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1.
J Opt Soc Am A Opt Image Sci Vis ; 36(12): D31-D40, 2019 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-31873366

RESUMO

This paper provides a tutorial of iterative phase retrieval algorithms based on the Gerchberg-Saxton (GS) algorithm applied in digital holography. In addition, a novel GS-based algorithm that allows reconstruction of 3D samples is demonstrated. The GS-based algorithms recover a complex-valued wavefront using wavefront back-and-forth propagation between two planes with constraints superimposed in these two planes. Iterative phase retrieval allows quantitatively correct and twin-image-free reconstructions of object amplitude and phase distributions from its in-line hologram. The present work derives the quantitative criteria on how many holograms are required to reconstruct a complex-valued object distribution, be it a 2D or 3D sample. It is shown that for a sample that can be approximated as a 2D sample, a single-shot in-line hologram is sufficient to reconstruct the absorption and phase distributions of the sample. Previously, the GS-based algorithms have been successfully employed to reconstruct samples that are limited to a 2D plane. However, realistic physical objects always have some finite thickness and therefore are 3D rather than 2D objects. This study demonstrates that 3D samples, including 3D phase objects, can be reconstructed from two or more holograms. It is shown that in principle, two holograms are sufficient to recover the entire wavefront diffracted by a 3D sample distribution. In this method, the reconstruction is performed by applying iterative phase retrieval between the planes where intensity was measured. The recovered complex-valued wavefront is then propagated back to the sample planes, thus reconstructing the 3D distribution of the sample. This method can be applied for 3D samples such as 3D distribution of particles, thick biological samples, and other 3D phase objects. Examples of reconstructions of 3D objects, including phase objects, are provided. Resolution enhancement obtained by iterative extrapolation of holograms is also discussed.

2.
Sci Rep ; 9(1): 8889, 2019 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-31222124

RESUMO

Low-energy electrons offer a unique possibility for long exposure imaging of individual biomolecules without significant radiation damage. In addition, low-energy electrons exhibit high sensitivity to local potentials and thus can be employed for imaging charges as small as a fraction of one elementary charge. The combination of these properties makes low-energy electrons an exciting tool for imaging charge transport in individual biomolecules. Here we demonstrate the imaging of individual deoxyribonucleic acid (DNA) molecules at the resolution of about 1 nm with simultaneous imaging of the charging of the DNA molecules that is of the order of less than one elementary charge per nanometer. The cross-correlation analysis performed on different sections of the DNA network reveals that the charge redistribution between the two regions is correlated. Thus, low-energy electron microscopy is capable to provide simultaneous imaging of macromolecular structure and its charge distribution which can be beneficial for imaging and constructing nano-bio-sensors.

3.
Appl Opt ; 58(13): 3597-3603, 2019 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-31044868

RESUMO

This work presents an overview of spatial resolution criteria in classical optics, digital optics, and holography. Although the classical Abbe and Rayleigh resolution criteria have been thoroughly discussed in the literature, there are a few issues that still need to be addressed, e.g., the axial resolution criteria for coherent and incoherent radiation (which is a crucial parameter in 3D imaging), the resolution criteria in the Fresnel regime, and the lateral and the axial resolution criteria in digital optics and holography. This work discusses these issues and provides a simple guide on which resolution criteria should be applied for a particular imaging scheme: coherent/incoherent, far- and near-field, lateral and axial resolution. Different resolution criteria such as two-points resolution and the resolution obtained from the image spectrum (diffraction pattern) are compared and demonstrated with simulated examples. It is shown that, for coherent light, the classical Abbe and Rayleigh resolution criteria do not provide accurate estimation of the lateral and axial resolution. The lateral and axial resolution criteria based on the evaluation of the spectrum of the diffracted wave provide more precise estimation of the resolution for coherent and incoherent light. It is also shown that the resolution criteria derived in approximation of the far-field can be applied for the near-field (Fresnel) imaging regime.

4.
Struct Dyn ; 6(2): 024304, 2019 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-31041361

RESUMO

We demonstrate that highly ordered two-dimensional crystals of ligand-capped gold nanoparticles display a local photo-mechanical stiffness as high as that of solids such as graphite. In out-of-equilibrium electron diffraction experiments, a strong temperature jump is induced in a thin film with a femtosecond laser pulse. The initial electronic excitation transfers energy to the underlying structural degrees of freedom, with a rate generally proportional to the stiffness of the material. Using femtosecond small-angle electron diffraction, we observe the temporal evolution of the diffraction feature associated with the nearest-neighbor nanoparticle distance. The Debye-Waller decay for the octanethiol-capped nanoparticle supracrystal, in particular, is found to be unexpectedly fast, almost as fast as the stiffest solid known and observed by the same technique, i.e., graphite. Our observations unravel that local stiffness in a dense supramolecular assembly can be created by van der Waals interactions up to a level comparable to crystalline systems characterized by covalent bonding.

5.
Ultramicroscopy ; 197: 46-52, 2019 02.
Artigo em Inglês | MEDLINE | ID: mdl-30496888

RESUMO

We investigate imaging of moiré structures in free-standing twisted bilayer graphene (TBG) carried out by transmission electron microscopy (TEM) in diffraction and in-line Gabor holography modes. Electron diffraction patterns of TBG acquired at typical TEM electron energies of 80-300 keV exhibit the diffraction peaks caused by diffraction on individual layers. However, diffraction peaks at the scattering angles related to the periodicity of the moiré structure have not been observed in such diffraction patterns. We show that diffraction on moiré structure can create intense diffraction peaks if the energy of the probing electrons is very low, in the range of a few tens of eV. Experimental diffraction patterns of TBG acquired with low-energy electrons of 236 eV exhibiting peaks attributed to the moiré structure periodicity are shown. In holography mode, the intensity of the wave transmitted through the sample and measured in the far-field can be enhanced or decreased depending on the atomic arrangement, as for example AA or AB stacking. Thus, a decrease of intensity in the far-field must not necessarily be associated with some absorption inside the sample but can simply be a result of a particular atomic arrangement. We believe that our findings can be important for exploiting graphene as a support in electron imaging.

6.
Opt Express ; 26(23): 30991-31017, 2018 Nov 12.
Artigo em Inglês | MEDLINE | ID: mdl-30469988

RESUMO

Coherent diffraction imaging (CDI) allows the retrieval of an isolated object's structure, such as a macromolecule, from its diffraction pattern. CDI requires the fulfillment of two conditions: the imaging radiation must be coherent and the object must be isolated. We discuss that it is possible to directly retrieve the molecular structure from its diffraction pattern, which was acquired neither with coherent radiation nor from an individual molecule. This is provided that the molecule exhibits periodicity in one direction, as in the case of fiber diffraction. We demonstrate that, when we apply iterative phase retrieval methods to a fiber diffraction pattern, the repeating unit; that is, the molecule structure, can directly be reconstructed without any prior modeling. For example, we recover the the DNA double helix's structure in three-dimensions from its two-dimensional X-ray fiber diffraction pattern, Photograph (Photo) 51, which was acquired in Raymond Gosling and Rosalind Franklin's famous experiment at a resolution of 3.4 Å.


Assuntos
DNA/química , Imagem Tridimensional/métodos , Difração de Raios X/métodos , Algoritmos , Animais , Humanos , Modelos Moleculares
7.
Appl Opt ; 57(25): 7187-7197, 2018 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-30182978

RESUMO

In this work, issues in phase retrieval in the coherent diffractive imaging (CDI) technique, from discussion on parameters for setting up a CDI experiment to evaluation of the goodness of the final reconstruction, are discussed. The distribution of objects under study by CDI often cannot be cross-validated by another imaging technique. It is therefore important to make sure that the developed CDI procedure delivers an artifact-free object reconstruction. Critical issues that can lead to artifacts are presented and recipes on how to avoid them are provided.

8.
Proc Natl Acad Sci U S A ; 115(29): 7473-7478, 2018 07 17.
Artigo em Inglês | MEDLINE | ID: mdl-29970422

RESUMO

The van der Waals heterostructures, which explore the synergetic properties of 2D materials when assembled into 3D stacks, have already brought to life a number of exciting phenomena and electronic devices. Still, the interaction between the layers in such assembly, possible surface reconstruction, and intrinsic and extrinsic defects are very difficult to characterize by any method, because of the single-atomic nature of the crystals involved. Here we present a convergent beam electron holographic technique which allows imaging of the stacking order in such heterostructures. Based on the interference of electron waves scattered on different crystals in the stack, this approach allows one to reconstruct the relative rotation, stretching, and out-of-plane corrugation of the layers with atomic precision. Being holographic in nature, our approach allows extraction of quantitative information about the 3D structure of the typical defects from a single image covering thousands of square nanometers. Furthermore, qualitative information about the defects in the stack can be extracted from the convergent diffraction patterns even without reconstruction, simply by comparing the patterns in different diffraction spots. We expect that convergent beam electron holography will be widely used to study the properties of van der Waals heterostructures.

9.
Nano Lett ; 18(6): 3421-3427, 2018 06 13.
Artigo em Inglês | MEDLINE | ID: mdl-29733660

RESUMO

The interaction of metals with carbon materials (and specifically with graphene) is of importance for various technological applications. In particular, the intercalation of alkali metals is believed to provide a means for tuning the electronic properties of graphene for device applications. While the macroscopic effects of such intercalation events can readily be studied, following the related processes at an atomic scale in detail and under well-defined experimental conditions constitutes a challenge. Here, we investigate in situ the adsorption and nucleation of the alkali metals K, Cs, and Li on free-standing graphene by means of low-energy electron point source microscopy. We find that alkali metals readily intercalate between the layers of bilayer graphene. In fact, the equilibrium distribution of K and Cs favors a much-higher particle density between the layers than on the single-layer graphene. We obtain a quantitative value for the difference of the free energy of the binding between these two domains. Our study is completed with a control experiment introducing Pd as a representative of the nonalkali metals. Now, we observe cluster formation in equal measure on both single-layer and bilayer graphene; however, there was no intercalation. Our investigations thus constitute the first in situ study of metal-atom sorption of different specificity on free-standing graphene.

10.
Opt Express ; 25(17): 20109-20124, 2017 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-29041695

RESUMO

Mechanical vibrations of components of the optical system is one of the sources of blurring of interference pattern in coherent imaging systems. The problem is especially important in holography where the resolution of the reconstructed objects depends on the effective size of the hologram, which is on the extent of the interference pattern, and on the contrast of the interference fringes. We discuss the mathematical relation between the vibrations, the hologram contrast and the reconstructed object. We show how vibrations can be post-filtered out from the hologram or from the reconstructed object assuming a Gaussian distribution of the vibrations. We also provide a numerical example of compensation for directional motion blur. We demonstrate our approach for light optical and electron holograms, acquired with both, plane- as well as spherical-waves. As a result of such hologram deblurring, the resolution of the reconstructed objects is enhanced by almost a factor of 2. We believe that our approach opens up a new venue of post-experimental resolution enhancement in in-line holography by adapting the rich database/catalogue of motion deblurring algorithms developed for photography and image restoration applications.

11.
Ultramicroscopy ; 182: 276-282, 2017 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-28780143

RESUMO

While imaging individual atoms can routinely be achieved in high resolution transmission electron microscopy, visualizing the potential distribution of individually charged adsorbates leading to a phase shift of the probing electron wave is still a challenging task. Low-energy electrons (30 - 250 eV) are sensitive to localized potential gradients. We employed low-energy electron holography to acquire in-line holograms of individual charged impurities on free-standing graphene. By applying an iterative phase retrieval reconstruction routine we recover the potential distribution of the localized charged impurities present on free-standing graphene.

12.
Nat Commun ; 8: 14440, 2017 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-28195123

RESUMO

There are only a handful of scanning techniques that can provide surface topography at nanometre resolution. At the same time, there are no methods that are capable of non-invasive imaging of the three-dimensional surface topography of a thin free-standing crystalline material. Here we propose a new technique-the divergent beam electron diffraction (DBED) and show that it can directly image the inhomogeneity in the atomic positions in a crystal. Such inhomogeneities are directly transformed into the intensity contrast in the first-order diffraction spots of DBED patterns and the intensity contrast linearly depends on the wavelength of the employed probing electrons. Three-dimensional displacement of atoms as small as 1 angstrom can be detected when imaged with low-energy electrons (50-250 eV). The main advantage of DBED is that it allows visualization of the three-dimensional surface topography and strain distribution at the nanometre scale in non-scanning mode, from a single shot diffraction experiment.

13.
Ultramicroscopy ; 175: 121-129, 2017 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-28236742

RESUMO

Sub-nanometer and nanometer-sized tips provide high coherence electron sources. Conventionally, the effective source size is estimated from the extent of the experimental biprism interference pattern created on the detector by applying the van Cittert Zernike theorem. Previously reported experimental intensity distributions on the detector exhibit Gaussian distribution and our simulations show that this is an indication that such electron sources must be at least partially coherent. This, in turn means that strictly speaking the Van Cittert Zernike theorem cannot be applied, since it assumes an incoherent source. The approach of applying the van Cittert Zernike theorem is examined in more detail by performing simulations of interference patterns for the electron sources of different size and different coherence length, evaluating the effective source size from the extent of the simulated interference pattern and comparing the obtained result with the pre-defined value. The intensity distribution of the source is assumed to be Gaussian distributed, as it is observed in experiments. The visibility or the contrast in the simulated holograms is found to be always less than 1 which agrees well with previously reported experimental results and thus can be explained solely by the Gaussian intensity distribution of the source. The effective source size estimated from the extent of the interference pattern turns out to be of about 2-3 times larger than the pre-defined size, but it is approximately equal to the intrinsic resolution of the imaging system. A simple formula for estimating the intrinsic resolution, which could be useful when employing nano-tips in in-line Gabor holography or point-projection microscopy, is provided.

14.
Proc Natl Acad Sci U S A ; 114(7): 1474-1479, 2017 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-28087691

RESUMO

Imaging single proteins has been a long-standing ambition for advancing various fields in natural science, as for instance structural biology, biophysics, and molecular nanotechnology. In particular, revealing the distinct conformations of an individual protein is of utmost importance. Here, we show the imaging of individual proteins and protein complexes by low-energy electron holography. Samples of individual proteins and protein complexes on ultraclean freestanding graphene were prepared by soft-landing electrospray ion beam deposition, which allows chemical- and conformational-specific selection and gentle deposition. Low-energy electrons do not induce radiation damage, which enables acquiring subnanometer resolution images of individual proteins (cytochrome C and BSA) as well as of protein complexes (hemoglobin), which are not the result of an averaging process.


Assuntos
Holografia/métodos , Proteínas/ultraestrutura , Imagem Individual de Molécula/métodos , Animais , Bovinos , Citocromos c/ultraestrutura , Elétrons , Grafite , Hemoglobinas/ultraestrutura , Holografia/instrumentação , Soroalbumina Bovina/ultraestrutura , Imagem Individual de Molécula/instrumentação , Espectrometria de Massas por Ionização por Electrospray/métodos , Eletricidade Estática , Vácuo
15.
Nano Lett ; 16(9): 5469-74, 2016 09 14.
Artigo em Inglês | MEDLINE | ID: mdl-27536886

RESUMO

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 behavior in a quantitative way. This makes electron holography a unique probing tool for directly visualizing 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.

16.
Appl Opt ; 55(22): 6095-101, 2016 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-27505393

RESUMO

We present a detailed study of two novel methods for shaping the light optical wavefront by employing a transmissive spatial light modulator (SLM). Conventionally, optical Airy beams are created by employing SLMs in the so-called all-phase mode. In the first method, a numerically simulated lens phase distribution is loaded directly onto the SLM, together with the cubic phase distribution. An Airy beam is generated at the focal plane of the numerical lens. We provide for the first time, to the best of our knowledge, quantitative properties of the formed Airy beam. We derive the formula for deflection of the intensity maximum of the so-formed Airy beam, which is different from the quadratic deflection typical of Airy beams. We cross-validate the derived formula by both simulations and experiment. The second method is based on the fact that a system consisting of a transmissive SLM sandwiched between two polarizers can create a transmission function with negative values. This observation alone has the potential for various other wavefront modulations where the transmission function requires negative values. As an example for this method, we demonstrate that a wavefront can be modulated by passing the SLM system with transmission function with negative values by loading an Airy function distribution directly onto the SLM. Since the Airy function is a real-valued function but also with negative values, an Airy beam can be generated by direct transfer of the Airy function distribution onto such an SLM system. In this way, an Airy beam is generated immediately behind the SLM. As both new methods do not employ a physical lens, the two setups are more compact than conventional setups for creating Airy beams. We compare the performance of the two novel methods and the properties of the created Airy beams.

17.
Sci Rep ; 6: 26312, 2016 05 20.
Artigo em Inglês | MEDLINE | ID: mdl-27199254

RESUMO

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.

18.
Nano Lett ; 16(4): 2705-13, 2016 Apr 13.
Artigo em Inglês | MEDLINE | ID: mdl-26918756

RESUMO

The design and the characterization of functionalized gold nanoparticles supracrystals require atomically resolved information on both the metallic core and the external organic ligand shell. At present, there is no known approach to characterize simultaneously the static local order of the ligands and of the nanoparticles, nor their dynamical evolution. In this work, we apply femtosecond small-angle electron diffraction combined with angular cross-correlation analysis, to retrieve the local arrangement from nanometer to interatomic scales in glassy aggregates. With this technique we study a two-dimensional distribution of functionalized gold nanoparticles deposited on amorphous carbon. We show that the dodecanethiol ligand chains, coating the gold cores, order in a preferential orientation on the nanoparticle surface and throughout the supracrystal. Furthermore, we retrieve the dynamics of the supracrystal upon excitation with light and show that the positional disorder is induced by light pulses, while its overall homogeneity is surprisingly found to transiently increase. This new technique will enable the systematic investigation of the static and dynamical structural properties of nanoassembled materials containing light elements, relevant for several applications including signal processing and biology.

19.
Proc Natl Acad Sci U S A ; 112(46): 14212-7, 2015 Nov 17.
Artigo em Inglês | MEDLINE | ID: mdl-26578765

RESUMO

Magnetic skyrmions are promising candidates as information carriers in logic or storage devices thanks to their robustness, guaranteed by the topological protection, and their nanometric size. Currently, little is known about the influence of parameters such as disorder, defects, or external stimuli on the long-range spatial distribution and temporal evolution of the skyrmion lattice. Here, using a large (7.3 × 7.3 µm(2)) single-crystal nanoslice (150 nm thick) of Cu2OSeO3, we image up to 70,000 skyrmions by means of cryo-Lorentz transmission electron microscopy as a function of the applied magnetic field. The emergence of the skyrmion lattice from the helimagnetic phase is monitored, revealing the existence of a glassy skyrmion phase at the phase transition field, where patches of an octagonally distorted skyrmion lattice are also discovered. In the skyrmion phase, dislocations are shown to cause the emergence and switching between domains with different lattice orientations, and the temporal fluctuation of these domains is filmed. These results demonstrate the importance of direct-space and real-time imaging of skyrmion domains for addressing both their long-range topology and stability.

20.
Appl Opt ; 54(9): 2424-34, 2015 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-25968531

RESUMO

Here we present practical methods for simulation and reconstruction of in-line digital holograms recorded with plane and spherical waves. The algorithms described here are applicable to holographic imaging of an object exhibiting absorption as well as phase-shifting properties. Optimal parameters, related to distances, sampling rate, and other factors for successful simulation and reconstruction of holograms are evaluated and criteria for the achievable resolution are worked out. Moreover, we show that the numerical procedures for the reconstruction of holograms recorded with plane and spherical waves are identical under certain conditions. Experimental examples of holograms and their reconstructions are also discussed.

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