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1.
Phys Rev Lett ; 132(20): 206102, 2024 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-38829060

RESUMO

The liquid-to-solid phase transition is a complex process that is difficult to investigate experimentally with sufficient spatial and temporal resolution. A key aspect of the transition is the formation of a critical seed of the crystalline phase in a supercooled liquid, that is, a liquid in a metastable state below the melting temperature. This stochastic process is commonly described within the framework of classical nucleation theory, but accurate tests of the theory in atomic and molecular liquids are challenging. Here, we employ femtosecond x-ray diffraction from microscopic liquid jets to study crystal nucleation in supercooled liquids of the rare gases argon and krypton. Our results provide stringent limits to the validity of classical nucleation theory in atomic liquids, and offer the long-sought possibility of testing nonclassical extensions of the theory.

2.
Phys Chem Chem Phys ; 25(35): 23417-23434, 2023 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-37486006

RESUMO

We apply ultrashort X-ray laser pulses to track optically excited structural dynamics of [Ir2(dimen)4]2+ molecules in solution. In our exploratory study we determine angular correlations in the scattered X-rays, which comprise a complex fingerprint of the ultrafast dynamics. Model-assisted analysis of the experimental correlation data allows us to elucidate various aspects of the photoinduced changes in the excited molecular ensembles. We unambiguously identify that in our experiment the photoinduced transition dipole moments in [Ir2(dimen)4]2+ molecules are oriented perpendicular to the Ir-Ir bond. The analysis also shows that the ground state conformer of [Ir2(dimen)4]2+ with a larger Ir-Ir distance is mostly responsible for the formation of the excited state. We also reveal that the ensemble of solute molecules can be characterized with a substantial structural heterogeneity due to solvent influence. The proposed X-ray correlation approach offers an alternative path for studies of ultrafast structural dynamics of molecular ensembles in the liquid and gas phases.

3.
J Synchrotron Radiat ; 29(Pt 3): 602-614, 2022 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-35510993

RESUMO

Serial crystallography of membrane proteins often employs high-viscosity injectors (HVIs) to deliver micrometre-sized crystals to the X-ray beam. Typically, the carrier medium is a lipidic cubic phase (LCP) media, which can also be used to nucleate and grow the crystals. However, despite the fact that the LCP is widely used with HVIs, the potential impact of the injection process on the LCP structure has not been reported and hence is not yet well understood. The self-assembled structure of the LCP can be affected by pressure, dehydration and temperature changes, all of which occur during continuous flow injection. These changes to the LCP structure may in turn impact the results of X-ray diffraction measurements from membrane protein crystals. To investigate the influence of HVIs on the structure of the LCP we conducted a study of the phase changes in monoolein/water and monoolein/buffer mixtures during continuous flow injection, at both atmospheric pressure and under vacuum. The reservoir pressure in the HVI was tracked to determine if there is any correlation with the phase behaviour of the LCP. The results indicated that, even though the reservoir pressure underwent (at times) significant variation, this did not appear to correlate with observed phase changes in the sample stream or correspond to shifts in the LCP lattice parameter. During vacuum injection, there was a three-way coexistence of the gyroid cubic phase, diamond cubic phase and lamellar phase. During injection at atmospheric pressure, the coexistence of a cubic phase and lamellar phase in the monoolein/water mixtures was also observed. The degree to which the lamellar phase is formed was found to be strongly dependent on the co-flowing gas conditions used to stabilize the LCP stream. A combination of laboratory-based optical polarization microscopy and simulation studies was used to investigate these observations.


Assuntos
Glicerídeos , Lipídeos , Glicerídeos/química , Proteínas de Membrana/química , Viscosidade , Água/química , Difração de Raios X
4.
Small ; 15(50): e1904954, 2019 12.
Artigo em Inglês | MEDLINE | ID: mdl-31729151

RESUMO

X-ray nanodiffraction is applied to study the formation and correlation of domain boundaries in mesocrystalline superlattices of PbS nanocrystals with face-centered cubic structure. Each domain of the superlattice can be described with one of two mesocrystalline polymorphs with different orientational orders. Close to a grain boundary, the lattice constant decreases and the superlattice undergoes an out-of-plane rotation, while the orientation of the nanocrystals with respect to the superlattice remains unchanged. These findings are explained with the release of stress on the expense of specific nanocrystal-substrate interactions. The fact that correlations between adjacent nanocrystals are found to survive the structural changes at most grain boundaries implies that the key to nanocrystal superlattices with macroscopic domain sizes are strengthened interactions with the substrate.

5.
Small ; 14(3)2018 01.
Artigo em Inglês | MEDLINE | ID: mdl-29171683

RESUMO

Ptychographic coherent X-ray imaging is applied to obtain a projection of the electron density of colloidal crystals, which are promising nanoscale materials for optoelectronic applications and important model systems. Using the incident X-ray wavefield reconstructed by mixed states approach, a high resolution and high contrast image of the colloidal crystal structure is obtained by ptychography. The reconstructed colloidal crystal reveals domain structure with an average domain size of about 2 µm. Comparison of the domains formed by the basic close-packed structures, allows us to conclude on the absence of pure hexagonal close-packed domains and confirms the presence of random hexagonal close-packed layers with predominantly face-centered cubic structure within the analyzed part of the colloidal crystal film. The ptychography reconstruction shows that the final structure is complicated and may contain partial dislocations leading to a variation of the stacking sequence in the lateral direction. As such in this work, X-ray ptychography is extended to high resolution imaging of crystalline samples.

6.
Soft Matter ; 14(33): 6849-6856, 2018 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-30095841

RESUMO

The structural rearrangement of polystyrene colloidal crystals under dry sintering conditions has been revealed by in situ grazing incidence X-ray scattering. The measured diffraction patterns were analysed using distorted wave Born approximation (DWBA) theory and the structural parameters of the as-grown colloidal crystals of three different particle sizes were determined for the in-plane and out-of-plane directions in a film. By analysing the temperature evolution of the diffraction peak positions, integrated intensities, and widths, the detailed scenario of the structural rearrangement of crystalline domains at the nanoscale has been revealed, including thermal expansion, particle shape transformation and crystal amorphisation. Based on DWBA analysis, we demonstrate that in the process of dry sintering, the shape of colloidal particles in a crystal transforms from a sphere to a polyhedron. Our results deepen the understanding of the thermal annealing of polymer colloidal crystals as an efficient route for the design of new nano-materials.

7.
Nano Lett ; 17(6): 3511-3517, 2017 06 14.
Artigo em Inglês | MEDLINE | ID: mdl-28485967

RESUMO

We show that the combination of X-ray scattering with a nanofocused beam and X-ray cross correlation analysis is an efficient way for the full structural characterization of mesocrystalline nanoparticle assemblies with a single experiment. We analyze several hundred diffraction patterns at individual sample locations, that is, individual grains, to obtain a meaningful statistical distribution of the superlattice and atomic lattice ordering. Simultaneous small- and wide-angle X-ray scattering of the same sample location allows us to determine the structure and orientation of the superlattice as well as the angular correlation of the first two Bragg peaks of the atomic lattices, their orientation with respect to the superlattice, and the average orientational misfit due to local structural disorder. This experiment is particularly advantageous for synthetic mesocrystals made by the simultaneous self-assembly of nanocrystals and surface-functionalization with conductive ligands. While the structural characterization of such materials has been challenging so far, the present method now allows correlating the mesocrystalline structure with optoelectronic properties.

8.
Phys Rev Lett ; 119(15): 158102, 2017 Oct 13.
Artigo em Inglês | MEDLINE | ID: mdl-29077445

RESUMO

We use extremely bright and ultrashort pulses from an x-ray free-electron laser (XFEL) to measure correlations in x rays scattered from individual bioparticles. This allows us to go beyond the traditional crystallography and single-particle imaging approaches for structure investigations. We employ angular correlations to recover the three-dimensional (3D) structure of nanoscale viruses from x-ray diffraction data measured at the Linac Coherent Light Source. Correlations provide us with a comprehensive structural fingerprint of a 3D virus, which we use both for model-based and ab initio structure recovery. The analyses reveal a clear indication that the structure of the viruses deviates from the expected perfect icosahedral symmetry. Our results anticipate exciting opportunities for XFEL studies of the structure and dynamics of nanoscale objects by means of angular correlations.


Assuntos
Vírus/ultraestrutura , Difração de Raios X , Lasers , Radiografia , Vírus/química
9.
Langmuir ; 31(19): 5274-83, 2015 May 19.
Artigo em Inglês | MEDLINE | ID: mdl-25594683

RESUMO

In situ X-ray diffraction studies of structural evolution of colloidal crystal films formed by polystyrene spherical particles upon incremental heating are reported. The Bragg peak parameters, such as peak position, integrated intensity, and radial and azimuthal widths were analyzed as a function of temperature. A quantitative study of colloidal crystal lattice distortions and mosaic spread as a function of temperature was carried out using Williamson-Hall plots based on mosaic block model. The temperature dependence of the diameter of polystyrene particles was obtained from the analysis of Bragg peaks, and the form factor contribution extracted from the diffraction patterns. Four stages of structural evolution in a colloidal crystal upon heating were identified. Based on this analysis, a model of the heating and melting process in the colloidal crystal film is suggested.

10.
Phys Chem Chem Phys ; 17(11): 7404-10, 2015 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-25700131

RESUMO

The hidden structural properties of semicrystalline polymer films are revealed by nanofocused X-ray scattering studies. X-ray cross-correlation analysis (XCCA) is employed to diffraction patterns from blends of poly(3-hexylthiophene) (P3HT) with gold nanoparticles (AuNPs). Spatially resolved maps of orientational distribution of crystalline domains allow us to distinguish sample regions of predominant face-on morphology, with a continuous transition to edge-on morphology. The average size of crystalline domains was determined to be of the order of 10 nm. As compared to pristine P3HT film, the P3HT/AuNPs blend is characterized by substantial ordering of crystalline domains, which can be induced by Au nanoparticles. The inhomogeneous structure of the polymer film is clearly visualized on the spatially resolved nanoscale 2D maps obtained using XCCA. Our results suggest that the observed changes of the polymer matrix within crystalline regions can be attributed to nanoconfinement in the presence of gold nanoparticles.

11.
J Appl Crystallogr ; 57(Pt 2): 324-343, 2024 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38596737

RESUMO

Fluctuation X-ray scattering (FXS) offers a complementary approach for nano- and bioparticle imaging with an X-ray free-electron laser (XFEL), by extracting structural information from correlations in scattered XFEL pulses. Here a workflow is presented for single-particle structure determination using FXS. The workflow includes procedures for extracting the rotational invariants from FXS patterns, performing structure reconstructions via iterative phasing of the invariants, and aligning and averaging multiple reconstructions. The reconstruction pipeline is implemented in the open-source software xFrame and its functionality is demonstrated on several simulated structures.

13.
Struct Dyn ; 8(4): 044305, 2021 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-34476285

RESUMO

Second-order intensity interferometry was employed to study the spatial and temporal properties of the European X-ray Free-Electron Laser (EuXFEL). Measurements were performed at the soft x-ray Self-Amplified Spontaneous Emission (SASE3) undulator beamline at a photon energy of 1.2 keV in the Self-Amplified Spontaneous Emission (SASE) mode. Two high-power regimes of the SASE3 undulator settings, i.e., linear and quadratic undulator tapering at saturation, were studied in detail and compared with the linear gain regime. The statistical analysis showed an exceptionally high degree of spatial coherence up to 90% for the linear undulator tapering. Analysis of the measured data in spectral and spatial domains provided an average pulse duration of about 10 fs in our measurements. The obtained results will be valuable for the experiments requiring and exploiting short pulse duration and utilizing high coherence properties of the EuXFEL.

14.
Phys Rev Lett ; 104(8): 085502, 2010 Feb 26.
Artigo em Inglês | MEDLINE | ID: mdl-20366944

RESUMO

The long-wavelength (LWL) limit of the elastic interactions in complex non-Bravais lattices is investigated on the basis of microscopic elasticity theory. The conceptual simplicity of our approach enables large-scale simulations in materials with complex crystalline structures. We demonstrate the method by calculating the LWL elastic energy of hcp-based Mg binary alloys for a variety of impurities. Our results show that for large coherent precipitates, the strain-induced interactions control the shape along the hexagonal axis, whereas the surface energy dictates the basal growth. The present formalism enables a straightforward treatment of the long-range elastic interactions in the cluster expansion method for complex crystals.

15.
Sci Rep ; 10(1): 10780, 2020 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-32612095

RESUMO

With the rapid development of short-pulse intense laser sources, studies of matter under extreme irradiation conditions enter further unexplored regimes. In addition, an application of X-ray Free-Electron Lasers (XFELs) delivering intense femtosecond X-ray pulses, allows to investigate sample evolution in IR pump - X-ray probe experiments with an unprecedented time resolution. Here we present a detailed study of the periodic plasma created from the colloidal crystal. Both experimental data and theory modeling show that the periodicity in the sample survives to a large extent the extreme excitation and shock wave propagation inside the colloidal crystal. This feature enables probing the excited crystal, using the powerful Bragg peak analysis, in contrast to the conventional studies of dense plasma created from bulk samples for which probing with Bragg diffraction technique is not possible. X-ray diffraction measurements of excited colloidal crystals may then lead towards a better understanding of matter phase transitions under extreme irradiation conditions.

16.
IUCrJ ; 7(Pt 6): 1102-1113, 2020 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-33209321

RESUMO

An improved analysis for single-particle imaging (SPI) experiments, using the limited data, is presented here. Results are based on a study of bacteriophage PR772 performed at the Atomic, Molecular and Optical Science instrument at the Linac Coherent Light Source as part of the SPI initiative. Existing methods were modified to cope with the shortcomings of the experimental data: inaccessibility of information from half of the detector and a small fraction of single hits. The general SPI analysis workflow was upgraded with the expectation-maximization based classification of diffraction patterns and mode decomposition on the final virus-structure determination step. The presented processing pipeline allowed us to determine the 3D structure of bacteriophage PR772 without symmetry constraints with a spatial resolution of 6.9 nm. The obtained resolution was limited by the scattering intensity during the experiment and the relatively small number of single hits.

17.
Sci Data ; 7(1): 404, 2020 11 19.
Artigo em Inglês | MEDLINE | ID: mdl-33214568

RESUMO

Single Particle Imaging (SPI) with intense coherent X-ray pulses from X-ray free-electron lasers (XFELs) has the potential to produce molecular structures without the need for crystallization or freezing. Here we present a dataset of 285,944 diffraction patterns from aerosolized Coliphage PR772 virus particles injected into the femtosecond X-ray pulses of the Linac Coherent Light Source (LCLS). Additional exposures with background information are also deposited. The diffraction data were collected at the Atomic, Molecular and Optical Science Instrument (AMO) of the LCLS in 4 experimental beam times during a period of four years. The photon energy was either 1.2 or 1.7 keV and the pulse energy was between 2 and 4 mJ in a focal spot of about 1.3 µm x 1.7 µm full width at half maximum (FWHM). The X-ray laser pulses captured the particles in random orientations. The data offer insight into aerosolised virus particles in the gas phase, contain information relevant to improving experimental parameters, and provide a basis for developing algorithms for image analysis and reconstruction.


Assuntos
Colífagos , Lasers , Aceleradores de Partículas , Vírion , Difração de Raios X
18.
IUCrJ ; 6(Pt 4): 635-648, 2019 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-31316808

RESUMO

Higher-order statistical analysis of X-ray scattering from dilute solutions of polydisperse goethite nanorods was performed and revealed structural information which is inaccessible by conventional small-angle scattering. For instance, a pronounced temperature dependence of the correlated scattering from suspension was observed. The higher-order scattering terms deviate from those expected for a perfectly isotropic distribution of particle orientations, demonstrating that the method can reveal faint orientational order in apparently disordered systems. The observation of correlated scattering from polydisperse particle solutions is also encouraging for future free-electron laser experiments aimed at extracting high-resolution structural information from systems with low particle heterogeneity.

19.
Materials (Basel) ; 12(21)2019 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-31652689

RESUMO

Angular X-ray cross-correlation analysis (AXCCA) is a technique which allows quantitative measurement of the angular anisotropy of X-ray diffraction patterns and provides insights into the orientational order in the system under investigation. This method is based on the evaluation of the angular cross-correlation function of the scattered intensity distribution on a two-dimensional (2D) detector and further averaging over many diffraction patterns for enhancement of the anisotropic signal. Over the last decade, AXCCA was successfully used to study the anisotropy in various soft matter systems, such as solutions of anisotropic particles, liquid crystals, colloidal crystals, superlattices composed by nanoparticles, etc. This review provides an introduction to the technique and gives a survey of the recent experimental work in which AXCCA in combination with micro- or nanofocused X-ray microscopy was used to study the orientational order in various soft matter systems.

20.
Struct Dyn ; 6(2): 024301, 2019 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-30915388

RESUMO

We applied angular X-ray Cross-Correlation analysis (XCCA) to scattering images from a femtosecond resolution X-ray free-electron laser pump-probe experiment with solvated PtPOP {[Pt2(P2O5H2)4]4-} metal complex molecules. The molecules were pumped with linear polarized laser pulses creating an excited state population with a preferred orientational (alignment) direction. Two time scales of 1.9 ± 1.5 ps and 46 ± 10 ps were revealed by angular XCCA associated with structural changes and rotational dephasing of the solvent molecules, respectively. These results illustrate the potential of XCCA to reveal hidden structural information in the analysis of time-resolved x-ray scattering data from molecules in solution.

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