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D Starodub,
A Aquila,
S Bajt,
M Barthelmess, A Barty,
C Bostedt,
J D Bozek,
N Coppola,
R B Doak,
S W Epp, [......],
F Stellato,
S Stern,
G Weidenspointner,
M Frank,
J Ullrich,
L Strüder,
I Schlichting,
H N Chapman,
J C H Spence,
M J Bogan
[show abstract]
[hide abstract]
ABSTRACT: Diffractive imaging with free-electron lasers allows structure determination from ensembles of weakly scattering identical nanoparticles. The ultra-short, ultra-bright X-ray pulses provide snapshots of the randomly oriented particles frozen in time, and terminate before the onset of structural damage. As signal strength diminishes for small particles, the synthesis of a three-dimensional diffraction volume requires simultaneous involvement of all data. Here we report the first application of a three-dimensional spatial frequency correlation analysis to carry out this synthesis from noisy single-particle femtosecond X-ray diffraction patterns of nearly identical samples in random and unknown orientations, collected at the Linac Coherent Light Source. Our demonstration uses unsupported test particles created via aerosol self-assembly, and composed of two polystyrene spheres of equal diameter. The correlation analysis avoids the need for orientation determination entirely. This method may be applied to the structural determination of biological macromolecules in solution.
Nature Communications 12/2012; 3:1276. · 7.40 Impact Factor
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N D Loh,
C Y Hampton,
A V Martin,
D Starodub,
R G Sierra, A Barty,
A Aquila,
J Schulz,
L Lomb,
J Steinbrener, [......],
S Bajt,
M Barthelmess,
P Bucksbaum,
K O Hodgson,
L Strüder,
J Ullrich,
M Frank,
I Schlichting,
H N Chapman,
M J Bogan
Nature 08/2012; · 36.28 Impact Factor
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N D Loh,
C Y Hampton,
A V Martin,
D Starodub,
R G Sierra, A Barty,
A Aquila,
J Schulz,
L Lomb,
J Steinbrener, [......],
S Bajt,
M Barthelmess,
P Bucksbaum,
K O Hodgson,
L Strüder,
J Ullrich,
M Frank,
I Schlichting,
H N Chapman,
M J Bogan
[show abstract]
[hide abstract]
ABSTRACT: The morphology of micrometre-size particulate matter is of critical importance in fields ranging from toxicology to climate science, yet these properties are surprisingly difficult to measure in the particles' native environment. Electron microscopy requires collection of particles on a substrate; visible light scattering provides insufficient resolution; and X-ray synchrotron studies have been limited to ensembles of particles. Here we demonstrate an in situ method for imaging individual sub-micrometre particles to nanometre resolution in their native environment, using intense, coherent X-ray pulses from the Linac Coherent Light Source free-electron laser. We introduced individual aerosol particles into the pulsed X-ray beam, which is sufficiently intense that diffraction from individual particles can be measured for morphological analysis. At the same time, ion fragments ejected from the beam were analysed using mass spectrometry, to determine the composition of single aerosol particles. Our results show the extent of internal dilation symmetry of individual soot particles subject to non-equilibrium aggregation, and the surprisingly large variability in their fractal dimensions. More broadly, our methods can be extended to resolve both static and dynamic morphology of general ensembles of disordered particles. Such general morphology has implications in topics such as solvent accessibilities in proteins, vibrational energy transfer by the hydrodynamic interaction of amino acids, and large-scale production of nanoscale structures by flame synthesis.
Nature 06/2012; 486(7404):513-7. · 36.28 Impact Factor
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A V Martin,
N D Loh,
C Y Hampton,
R G Sierra,
F Wang,
A Aquila,
S Bajt,
M Barthelmess,
C Bostedt,
J D Bozek, [......],
F Stellato,
L Strüder,
J Ullrich,
G Weidenspointner,
T A White,
C B Wunderer, A Barty,
I Schlichting,
M J Bogan,
H N Chapman
[show abstract]
[hide abstract]
ABSTRACT: The emergence of femtosecond diffractive imaging with X-ray lasers has enabled pioneering structural studies of isolated particles, such as viruses, at nanometer length scales. However, the issue of missing low frequency data significantly limits the potential of X-ray lasers to reveal sub-nanometer details of micrometer-sized samples. We have developed a new technique of dark-field coherent diffractive imaging to simultaneously overcome the missing data issue and enable us to harness the unique contrast mechanisms available in dark-field microscopy. Images of airborne particulate matter (soot) up to two microns in length were obtained using single-shot diffraction patterns obtained at the Linac Coherent Light Source, four times the size of objects previously imaged in similar experiments. This technique opens the door to femtosecond diffractive imaging of a wide range of micrometer-sized materials that exhibit irreproducible complexity down to the nanoscale, including airborne particulate matter, small cells, bacteria and gold-labeled biological samples.
Optics Express 06/2012; 20(12):13501-12. · 3.59 Impact Factor
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A. V. Martin,
F. Wang,
N. D. Loh,
T. Ekeberg,
F. R. N. C. Maia,
M. Hantke,
G. van der Schot,
C. Y. Hampton,
R. G. Sierra,
A. Aquila, [......],
F. Stellato,
L. Str¸der,
J. Ullrich,
G. Weidenspointner,
T. A. White,
C. B. Wunderer, A. Barty,
I. Schlichting,
M. J. Bogan,
H. N. Chapman
[show abstract]
[hide abstract]
ABSTRACT: The resolution of single-shot coherent diffractive imaging at X-ray free-electron laser facilities is limited by the low signal-to-noise level of diffraction data at high scattering angles. The iterative reconstruction methods, which phase a continuous diffraction pattern to produce an image, must be able to extract information from these weak signals to obtain the best quality images. Here we show how to modify iterative reconstruction methods to improve tolerance to noise. The method is demonstrated with the hybrid input-output method on both simulated data and single-shot diffraction patterns taken at the Linac Coherent Light Source.
Optics Express. 01/2012; 20(15):16650-16661.
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L. C. Johansson,
D. Arnlund,
T. A. White,
G. Katona,
D. Deponte,
U. Weierstall,
R. B. Doak,
R. L. Shoeman,
L. Lomb,
E. Malmerberg, [......],
E. S. Stern,
L. Struder,
N. Timneanu,
J. Ullrich,
X. Wang,
G. Weidenspointer,
C. Wunderer,
H. N. Chapman,
J. C. H. Spence,
R. Neutze
Nature Methods 01/2012; 9(3):263-265. · 19.28 Impact Factor
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N D Loh,
M J Bogan,
V Elser, A Barty,
S Boutet,
S Bajt,
J Hajdu,
T Ekeberg,
F R N C Maia,
J Schulz,
M M Seibert,
B Iwan,
N Timneanu,
S Marchesini,
I Schlichting,
R L Shoeman,
L Lomb,
M Frank,
M Liang,
H N Chapman
[show abstract]
[hide abstract]
ABSTRACT: We reconstructed the 3D Fourier intensity distribution of monodisperse prolate nanoparticles using single-shot 2D coherent diffraction patterns collected at DESY's FLASH facility when a bright, coherent, ultrafast x-ray pulse intercepted individual particles of random, unmeasured orientations. This first experimental demonstration of cryptotomography extended the expansion-maximization-compression framework to accommodate unmeasured fluctuations in photon fluence and loss of data due to saturation or background scatter. This work is an important step towards realizing single-shot diffraction imaging of single biomolecules.
Physical Review Letters 06/2010; 104(22):225501. · 7.37 Impact Factor
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S. P. Hau-Riege,
S. Boutet, A. Barty,
S. Bajt,
M. J. Bogan,
M. Frank,
J. Andreasson,
B. Iwan,
M. M. Seibert,
J. Hajdu,
A. Sakdinawat,
J. Schulz,
R. Truesch,
H. N. Chapman
Physical Review Letters 01/2010; 104:064801. · 7.37 Impact Factor
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M. J. Bogan,
S. Boutet, A. Barty,
W. H. Benner,
M. Frank,
L. Lomb,
R. Shoeman,
D. Starodub,
M. M. Seibert,
S. P. Hau-Riege, [......],
P. Decorwin-Martin,
S. Bajt,
J. Schulz,
U. Rohner,
B. Iwan,
N. Timneanu,
S. Marchesini,
I. Schlichting,
J. Hajdu,
H. Chapman
Physical Review Special Topics - Accelerators and Beams 01/2010; 13:094791. · 1.52 Impact Factor
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A Barty,
S Marchesini,
H N Chapman,
C Cui,
M R Howells,
D A Shapiro,
A M Minor,
J C H Spence,
U Weierstall,
J Ilavsky,
A Noy,
S P Hau-Riege,
A B Artyukhin,
T Baumann,
T Willey,
J Stolken,
T van Buuren,
J H Kinney
[show abstract]
[hide abstract]
ABSTRACT: Ultralow density polymers, metals, and ceramic nanofoams are valued for their high strength-to-weight ratio, high surface area, and insulating properties ascribed to their structural geometry. We obtain the labrynthine internal structure of a tantalum oxide nanofoam by x-ray diffractive imaging. Finite-element analysis from the structure reveals mechanical properties consistent with bulk samples and with a diffusion-limited cluster aggregation model, while excess mass on the nodes discounts the dangling fragments hypothesis of percolation theory.
Physical Review Letters 09/2008; 101(5):055501. · 7.37 Impact Factor
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A. Barty,
S. Marchesini,
H. N. Chapman,
C. Cui,
M. R. Howells,
D. A. Shapiro,
A. M. Minor,
J. C. H. Spence,
U. Weierstall,
J. Ilavsky,
A. Noy,
S. P. Hau-Riege,
A. B. Artyukhin,
T. Baumann,
T. Willey,
J. Stolken,
T. Buuren van,
J. H. Kinney
Phys Rev Lett. 08/2008; 101(5):055501.
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S. Marchesini,
S. Boutet,
A. E. Sakdinawat,
M.J. Bogan,
S. Bajt, A. Barty,
H.N. Chapman,
M Frank,
S.P. Hau-Riege,
A. Szoke,
C. Cui,
M. R. Howells,
D A Shapiro,
J C H Spence,
J.W. Shaevitz,
J.Y. Lee,
J Hajdu,
M.M. Seibert
[show abstract]
[hide abstract]
ABSTRACT: Advances in the development of free-electron lasers offer the realistic prospect of high-resolution imaging to study the nanoworld on the time-scale of atomic motions. We identify X-ray Fourier Transform holography, (FTH) as a promising but, so far, inefficient scheme to do this. We show that a uniformly redundant array (URA) placed next to the sample, multiplies the efficiency of X-ray FTH by more than one thousand (approaching that of a perfect lens) and provides holographic images with both amplitude- and phase-contrast information. The experiments reported here demonstrate this concept by imaging a nano-fabricated object at a synchrotron source, and a bacterial cell at a soft X-ray free-electron-laser, where illumination by a single 15 fs pulse was successfully used in producing the holographic image. We expect with upcoming hard X-ray lasers to achieve considerably higher spatial resolution and to obtain ultrafast movies of excited states of matter.
03/2008;
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D Starodub,
R B Doak,
K Schmidt,
U Weierstall,
J S Wu,
J C H Spence,
M Howells,
M Marcus,
D Shapiro, A Barty,
H N Chapman
[show abstract]
[hide abstract]
ABSTRACT: We consider a monodispersed Rayleigh droplet beam of water droplets doped with proteins. An intense infrared laser is used to align these droplets. The arrangement has been proposed for electron- and x-ray-diffraction studies of proteins which are difficult to crystallize. This paper considers the effect of thermal fluctuations on the angular spread of alignment in thermal equilibrium, and relaxation phenomena, particularly the damping of oscillations excited as the molecules enter the field. The possibility of adiabatic alignment is also considered. We find that damping times in a high-pressure gas cell as used in x-ray-diffraction experiments are short compared with the time taken for molecules to traverse the beam and that a suitably shaped field might be used for electron-diffraction experiments in vacuum to provide adiabatic alignment, thus obviating the need for a damping gas cell.
The Journal of Chemical Physics 01/2006; 123(24):244304. · 3.33 Impact Factor
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[show abstract]
[hide abstract]
ABSTRACT: In coherent X-ray diffraction microscopy the diffraction pattern generated by a sample illuminated with coherent x-rays is recorded, and a computer algorithm recovers the unmeasured phases to synthesize an image. By avoiding the use of a lens the resolution is limited, in principle, only by the largest scattering angles recorded. However, the imaging task is shifted from the experiment to the computer, and the algorithm's ability to recover meaningful images in the presence of noise and limited prior knowledge may produce aberrations in the reconstructed image. We analyze the low order aberrations produced by our phase retrieval algorithms. We present two methods to improve the accuracy and stability of reconstructions.
11/2005;
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S. Marchesini,
H.N. Chapman, A. Barty,
A. Noy,
S.P. Hau-Riege,
J. M. Kinney,
C. Cui,
M. R. Howells,
R. Rosen,
J C H Spence,
U Weierstall,
D. Shapiro,
T. Beetz,
C Jacobsen,
E. Lima,
A. M. Minor,
H. He
[show abstract]
[hide abstract]
ABSTRACT: The Fourier inversion of phased coherent diffraction patterns offers images without the resolution and depth-of-focus limitations of lens-based tomographic systems. We report on our recent experimental images inverted using recent developments in phase retrieval algorithms, and summarize efforts that led to these accomplishments. These include ab-initio reconstruction of a two-dimensional test pattern, infinite depth of focus image of a thick object, and its high-resolution (~10 nm resolution) three-dimensional image. Developments on the structural imaging of low density aerogel samples are discussed.
11/2005;
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H.N. Chapman, A. Barty,
S. Marchesini,
A. Noy,
C. Cui,
M. R. Howells,
R. Rosen,
H. He,
J C H Spence,
U Weierstall,
T. Beetz,
C Jacobsen,
D. Shapiro
[show abstract]
[hide abstract]
ABSTRACT: Coherent X-ray diffraction microscopy is a method of imaging non-periodic isolated objects at resolutions only limited, in principle, by the largest scattering angles recorded. We demonstrate X-ray diffraction imaging with high resolution in all three dimensions, as determined by a quantitative analysis of the reconstructed volume images. These images are retrieved from the 3D diffraction data using no a priori knowledge about the shape or composition of the object, which has never before been demonstrated on a non-periodic object. We also construct 2D images of thick objects with infinite depth of focus (without loss of transverse spatial resolution). These methods can be used to image biological and materials science samples at high resolution using X-ray undulator radiation, and establishes the techniques to be used in atomic-resolution ultrafast imaging at X-ray free-electron laser sources.
10/2005;
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[show abstract]
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ABSTRACT: This document is the third sub-report of the EUV AIM design study being conducted at LLNL on behalf of International Sematech (ISMT). The purpose of this study as identified in section 1.2 of the statement of work is to research the basic user requirements of an actinic defect characterization tool, potential design configurations and top-level specifications. The objectives of this design study specifically identified in section 1.3 of the statement of work were to: (1) Determine the user requirements of an actinic defect characterization tool; (2) Determine if an EUV AIM tool is an appropriate platform for actinic defect characterization; (3) Determine possible design configurations and top-level performance specifications; (4) Identify potential technical issues and risks of different technical approaches; (5) Provide estimates of cost relating to different technical approaches; and (6) Provide simulated performance for key subsystems and the entire system. The sub-sections of the study to be addressed were accordingly defined in the statement of work as being: (1) Formulation of top-level specifications; (2) Identification of system configurations suitable for meeting the top-level specifications; (3) Preliminary design of imaging systems; (4) Preliminary design of illumination systems; (5) Prediction and comparison of performance through aerial image calculation; (6) Identification of sub-system requirements; (7) Identification of potential vendors; (8) Estimation of system cost; (9) Identification of technical issues; and (10) Definition of technology transfer or development required. Points 1 and 2 have already been addressed in previous reports to ISMT. This document addresses points 3 to 7, and 9 to 10 of the above list--formulation of a preliminary design of the imaging and illumination systems and the evaluation and comparison of potential designs through aerial image analysis. As such this report should be read in conjunction with and in the context of the previous two reports which separately addressed points 1 and 2 above. Item 8, estimation of system cost, will be addressed in a separate confidential report to ISMT. A number of potential configurations for an EUV AIM tool have been studied and technical aspects of the design approaches investigated. The requirements for AIM mode of emulating stepper quality imaging have been spelt out and strategies developed for assessing the suitability of different approaches to satisfying the technical requirements for AIM mode. A synopsis of the approaches considered, and conclusions reached, is presented in Table 17 below. Preliminary designs of several system configurations have been performed, and for each approach potential technical risks have been identified; illumination and source requirements have been analyzed for each implementation and may factor into selection of technical approach. It is important to note that identification of risk or required development does not disqualify a particular approach, rather it serves to raise an issue which must be addressed in any proposal to build a tool.
08/2002
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H N Chapman,
S Bajt, A Barty,
W H Benner,
M J Bogan,
M Frank,
S P Hau-Riege,
R A London,
S Marchesini,
E Spiller,
A Szöke,
B W Woods,
J Hajdu,
M Bergh,
F Burmeister,
C Caleman,
G Huldt,
F R N C Maia,
M M Seibert,
D Van
[show abstract]
[hide abstract]
ABSTRACT: The ultrafast pulses from X-ray free-electron lasers will enable imaging of non-periodic objects at near-atomic resolution [1]. These objects could include single molecules, protein complexes, or virus particles. The specimen would be completely destroyed by the pulse in a Coulomb explosion, but that destruction will only happen after the pulse. The scattering from the sample will give structural information about the undamaged object. There are many technical challenges in carrying out such experiments at an XFEL. We are addressing some of these challenges with experiments at the FLASH soft-X-ray FEL at DESY.
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[show abstract]
[hide abstract]
ABSTRACT: We describe a novel method for solving the twin image problem of in-line holography using a new technique for deterministic phase retrieval combined with numerical back-propagation of the reconstructed complex field. The technique presented here is applicable to any field described by the paraxial scalar wave equation, and is therefore equally applicable to X-ray, electron and neutron optics as well as visible light optics.
Optics Communications.
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[show abstract]
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ABSTRACT: We describe the application of a new technique for the simultaneous determination of three-dimensional absorption and refractive index distributions using a combination of quantitative phase-amplitude microscopy and tomographic reconstruction techniques. We briefly review the phase-amplitude microscopy technique and present experimental results in which we have successfully reconstructed the refractive index profile of two different optical fibres.
Optics Communications.
