Angular correlations of photons from solution diffraction at a free-electron laser encode molecular structure

Mendez, Derek; Watkins, Herschel M.; Qiao, Shenglan; Raines, Kevin S.; Lane, Thomas J; Schenk, Gundolf; Nelson, Garrett; Subramanian, Ganesh; Tono, Kensuke; Joti, Yasumasa; Yabashi, Makina; Ratner, Daniel; Doniach, Sebastian

doi:10.1107/s2052252516013956

Cited by 23 publications

(31 citation statements)

References 54 publications

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“…As demonstrated in previous publications, these are sensitive to four‐ and sixfold symmetries of the diffraction pattern, respectively. For crystalline materials, correlations of Bragg reflections dominate . In particular, C is found to peak for Δ corresponding to angles between equivalent lattice planes.…”

Section: Resultsmentioning

confidence: 97%

“…Due to small variations in the sample volume and the solvent amount needed for chamber saturation, the absolute time differs from that shown in Figure a. Cross‐correlations of Bragg reflections have been recently demonstrated as a valuable tool to access structural information beyond conventional pair‐correlation as probed in the standard SAXS analysis. Here, Fourier coefficients of the correlation function

C (q, Δ) = \frac{〈 I (q, ϕ) I {(q, ϕ + Δ 〉}_{ϕ} - {〈 I (q, ϕ) 〉}_{ϕ}^{2}}{{〈 I (q, ϕ) 〉}_{ϕ}^{2}}

are calculated from the 2D diffraction patterns.…”

Section: Resultsmentioning

confidence: 99%

“…This coincides with the transition to the bcc superlattice, where the correlations are observed at the {110} bcc reflection. Since equivalent lattice planes of this reflection show an angle of multiples of 60°, only correlations with a sixfold symmetry are expected . Thus, the absence of c 4 supports the formation of the bcc structure.…”

Section: Resultsmentioning

confidence: 99%

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Monitoring Nanocrystal Self‐Assembly in Real Time Using In Situ Small‐Angle X‐Ray Scattering

Lokteva

Koof

Walther

et al. 2019

Small

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involve a variety of interactions and driving forces between inorganic hard core, organic soft surface-coating ligands, and surrounding solvent molecules. [2,[7][8][9] As a consequence, a thorough understanding of a solvent-mediated assembly process is required to produce NC solids with programmable properties.Here, we have chosen lead sulfide (PbS) nanocrystals as a model system for the investigation of the in situ self-assembly due to the possibility to produce monodisperse particles in a colloidal solution with a precisely controlled size. Additionally, the unique electronic properties of semiconductor PbS NCs with tunable bandgap make them attractive for many potential technological applications, including solar cells, light-emitting diodes, transistors, photodetectors, etc. [10][11][12][13] The structure and degree of order in NC superlattices depend on several factors, such as NC size and shape, ligand length, grafting density, ligand-solvent interactions, NC concentration, solvent evaporation rate (in case of evaporative assembly), and cell geometry or substrate where the assembly takes place. Thus, recent studies on lead chalcogenide NC assemblies revealed the formation of face-centered cubic (fcc) or body-centered cubic (bcc) superstructures as well as lattice distorted facecentered tetragonal (fct) and body-centered tetragonal (bct) superlattices. [14][15][16][17][18] However, their assembling mechanism remains largely unresolved mainly due to the challenge in measuring intermediate transitions between the initial colloidal state and the final superlattice state, especially in real time.Recently, in situ scattering methods have emerged as a powerful characterization tool to study the nucleation and growth of nanoparticle superlattices. [19][20][21][22] Small-angle X-ray scattering (SAXS) allows for monitoring the self-assembly dynamics with subsecond temporal resolution over large sample volumes under controlled conditions (e.g., controlled solvent vapor environment and temperature) and provides realtime information on long range order in the assembled structures. Often, the grazing-incidence small-angle X-ray scattering (GISAXS) technique is applied for in situ measurements, where a drop of nanocrystal suspension is placed on a substrate and evaporated in a controlled manner. [16,20,23,24] However, at small incident angles of the X-ray beam GISAXS is able to probe only up to several monolayers and is thus limited to the surface regime. For bulk measurements transmission SAXS is Self-assembled nanocrystal superlattices have attracted large scientific attention due to their potential technological applications. However, the nucleation and growth mechanisms of superlattice assemblies remain largely unresolved due to experimental difficulties to monitor intermediate states. Here, the self-assembly of colloidal PbS nanocrystals is studied in real time by a combination of controlled solvent evaporation from the bulk solution and in situ small-angle X-ray scattering (SAXS) in transmission geometry. For the fi...

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Section: Resultsmentioning

confidence: 97%

C (q, Δ) = \frac{〈 I (q, ϕ) I {(q, ϕ + Δ 〉}_{ϕ} - {〈 I (q, ϕ) 〉}_{ϕ}^{2}}{{〈 I (q, ϕ) 〉}_{ϕ}^{2}}

are calculated from the 2D diffraction patterns.…”

Section: Resultsmentioning

confidence: 99%

See 1 more Smart Citation

Monitoring Nanocrystal Self‐Assembly in Real Time Using In Situ Small‐Angle X‐Ray Scattering

Lokteva

Koof

Walther

et al. 2019

Small

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“…The application of XSI to nanocrystal-labeled proteins will provide a new window into protein conformational ensembles, especially for folding intermediates and intrinsically disordered proteins (IDPs). Finally, the application of next-generation free electron lasers with very high brilliance could allow measurement of correlated and time resolved distances between multiple sites in a macromolecule, with a time resolution of tens of femtoseconds (Arnlund et al, 2014; Bada et al, 2000; Ball, 2017; Doniach, 2000; Mendez et al, 2014; Mendez et al, 2016; Schenk et al, 2016; SLAC & LCLS, 2010; Smolsky et al, 2007). …”

Section: Commentarymentioning

confidence: 99%

Recording and Analyzing Nucleic Acid Distance Distributions with X‐Ray Scattering Interferometry (XSI)

Zettl

Das

Harbury

et al. 2018

CP Nucleic Acid Chemistry

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Most structural techniques provide averaged information or information about a single predominant conformational state. However, biological macromolecules typically function through series of conformations. Therefore, a complete understanding of macromolecular structures requires knowledge of the ensembles that represent probabilities on a conformational free energy landscape. Here we describe an emerging approach, X-ray scattering interferometry (XSI), a method that provides instantaneous distance distributions for molecules in solution. XSI uses gold nanocrystal labels site-specifically attached to a macromolecule and measures the scattering interference from pairs of heavy metal labels. The recorded signal can directly be transformed into a distance distribution between the two probes. We describe the underlying concepts, present a detailed protocol for preparing samples and recording XSI data, and provide a custom-written graphical user interface to facilitate XSI data analysis. © 2018 by John Wiley & Sons, Inc.

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“…The difference FCs C̃ n ( q 1 , q 2 ) help to mitigate various systematic issues and improve the FXS data quality as compared to

{〈 C_{i i}^{n} (q_{1}, q_{2}) 〉}_{i}

alone [38,56,64]. …”

mentioning

confidence: 99%

Correlations in Scattered X-Ray Laser Pulses Reveal Nanoscale Structural Features of Viruses

et al. 2017

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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.

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Angular correlations of photons from solution diffraction at a free-electron laser encode molecular structure

Abstract: An atomic twinning structure is observed by averaging intensity correlations from many snapshots of gold nanoparticles in solution.

Cited by 23 publications

References 54 publications

Monitoring Nanocrystal Self‐Assembly in Real Time Using In Situ Small‐Angle X‐Ray Scattering

Monitoring Nanocrystal Self‐Assembly in Real Time Using In Situ Small‐Angle X‐Ray Scattering

Recording and Analyzing Nucleic Acid Distance Distributions with X‐Ray Scattering Interferometry (XSI)

Correlations in Scattered X-Ray Laser Pulses Reveal Nanoscale Structural Features of Viruses

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