describe the scattering of electron ensembles by either a particle picture (Figure 1a) or a wave picture (Figure 1b). Sometimes both pictures are mixed. In spite of calls for solving Schrödinger’s time dependent equation [5], the static Schrödinger equation of wave functions is almost exclusively used to reliably simulate the image formation process using multislice calculations for coherent-elastically scattered electron ensembles [6, 7]. Moreover, the Copenhagen convention of quantum mechanics [8] is adopted, which emphasizes the importance of an observation for the collapse of wave functions (Figure 1b). In order to foster further insight into fundamental quantum-mechanical aspects we pursue a series of experiments with low electron dose rates that guarantee the presence of single electrons in the microscope column at any given time [9]. Consequently, we address the scattering of single electrons (Figure 1c) and build up intensities from electron ensembles over time. In such conditions energy filtered TEM recently revealed the presence of image intensity at sample/vacuum interfaces that cannot be simulated using the established (static) calculation tools even if frozen phonon excitations are considered [10]. In contrast, these intensities can be explained by the time-dependent Schrödinger equation assuming that an energy exchange ΔE occurs during any interaction of the electron with the sample in the Heisenberg limit ΔE = ℏ/2 Δt−1 (coherent-inelastic scattering). In this process a wave package is formed by the superposition of partial waves and a decoherence phase of 0.5-1 radian [10]. The time-dependent Schrödinger equation yields two parameters that characterize the static and the dynamic behavior of any wave function ψ(r, t) = ψ(r) ϕ(t), namely xstatic = ℏ/(2mΔE)1/2 and xdynamic = ℏc/ΔE [11]. The former is the de Broglie wavelength if ΔE is a kinetic energy and the latter becomes an expression for self-coherence if the scattering process is coherent-inelastic in the Heisenberg limit. In these circumstances, the product of Planck’s constant and the speed of light hc is given by the product of the expression for temporal coherence λ2/Δλ and the energy loss ΔE (hc = (λ2/Δλ) ΔE). The validity of the relation is shown in Figure 2 [11]. Thus, the temporal part of Schrödinger’s equation adds contributions of a finite self-coherence length (or time if the electron velocity is considered) to any scattering process, which is neglected if only the static expression is exploited. Further, the formation of wave packages rationalizes the wave-particle duality. The width of wave packages is described by a self-coherence length ls that can vary by over 40 orders of magnitude depending on the strength of interactions [11]. For Coulomb interactions, ls explains the vanishing phase contrast from EF-HRTEM images when the energy loss exceeds values of ΔE > 200 eV [11]. A procedure to experimentally determine the self-coherence length was established earlier by measuring the energy dependent localization of scattered matter waves in surface proximity [10]. Therefore, electron microscopy can be used as a general tool to measure the self-coherence length in real space images on a scale of nanometers and relate this these values to a self-coherence time that reaches attoseconds [12]. Particle and wave descriptions of electron scattering. a) Scattering of electron ensembles in a particle picture. The process is often described by Feynman diagrams, which involves the emission of a virtual photon of lifetime given by Heisenbergs Uncertainty Principle. b) Scattering of electron ensembles in a wave picture that underlies the multi-slice calculations. Infinite wave functions entangle source, sample and detector. The Copenhagen convention requires a wave function collapse upon observation. c) Proposed scattering process of a single electron wave function. The energy exchange occurs in the Heisenberg limit ΔEloss = E2-E1= ℏ/2 (t2-t1)−1= ℏ/2 Δt−1 when a wave package is formed during Δt because of existing energy (wavelength) differences ΔEloss of partial waves [11]. Measurements of self-coherence length and the related self-coherence time at the calculated Heisenberg limit. The colored background marks the quantum realm. The solid lines represent the Heisenberg limit in space and time, which includes the constant ℏc [11].