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The spatial distributions of anti-bonding $\pi^\ast$ and $\sigma^\ast$ states in epitaxial graphene multilayers are mapped using electron energy-loss spectroscopy in a scanning transmission electron microscope. Inelastic channeling simulations validate the interpretation of the spatially-resolved signals in terms of electronic orbitals, and demonstrate the crucial effect of the material thickness on the experimental capability to resolve the distribution of unoccupied states. This work illustrates the current potential of core-level electron energy-loss spectroscopy towards the direct visualization of electronic orbitals in a wide range of materials, of huge interest to better understand chemical bonding among many other properties at interfaces and defects in solids.

In light optics, beams with orbital angular momentum (OAM) can be produced by employing a properly-tuned two-cylinder-lens arrangement, also called $\pi$/2 mode converter. It is not possible to convey this concept directly to the beam in an electron microscope due to the non-existence of cylinder lenses in commercial transmission electron microscope (TEM). A viable work-around are readily-available electron optical elements in the form of quadrupole lenses. In a proof-of-principle experiment in 2012, it has been shown that a single quadrupole in combination with a Hilbert phase plate produces a spatially-confined, transient vortex mode. Here, an analogue to an optical $\pi$/2 mode converter is realized by repurposing a CEOS DCOR probe corrector in an aberration corrected TEM in a way that it resembles a dual cylinder lens using two quadrupoles. In order to verify the presence of OAM in the output beam, a fork dislocation grating is used as an OAM analyser. The possibility to use magnetic quadrupole fields instead of, e.g., prefabricated fork dislocation gratings to produce electron beams carrying OAM enhances the beam brightness by almost an order of magnitude and delivers switchable high-mode purity vortex beams without unwanted side-bands.

Landau levels and states of electrons in a magnetic field are fundamental quantum entities underlying the quantum-Hall and related effects in condensed matter physics. However, the real-space properties and observation of Landau wave functions remain elusive. Here we report the first real-space observation of Landau states and the internal rotational dynamics of free electrons. States with different quantum numbers are produced using nanometer-size electron vortex beams, with a radius chosen to match the waist of the Landau states, in a quasi-uniform magnetic field. Scanning the beams along the propagation direction, we reconstruct the rotational dynamics of the Landau wave functions with angular frequency ~100 GHz. We observe that Landau modes with different azimuthal quantum numbers belong to three classes, which are characterized by rotations with zero, Larmor, and cyclotron frequencies, respectively. This is in sharp contrast to the uniform cyclotron rotation of classical electrons, and in perfect agreement with recent theoretical predictions., Comment: 10 pages, 4 figures

Electron vortex beams were only recently discovered and their potential as a probe for magnetism in materials was shown. Here we demonstrate a new method to produce electron vortex beams with a diameter of less than 1.2 \AA. This unique way to prepare free electrons to a state resembling atomic orbitals is fascinating from a fundamental physics point of view and opens the road for magnetic mapping with atomic resolution in an electron microscope.

The holographic mask technique is used to create freely moving electrons with quantized angular momentum. With electron optical elements they can be focused to vortices with diameters below the nanometer range. The understanding of these vortex beams is important for many applications. Here we present a theory of focused free electron vortices. The agreement with experimental data is excellent. As an immediate application, fundamental experimental parameters like spherical aberration and partial coherence are determined., Comment: 4 pages, 5 figures