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Enzo Rotunno

Publications and source records attributed to Enzo Rotunno.

16 recordsLinked to original sources

Transverse quantum-state characterization of programmable electron optics

Programmable electron optics -- electronically controlled phase plates -- underpin proposals from dose-efficient phase imaging to shaped-electron X-ray sources, nearly all assuming a pure, fully coherent delivered wave whose purity has never been measured. Here we reconstruct the transverse density matrix of a microelectromechanical electrostatic spiral phase plate by mixed-state ptychography, from one four-dimensional STEM scan per state and without added hardware. The delivered beam is substantially mixed: its purity falls from approximately 0.47 to approximately 0.24 as the applied bias grows, inconsistent with a fixed lateral source-blur model, while the real-space coherence width stays near 1 nm. The same scans calibrate the device in situ, allow virtual orbital-angular-momentum sorting and, through a partial-coherence-aware transfer theory, indicate that purifying the output could improve dose efficiency roughly threefold. One acquisition thus becomes a quantum-state acceptance test for programmable electron optics, supplying the purity and coherence that emerging phase-plate and diffractive-imaging schemes assume but leave unquantified.

physics.optics

Quantum tomography of inelastic electron scattering \emph{via} orbital angular momentum states

The physical properties of a quantum system, whether pure or mixed, are described fully by its density matrix. Recovery of the density matrix through projective measurements -- referred to as quantum state tomography -- is a cornerstone of quantum optics and metrology. The implementation of this approach in transmission electron microscopy, in particular for the characterisation of an electron beam after inelastic scattering, has remained a longstanding challenge as a result of the complexity of scanning high-dimensional phase spaces, with the number of required measurements growing quadratically with space dimensionality. Here, we introduce a simplified approach by restricting tomography to the electron orbital angular momentum (OAM) subspace. By using an electron optical device known as an OAM sorter, we discretise the phase space into a finite set of measurable states, thus significantly reducing the experimental and computational burden. The resulting measurements suffice to probe essential features of inelastic scattering. We demonstrate the technique by studying the inelastic scattering of a structured electron probe exciting volume plasmons in a carbon film. The combined use of a structured beams and OAM-resolved quantum tomography reveals symmetry-breaking effects and offers insight into the coherence and evolution of the scattered quantum states. Analysis of the diagonalised density matrices further reveals the nature of the induced state transitions, demonstrating the power of the approach for quantum tomography of electron scattering.

quant-ph

Designing electrostatic MEMS-based electron optics: the case of the spiral phase plate

A new generation of microfabricated MEMS for electron optics is changing electron microscopy for the better. These devices allow operations on the electron beam that are impossible with conventional electron optics. Unprecedented phase landscapes like tunable spiral phase plates and localized strong phase gradients are just some examples of what can be achieved. This work establishes the methodological foundation to design and control MEMS based phase plates. The design strategy is rooted on a novel analytical and numerical modeling of thin electrodes with accurate account of the fringing fields having a major role in the thin-MEMS geometry. We designed, fabricated and characterized experimentally a spiral phase plate, and assessed the quality of the generated vortex beam while discussing the most relevant control parameters and design approaches.

physics.ins-det

Artificial Intelligence-Assisted Workflow for Transmission Electron Microscopy: From Data Analysis Automation to Materials Knowledge Unveiling

(Scanning) transmission electron microscopy ((S)TEM) has significantly advanced materials science but faces challenges in correlating precise atomic structure information with the functional properties of devices due to its time-intensive nature. To address this, we introduce an analytical workflow for the holistic characterization, modelling, and simulation of device heterostructures. This workflow automates the experimental (S)TEM data analysis, providing an in-depth characterization of crystallographic information, 3D orientation, elemental composition, and strain distribution. It reduces a process that typically takes days for a trained human into an automatic routine solved in minutes. Utilizing a physics-guided artificial intelligence model, it generates representative descriptions of materials and samples. The workflow culminates in creating digital twins, 3D finite element and atomic models of millions of atoms, enabling simulations that provide crucial insights into device behaviour in practical applications. Demonstrated with SiGe planar heterostructures for scalable spin qubits, the workflow links digital twins to theoretical properties, revealing how atomic structure impacts materials and functional properties such as spatially-resolved phononic or electronic characteristics, or (inverse) spin orbit lengths. The versatility of our workflow is demonstrated through its application to a wide array of materials systems, device configurations, and sample morphologies.

cond-mat.mtrl-sci

Near-real-time diagnosis of electron optical phase aberrations in scanning transmission electron microscopy using an artificial neural network

The key to optimizing spatial resolution in a state-of-the-art scanning transmission electron microscope is the ability to precisely measure and correct for electron optical aberrations of the probe-forming lenses. Several diagnostic methods for aberration measurement and correction with maximum precision and accuracy have been proposed, albeit often at the cost of relatively long acquisition times. Here, we illustrate how artificial intelligence can be used to provide near-real-time diagnosis of aberrations from individual Ronchigrams. The demonstrated speed of aberration measurement is important as microscope conditions can change rapidly, as well as for the operation of MEMS-based hardware correction elements that have less intrinsic stability than conventional electromagnetic lenses.

physics.ins-det

Computational ghost imaging for transmission electron microscopy

While transmission electron microscopes (TEM) can achieve a much higher resolution than optical microscopes, they face challenges of damage to samples during the high energy processes involved. Here, we explore using computational ghost imaging techniques in electron microscopy to reduce the total required intensity. The technological lack of the equivalent high-resolution, optical spatial light modulator for electrons means that a different approach needs to be pursued. To this end, we show a beam shaping technique based on the use of a distribution of electrically charged metal needles to structure the beam, alongside a novel reconstruction method to handle the resulting highly non-orthogonal patterns. Second, we illustrate the application of this ghost imaging approach in electron microscopy. To test the full extent of the capabilities of this technique, we realised an analogous optical setup method. In both regimes, the ability to reduce the amount of total illumination intensity is evident in comparison to raster scanning.

physics.optics

Single-Pixel Imaging in Space and Time with Optically-Modulated Free Electrons

Single-pixel imaging, originally developed in light optics, facilitates fast three-dimensional sample reconstruction, as well as probing with light wavelengths undetectable by conventional multi-pixel detectors. However, the spatial resolution of optics-based single-pixel microscopy is limited by diffraction to hundreds of nanometers. Here, we propose an implementation of single-pixel imaging relying on attainable modifications of currently available ultrafast electron microscopes in which optically-modulated electrons are used instead of photons to achieve sub-nanometer spatially- and temporally-resolved single-pixel imaging. We simulate electron beam profiles generated by interaction with the optical field produced by an externally programable spatial light modulator and demonstrate the feasibility of the method by showing that the sample image and its temporal evolution can be reconstructed using realistic imperfect illumination patterns. Electron single-pixel imaging holds strong potential for application in low-dose probing of beam-sensitive biological and molecular samples, including rapid screening during in-situ experiments.

physics.optics

Theoretical and practical aspects of the design and production of synthetic holograms for transmission electron microscopy

Beam shaping - the ability to engineer the phase and the amplitude of massive and massless particles - has long interested scientists working on communication, imaging and the foundations of quantum mechanics. In light optics, the shaping of electromagnetic waves (photons) can be achieved using techniques that include, but are not limited to, direct manipulation of the beam source (as in X-ray Free Electron Lasers (XFELs) and Synchrotrons), deformable mirrors, spatial light modulators, mode converters and holograms. The recent introduction of holographic masks for electrons provides new possibilities for electron beam shaping. Their fabrication has been made possible by advances in micrometric and nanometric device production using lithography and focused ion beam patterning. This article provides a tutorial on the generation, production and analysis of synthetic holograms for transmission electron microscopy. It begins with an introduction to synthetic holograms, outlining why they are useful for beam shaping to study material properties. It then focuses on the fabrication of the required devices from theoretical and experimental perspectives, with examples taken from both simulations and experimental results. Applications of synthetic electron holograms as aberration correctors, electron vortex generators and spatial mode sorters are then presented.

physics.optics

Exploring the spatial features of electronic transitions in molecular and biomolecular systems by swift electrons

Electron energy loss spectroscopy is consolidating as a powerful tool to explore electronic (as well as vibrational) excitations of matter, including molecules. Performed in a scanning transmission electron microscope, this technique is based on inelastic scattering of fast electrons in a thin specimen. Very recently, new electron optics configuration have been introduced, opening the way to the analysis of the single components of orbital angular momentum of the outcoming electrons, that convey additional information on the spatial features of the investigated excitations: innovative double-dispersed spectroscopic experiments for metallic nanostructures have been therefore suggested. We propose here to extend this technology to probe molecular and supra-molecular systems, devising new kind of experiments: using state of the art quantum chemical methods to describe the molecular system in presence of an electron beam in a configuration that avoid molecular damage, we show that scattered electrons acquire the different azimuthal components of induced molecular transition potentials. Numerical simulations performed for systems of increasing size, point out that the conceived new technique can open up the possibility of probing the multipolar components and even the chirality of molecular transitions, superseding the usual optical spectroscopies for those cases that are problematic, such as dipole-forbidden transitions, at a very high spatial resolution.

physics.chem-ph

The role of 2s Bloch wave state excitations on STEM-HAADF intensity in quantitative analysis of alloys

In this work, we emphasize the important contribution of the 2s Bloch wave state to the properties of a STEM electron probe propagating on an atomic column. For a strong enough column potential, the confinement of the 2s state leads to a long-period oscillation of the electron wave function, which is reflected in the resulting STEM-HAADF intensity. We show how this influences STEM composition quantification even at large thicknesses. We found additionally that the excitation of the 2s state affects the intensity of alloys where long-range order phenomena are present, which in turn provides a way to probe the degree of order in alloys.

cond-mat.mtrl-sci

A general framework for conformal transformations in electron optics

The implementation of log-pol transformation has recently introduced a new boost in electron optics with charged matter vortices, allowing to map conformally between linear and orbital angular momentum (OAM) states and to measure them. That coordinate change belongs to the general framework of Hossack's transformations and it has been recently realized efficiently by means of electrostatic elements. In this letter we show that it is a general property of those conformal transformations to be produced by harmonic phase elements and therefore to admit an electrostatic implementation in the electron optics scenario. We consider a new kind of conformal mapping, the circular-sector transformation, which has been recently introduced for OAM multiplication and division in optics, and discuss how it represents a general solution of Laplace's equation, showing the analogy of the generating phase elements with projected multipole fields and linear charge distributions. Moreover, we demonstrate its capability to perform the sorting of multipole wavefronts, discovering a novel and effective method to measure the strength and orientation of a dipole field in a fast, compact and direct way.

quant-ph

Efficient molecule discrimination in electron microcopy through an optimized orbital angular momentum sorter

We consider the problem of discriminating macromolecular structures in an electron microscope, through a specific beam shaping technique. Our approach is based on maximizing the which-molecule information extracted from the state of each electron. To this aim, the optimal observables are derived within the framework of quantum state discrimination, which allows one to fully account from the quantum character of the probe. We simulate the implementation of such optimal observable on a generalized orbital angular momentum (OAM) sorter and benchmark its performance against the best known real space approach.

quant-ph

Sum rules in zone axis STEM-orbital angular momentum resolved electron magnetic chiral dichroism

In this work we derive sum rules for orbital angular momentum(OAM) resolved electron magnetic chiral dichroism (EMCD) which enable the evaluation of the strength of spin and orbital components of the atomic magnetic moments in a crystalline sample. We also demonstrate through numerical simulations that these rules appear to be only slightly dependent from the dynamical diffraction of the electron beam in the sample, making possible their application without the need of additional dynamical diffraction calculations.

cond-mat.mtrl-sci

Experimental demonstration of an electrostatic orbital angular momentum sorter for electrons

We report the first experimental demonstration of an electrostatic electron orbital angular momentum (OAM) sorter, which can be used to analyze the OAM states of electrons in a transmission electron microscope. We verify the sorter functionality for several electron beams possessing different superpositions of OAM states, and use it to record the electron beams OAM spectra. Our current electrostatic OAM sorter has an OAM resolution of 2 in the units of h/bar - the reduced Planck constant. It is expected to increase the OAM resolution of the sorter to the optimal resolution of 1 in the future via fine control of the sorting phase elements.

physics.ins-det

Orbital-angular-momentum-resolved electron magnetic chiral dichroism

We propose a highly efficient atomically-resolved mode of electron magnetic chiral dichroism. This method exploits the recently introduced orbital angular momentum spectrometer to analyze the inelastically scattered electrons allowing for simultaneous dispersion in both energy and angular momentum. The technique offers several advantages over previous formulations of electron magnetic chiral dichroism as it requires much simpler experimental conditions in terms of specimen orientation and thickness. A novel simulation algorithm, based on the multislice description of the beam propagation, is used to anticipate the advantages of the new approach over current electron magnetic chiral dichroism implementations. Numerical calculations confirm an increased magnetic signal to noise ratio with in plane atomic resolution.

cond-mat.mtrl-sci

Orbital angular momentum and energy loss characterization of plasmonic excitations in metallic nanostructures in TEM

Recently, a new device to measure the Orbital Angular Momentum (OAM) electronic spectrum after elastic/inelastic scattering in a transmission electron microscope has been introduced. We modified the theoretical framework needed to describe conventional low loss electron energy loss spectroscopy (EELS) experiments in transmission electron microscopes (TEM) to study surface plasmons in metallic nanostructures, to allow for an OAM post selection and devise new experiments for the analysis of these excitations in nanostructures. We found that unprecedented information on the symmetries and on the chirality of the plasmonic modes can be retrieved even with limited OAM and energy resolutions.

physics.ins-det