Single-shot 3D coherent diffractive imaging of core-shell nanoparticles with elemental specificity

Pryor, Alan; Rana, Arjun; Xu, Rui; Rodríguez, José A.; Yang, Yongsoo; Gallagher-Jones, Marcus; Jiang, Huaidong; Kanhaiya, Krishan; Nathanson, Michael H.; Park, Jaehyun; Kim, Sunam; Kim, Sang Soo; Nam, Daewoong; Yu, Yue; Fan, Jiadong; Sun, Zhibin; Zhang, Bosheng; Gardner, Dennis F.; Dias, Carlos Sato Baraldi; Joti, Yasumasa; Hatsui, Takaki; Kameshima, Takashi; Inubushi, Yuichi; Tono, Kensuke; Lee, Jim Yang; Yabashi, Makina; Song, Changyong; Ishikawa, Tetsuya; Kapteyn, Henry C.; Murnane, Margaret M.; Heinz, Hendrik; Miao, Jianwei

doi:10.1038/s41598-018-26182-1

Cited by 13 publications

(23 citation statements)

References 60 publications

(61 reference statements)

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“…However, limited spatial resolution (6–8 nm) of the strain map prohibits the acquisition of the full internal 3D atomic structure. [ 30 ] To obtain more detailed atomistic information, molecular dynamics (MD) simulation was proposed to assess the misfit strain in nanocrystals. The MD method predicts atomic positions and displacement at equilibrium by solving the equations of motions for atoms in nanocrystals.…”

Section: Fundamentals Of Misfit Strainmentioning

confidence: 99%

“…The strain distribution is described by the d ‐spacing profile in three different crystallographic directions, which was directly obtained from the atomistic model generated by the MD calculation ( Figure a). [ 30b ]…”

Section: Fundamentals Of Misfit Strainmentioning

confidence: 99%

“…Adapted with permission. [ 30b ] Copyright 2018, American Chemical Society. b) Calculated strain distribution in Pt 50 Cu 50 @Pt nanocrystals with a three‐ or five‐layer shell by finite element simulation.…”

Section: Fundamentals Of Misfit Strainmentioning

confidence: 99%

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Shedding Light on the Role of Misfit Strain in Controlling Core–Shell Nanocrystals

2020

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components including metals, semiconductors, and insulators into various coreshell configurations. The compositional flexibility and structural tunability of coreshell nanocrystals open up tremendous opportunities for obtaining highly designable physical and chemical properties. [5] For most combinations of materials, the epitaxy is associated with the buildup of elastic strains that result from mismatched lattices of the constituent parts. The misfit strain has long been recognized as an important factor that affects the formation and property of epitaxial structures. For example, misfit strain can induce lattice defects such as dislocations, which degrade the quality of the epitaxial layers and cause problems in device fabrication. [6] On the other hand, misfit strain in defect-free epilayers is very useful for optimizing the properties of heterostructures. Elastic strain has been shown to stabilize single crystallite cubic formamidinium lead iodide (FAPbI 3) thin films that offer high quantum efficiency for photodetection. [7] The strain controlled ferroelastic switching in PbTiO 3 thin films also demonstrates high sensitivity for potential applications in pressure sensors and switches. [8] Misfit stain holds more leverage in heteroepitaxial core-shell nanocrystals than in epitaxial thin-films grown on bulk substrates. Owing to the large specific surface area, nanocrystals are enclosed by various crystal facets with distinct crystallographic parameters. Accordingly, nanocrystal heteroepitaxy is characterized by concurrent deposition of epilayers on all the exposed crystal facets of the core nanocrystals. [9] From a crystallographic point of view, epitaxial deposition on different crystal facets may be subjected to a variation of interfacial strains. Besides, misfit strains in core-shell nanocrystals are usually shared by the epilayer and substrate, [10] which gives rise to diversified strain build-up and relaxation processes. Consequently, epitaxial kinetics in different crystallographic directions are largely manipulated by the structure symmetry as well as the size and morphology of the core nanocrystals. [11] On a separate note, nanocrystals are more amenable to strain than the bulk counterparts due to the increase of elasticity at the nanometer length scale. [12] Therefore, strain engineering is increasingly employed to control the formation and functionality of heteroepitaxial nanostructures in recent years. [13] In this review, we summarize recent developments in the understanding and exploitation of misfit strain in heteroepitaxial core-shell nanocrystals (Figure 1). In Section 2, we Heteroepitaxial modification of nanomaterials has become a powerful means to create novel functionalities for various applications. One of the most elementary factors in heteroepitaxial nanostructures is the misfit strain arising from mismatched lattices of the constituent parts. Misfit strain not only dictates epitaxy kinetics for diversifying nanocrystal morphologies but also provides rational control over materials prope...

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Section: Fundamentals Of Misfit Strainmentioning

confidence: 99%

Section: Fundamentals Of Misfit Strainmentioning

confidence: 99%

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Shedding Light on the Role of Misfit Strain in Controlling Core–Shell Nanocrystals

2020

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“…Ultimately, our encryption-decryption approach demonstrably overcomes the difficulties of using FSC as a validation measure for XFEL-SPI, in spite of FSC's popularity 13,16,[18][19][20][21][22][23][24][25][26][27][28][29] . The data throughput from XFELS will rapidly increase because of higher pulse repetition rates 46 , and more efficient sample injection techniques.…”

Section: Discussionmentioning

confidence: 99%

An encryption–decryption framework to validating single-particle imaging

Zhou

Teo

Ayyer

et al. 2021

Sci Rep

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We propose an encryption–decryption framework for validating diffraction intensity volumes reconstructed using single-particle imaging (SPI) with X-ray free-electron lasers (XFELs) when the ground truth volume is absent. This conceptual framework exploits each reconstructed volumes’ ability to decipher latent variables (e.g. orientations) of unseen sentinel diffraction patterns. Using this framework, we quantify novel measures of orientation disconcurrence, inconsistency, and disagreement between the decryptions by two independently reconstructed volumes. We also study how these measures can be used to define data sufficiency and its relation to spatial resolution, and the practical consequences of focusing XFEL pulses to smaller foci. This conceptual framework overcomes critical ambiguities in using Fourier Shell Correlation (FSC) as a validation measure for SPI. Finally, we show how this encryption-decryption framework naturally leads to an information-theoretic reformulation of the resolving power of XFEL-SPI, which we hope will lead to principled frameworks for experiment and instrument design.

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“…The second work we comment on is a recent single-shot 3D CDI experiment in which core-shell cubic Au/Pd nanoparticles have been imaged (Pryor et al, 2018). The experiment was done in forward scattering geometry using 6 keV X-rays, and therefore Compton scattering is completely negligible.…”

Section: Figurementioning

confidence: 99%

On Compton scattering as a source of background in coherent diffraction imaging experiments

Bikondoa¹,

Carbone²

2021

J Synchrotron Radiat

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Compton scattering is generally neglected in diffraction experiments because the incoherent radiation it generates does not give rise to interference effects and therefore is negligible at Bragg peaks. However, as the scattering volume is reduced, the difference between the Rayleigh (coherent) and Compton (incoherent) contributions at Bragg peaks diminishes and the incoherent part may become substantial. The consequences can be significant for coherent diffraction imaging at high scattering angles: the incoherent radiation produces background that smears out the secondary interference fringes, affecting thus the achievable resolution of the technique. Here, a criterion that relates the object shape and the resolution is introduced. The Compton contribution for several object shapes is quantified, and it is shown that the maximum achievable resolution along different directions has a strong dependence on the crystal shape and size.

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Single-shot 3D coherent diffractive imaging of core-shell nanoparticles with elemental specificity

Cited by 13 publications

References 60 publications

Shedding Light on the Role of Misfit Strain in Controlling Core–Shell Nanocrystals

Shedding Light on the Role of Misfit Strain in Controlling Core–Shell Nanocrystals

An encryption–decryption framework to validating single-particle imaging

On Compton scattering as a source of background in coherent diffraction imaging experiments

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