arXiv subjects

Tatiana Latychevskaia

Publications and source records attributed to Tatiana Latychevskaia.

At least 55 records · Page 3Linked to original sources

arXiv2016

Application of iterative phase-retrieval algorithms to ARPES orbital tomography

Electronic wave functions of planar molecules can be reconstructed via inverse Fourier transform of angle-resolved photoelectron spectroscopy (ARPES) data, provided the phase of the electron wave in the detector plane is known. Since the recorded intensity is proportional to the absolute square of the Fourier transform of the initial state wave function, information about the phase distribution is lost in the measurement. It was shown that the phase can be retrieved in some cases by iterative algorithms using a priori information about the object such as its size and symmetry. We suggest a more generalized and robust approach for the reconstruction of molecular orbitals based on state-of-the-art phase-retrieval algorithms currently used in coherent diffraction imaging. We draw an analogy between the phase problem in molecular orbital imaging by ARPES and of that in optical coherent diffraction imaging by performing an optical analogue experiment on micrometer-sized structures. We successfully reconstruct amplitude and phase of both the micrometer-sized objects and a molecular orbital from the optical and photoelectron far-field intensity distributions, respectively, without any prior information about the shape of the objects.

cond-mat.other↗

arXiv2016

Direct observation of individual charges and their dynamics on graphene by low-energy electron holography

Visualizing individual charges confined to molecules and observing their dynamics with high spatial resolution is a challenge for advancing various fields in science, ranging from mesoscopic physics to electron transfer events in biological molecules. We show here, that the high sensitivity of low-energy electrons to local electric fields can be employed to directly visualize individual charged adsorbates and to study their behaviour in a quantitative way. This makes electron holography a unique probing tool for directly visualising charge distributions with a sensitivity of a fraction of an elementary charge. Moreover, spatial resolution in the nanometer range and fast data acquisition inherent to lens-less low-energy electron holography allows for direct visual inspection of charge transfer processes.

cond-mat.mes-hall↗

arXiv2016

Mapping Unoccupied Electronic States of Freestanding Graphene by Angle-Resolved Low-Energy Electron Transmission

We report angle-resolved electron transmission measurements through freestanding graphene sheets in the energy range of 18 to 30 eV above the Fermi level. The measurements are carried out in a low-energy electron point source microscope, which allows simultaneously probing the transmission for a large angular range. The characteristics of low-energy electron transmission through graphene depend on its electronic structure above the vacuum level. The experimental technique described here allows mapping the unoccupied band structure of freestanding two-dimensional materials as a function of energy and probing angle, respectively in-plane momentum. Our experimental findings are consistent with theoretical predictions of a resonance in the band structure of graphene above the vacuum level [V. U. Nazarov, E. E. Krasovskii, and V. M. Silkin, Physical Review B 87, 041405 (2013)].

cond-mat.mes-hall↗

arXiv2016

Inverted Gabor holography principle for tailoring arbitrary shaped three-dimensional beams

It is well known that by modifying the wavefront in a certain manner, the light intensity can be turned into a certain shape. However, all known light modulation techniques allow for limited light modifications only: focusing within a restricted region in space, shaping into a certain class of parametric curves along the optical axis or bending described by a quadratic-dependent deflection as in the case of Airy beams. We show a general case of classical light wavefront shaping that allows for intensity and phase redistribution into an arbitrary profile including pre-determined switching-off of the intensity. To create an arbitrary three-dimensional path of intensity, we represent the path as a sequence of closely packed individual point-like absorbers and simulate the in-line hologram of the created object set; when such a hologram is contrast inverted, thus giving rise to a diffractor, it creates the pre-determined three-dimensional path of intensity behind the diffractor under illumination. The crucial parameter for a smooth optical path is the sampling of the predetermined curves, which is given by the lateral and axial resolution of the optical system. We provide both, simulated and experimental results to demonstrate the power of this novel method.

physics.optics↗

arXiv2016

Resolution enhancement by extrapolation of coherent diffraction images: A quantitative study on the limits and a numerical study of non-binary and phase objects

In coherent diffractive imaging (CDI) the resolution of the reconstructed object is limited by the numerical aperture of the experimental setup. We present here a theoretical and numerical study for achieving super-resolution by post-extrapolation of coherent diffraction images, such as diffraction patterns or holograms. We demonstrate that a diffraction pattern can unambiguously be extrapolated from only a fraction of the entire pattern and that the ratio of the extrapolated signal to the originally available signal is linearly proportional to the oversampling ratio. While there could be in principle other methods to achieve extrapolation, we devote our discussion to employing iterative phase retrieval methods and demonstrate their limits. We present two numerical studies; namely the extrapolation of diffraction patterns of non-binary and that of phase objects together with a discussion of the optimal extrapolation procedure.

physics.data-an↗

arXiv2016

Order/disorder dynamics in a dodecanethiol-capped gold nanoparticles supracrystal by small-angle ultrafast electron diffraction

In metal nanoparticles (NPs) supracrystals, the metallic core provides some key properties, e.g. magnetization, plasmonic response or conductivity, with the ligand molecules giving rise to others like solubility, assembly or interaction with biomolecules. The formation of these supracrystals depends on a complex interplay between many forces, some stemming from the core, some from the ligands. At present, there is no known approach to characterize the local order of ligand molecules or their dynamics with atomic spatial resolution. Here, we develop a methodology based on small-angle ultrafast electron diffraction combined with angular cross-correlation analysis to characterize a two-dimensional supracrystal of dodecanethiol-coated gold NPs. We retrieve the static arrangement of the ligands, showing that at equilibrium they order in a preferential orientation on the NPs surface and throughout the two-dimensional supracrystal. Upon light excitation, positional disorder is induced in the supracrystal, while its overall homogeneity is surprisingly found to transiently increase. This suggests that transient annealing of the supracrystal takes place within few picoseconds (ps). This methodology will enable the systematic investigation of the dynamical structural properties of nano-assembled materials containing light elements, relevant for biological applications.

cond-mat.mtrl-sci↗

arXiv2015

Imaging outside the box: Resolution enhancement in X-ray coherent diffraction imaging by extrapolation of diffraction patterns

Coherent diffraction imaging is a high-resolution imaging technique whose potential can be greatly enhanced by applying the extrapolation method presented here. We demonstrate enhancement in resolution of a non-periodical object reconstructed from an experimental X-ray diffraction record which contains about 10% missing information, including the pixels in the center of the diffraction pattern. A diffraction pattern is extrapolated beyond the detector area and as a result, the object is reconstructed at an enhanced resolution and better agreement with experimental amplitudes is achieved. The optimal parameters for the iterative routine and the limits of the extrapolation procedure are discussed.

physics.optics↗

arXiv2015

Low-energy electron holographic imaging of individual tobacco mosaic virions

Modern structural biology relies on NMR, X-ray crystallography and cryo-electron microscopy for gaining information on biomolecules at nanometer, sub-nanometer or atomic resolution. All these methods, however, require averaging over a vast ensemble of entities and hence knowledge on the conformational landscape of an individual particle is lost. Unfortunately, there are now strong indications that even X-ray free electron lasers will not be able to image individual molecules but will require nanocrystal samples. Here, we show that non-destructive structural biology of single particles has now become possible by means of low-energy electron holography. As an example, individual tobacco mosaic virions deposited on ultraclean freestanding graphene are imaged at one nanometer resolution revealing structural details arising from the helical arrangement of the outer protein shell of the virus. Since low-energy electron holography is a lens-less technique and since electrons with a deBroglie wavelength of approximately 1 Angstrom do not impose radiation damage to biomolecules, the method has the potential for Angstrom resolution imaging of single biomolecules.

physics.bio-ph↗

arXiv2015

A quantum mechanical scheme to reduce radiation damage in electron microscopy

We show that radiation damage to unstained biological specimens is not an intractable problem in electron microscopy. When a structural hypothesis of a specimen is available, quantum mechanical principles allow us to verify the hypothesis with a very low electron dose. Realization of such a concept requires precise control of the electron wave front. Based on a diffractive electron optical implementation, we demonstrate the feasibility of this new method by both experimental and numerical investigations.

quant-ph↗

arXiv2015

The role of the coherence in the cross-correlation analysis of diffraction patterns from two-dimensional dense mono-disperse systems

The investigation of the static and dynamic structural properties of colloidal systems relies on techniques capable of atomic resolution in real space and femtosecond resolution in time. Recently, the cross-correlation function (CCF) analysis of both X-rays and electron diffraction patterns from dilute and dense aggregates has demonstrated the ability to retrieve information on the sample's local order and symmetry. Open questions remain regarding the role of the beam coherence in the formation of the diffraction pattern and the properties of the CCF, especially in dense systems. Here, we simulate the diffraction patterns of dense two-dimensional monodisperse systems of different symmetries, varying the transverse coherence of the probing wave, and analyze their CCF. We study samples with different symmetries at different size scale, as for example, pentamers arranged into a four-fold lattice where each pentamer is surrounded by triangular lattices, both ordered and disordered. In such systems, different symmetry modulations are arising in the CCF at specific scattering vectors. We demonstrate that the amplitude of the CCF is a fingerprint of the degree of the ordering in the sample and that at partial transverse coherence, the CCF of a dense sample corresponds to that of an individual scattering object.

cond-mat.other↗

arXiv2015

Reconstruction of purely absorbing, absorbing and phase-shifting, and strong phase-shifting objects from their single-shot in-line holograms

We address the problem of reconstructing phase-shifting objects from their single shot in-line holograms. We show that a phase-shifting object cannot be reliably recovered from its in-line hologram by non-iterative reconstruction routines, and that an iterative reconstruction should be applied. We demonstrate examples of simulated in-line holograms of objects with the following properties: purely absorbing, both absorbing and phase shifting, and strong phase-shifting. We investigate the effects of noise and interference contrast in holograms on the reconstruction results and discuss details of an optimal iterative procedure to quantitatively recover the correct absorbing and phase-shifting properties of the object. We also review previously published reconstructions of experimental holograms and summarize the optimal parameters for retrieval of phase-shifting objects from their in-line holograms.

physics.optics↗

arXiv2015

The method of exchange perturbation theory as applied to magnetic ordering in high-Tc materials

We unify the method of exchange perturbation theory for multicenter systems. For the case of exchange degeneracy in the total spin of the system we give a secular equation that is more compact and convenient for calculations than those obtained earlier. On the basis of this formalism we develop an algorithm for calculating the Heisenberg parameter for magnetic materials. Finally, we calculate the characteristics of antiferromagnetic transitions for the high-Tc materials La2-xMeCuO4 and YBa2Cu3O6.

cond-mat.str-el↗

arXiv2015

Invariant Time-Dependent Exchange Perturbation Theory and its Application to the Particles Collision Problem

We present the formalism of Time-dependent Exchange Perturbation Theory (TDEPT) built to all orders of perturbation, for the arbitrary time dependency of perturbation. The theory takes into account the rearrangement of electrons among centres. We show how the formalism can be reduced to the standard form of invariant perturbation theory by 'switching off' the re-arrangement of electrons among centres. The elements of the scattering S-matrix and transitions T-matrix and the formula for the electron scattering differential cross section are derived. The application of the theory to scattering and collision problems is discussed. As an example, we apply the theory to proton scattering on a Lithium atom, calculating the differential and total cross-sections.

quant-ph↗

arXiv2015

Holography and Coherent Diffraction with Low-Energy Electrons: A Route towards Structural Biology at the Single Molecule Level

The current state of the art in structural biology is led by NMR, X-ray crystallography and TEM investigations. These powerful tools however all rely on averaging over a large ensemble of molecules. Here, we present an alternative concept aiming at structural analysis at the single molecule level. We show that by combining electron holography and coherent diffraction imaging estimations concerning the phase of the scattered wave become needless as the phase information is extracted from the data directly and unambiguously. Performed with low-energy electrons the resolution of this lens-less microscope is just limited by the De Broglie wavelength of the electron wave and the numerical aperture, given by detector geometry. In imaging freestanding graphene, a resolution of 2 Angstrom has been achieved revealing the 660.000 unit cells of the graphene sheet from one data set at once. Applied to individual biomolecules the method allows for non-destructive imaging and imports the potential to distinguish between different conformations of proteins with atomic resolution.

physics.atm-clus↗

arXiv2015

Atomically resolved structural determination of graphene and its point defects via extrapolation assisted phase retrieval

Previously reported crystalline structures obtained by an iterative phase retrieval reconstruction of their diffraction patterns seem to be free from displaying any irregularities or defects in the lattice, which appears to be unrealistic. We demonstrate here that the structure of a nanocrystal including its atomic defects can unambiguously be recovered from its diffraction pattern alone by applying a direct phase retrieval procedure not relying on prior information of the object shape. Individual point defects in the atomic lattice are clearly apparent. Conventional phase retrieval routines assume isotropic scattering. We show that when dealing with electrons, the quantitatively correct transmission function of the sample cannot be retrieved due to anisotropic, strong forward scattering specific to electrons. We summarize the conditions for this phase retrieval method and show that the diffraction pattern can be extrapolated beyond the original record to even reveal formerly not visible Bragg peaks. Such extrapolated wave field pattern leads to enhanced spatial resolution in the reconstruction.

cond-mat.mtrl-sci↗

arXiv2014

Terahertz in-line digital holography of dragonfly hindwing: amplitude and phase reconstruction at enhanced resolution by extrapolation

We report here on terahertz (THz) digital holography on a biological specimen. A continuous-wave (CW) THz in-line holographic setup was built based on a 2.52 THz CO2 pumped THz laser and a pyroelectric array detector. We introduced novel statistical method of obtaining true intensity values for the pyroelectric array detector's pixels. Absorption and phase-shifting images of a dragonfly's hind wing were reconstructed simultaneously from single in-line hologram. Furthermore, we applied phase retrieval routines to eliminate twin image and enhanced the resolution of the reconstructions by hologram extrapolation beyond the detector area. The finest observed features are 35 μm width cross veins.

physics.optics↗

arXiv2014

Low-energy electron holographic imaging of gold nanorods supported by ultraclean graphene

An ideal support for electron microscopy shall be as thin as possible and interact as little as possible with the primary electrons. Since graphene is atomically thin and made up of carbon atoms arranged in a honeycomb lattice, the potential to use graphene as substrate in electron microscopy is enormous. Until now graphene has hardly ever been used for this purpose because the cleanliness of freestanding graphene before or after deposition of the objects of interest was insufficient. We demonstrate here by means of low-energy electron holographic imaging that freestanding graphene prepared with the Platinum-metal catalysis method remains ultraclean even after re-exposure to ambient conditions and deposition of gold-nanorods from the liquid phase. In the holographic reconstruction of the gold particles the organic shell surrounding the objects is imaged while it is not detectable in SEM images of the very same sample, demonstrating the tremendous potential of low-energy electron holography for the imaging of graphene-supported single biomolecules.

cond-mat.mtrl-sci↗

arXiv2013

Coherent microscopy at resolution beyond diffraction limit using post-experimental data extrapolation

Conventional microscopic records represent intensity distributions whereby local sample information is mapped onto local information at the detector. In coherent microscopy, the superposition principle of waves holds; field amplitudes are added, not intensities. This non-local representation is spread out in space and interference information combined with wave continuity allows extrapolation beyond the actual detected data. Established resolution criteria are thus circumvented and hidden object details can retrospectively be recovered from just a fraction of an interference pattern.

physics.optics↗