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At least 361 records · Page 20

Oxyanion Surface Complexes Control the Kinetics and Pathway of Ferrihydrite Transformation to Goethite and Hematite

The rate and pathway of ferrihydrite (Fh) transformation at oxic conditions to more stable products is controlled largely by temperature, pH, and the presence of other ions in the system such as nitrate (NO 3 - ), sulfate (SO 4 2- ), and arsenate (AsO 4 3- ). Although the mechanism of Fh transformation and oxyanion complexation have been separately studied, the effect of surface complex type and strength on the rate and pathway remains only partly understood. We have developed a kinetic model that describes the effects of surface complex type and strength on Fh transformation to goethite (Gt) and hematite (Hm). Two sets of oxyanion-adsorbed Fh samples were prepared, nonbuffered and buffered, aged at 70 ± 1.5 °C, and then characterized using synchrotron X-ray scattering methods and wet chemical analysis. Kinetic modeling showed a significant decrease in the rate of Fh transformation for oxyanion surface complexes dominated by strong inner-sphere (SO 4 2- and AsO 4 3- ) versus weak outer-sphere (NO 3 - ) bonding and the control. The results also showed that the Fh transformation pathway is influenced by the type of surface complex such that with increasing strength of bonding, a smaller fraction of Gt forms compared with Hm. In conclusion, these findings are important for understanding and predicting the role of Fh in controlling the transport and fate of metal and metalloid oxyanions in natural and applied systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

WE-AB-202-06: Correlating Lung CT HU with Transformation-Based and Xe-CT Derived Ventilation

Purpose: Regional lung ventilation is useful to reduce radiation-induced function damage during lung cancer radiation therapy. Recently a new direct HU (Hounsfield unit)-based method was proposed to estimate the ventilation potential without image registration. The purpose of this study is to examine if there is a functional dependence between HU values and transformation-based or Xe-CT derived ventilation. Methods: 4DCT images acquired from 13 patients prior to radiation therapy and 4 mechanically ventilated sheep subjects which also have associated Xe-CT images were used for this analysis. Transformation-based ventilation was computed using Jacobian determinant of the transformation field between peak-exhale and peak-inhale 4DCT images. Both transformation and Xe-CT derived ventilation was computed for each HU bin. Color scatter plot and cumulative histogram were used to compare and validate the direct HU-based method. Results: There was little change of the center and shape of the HU histograms between free breathing CT and 4DCT average, with or without smoothing, and between the repeated 4DCT scans. HU of −750 and −630 were found to have the greatest transformation-based ventilation for human and sheep subjects, respectively. Maximum Xe-CT derived ventilation was found to locate at HU of −600 in sheep subjects. The curve between Xe-CT ventilation and HU was noisy for tissue above HU −400, possibly due to less intensity change of Xe gas during wash-out and wash-in phases. Conclusion: Both transformation-based and Xe-CT ventilation demonstrated that lung tissues with HU values in the range of (-750, −600) HU have the maximum ventilation potential. The correlation between HU and ventilation suggests that HU might be used to help guide the ventilation calculation and make it more robust to noise and image registration errors. Research support from NIH grants CA166703 and CA166119 and a gift from Roger Koch.

60 APPLIED LIFE SCIENCES↗

Ink-substrate interactions during 3D printing revealed by time-resolved coherent X-ray scattering

Additive printing techniques are regarded as revolutionary and versatile methods of advanced device manufacturing, stemming from the possibility to pattern materials on a custom-based approach and the potential to create novel microstructures and achieve new functionalities. Despite these advantages, the inherent anisotropy of the printing process is a source of property gradients within the printed materials, often associated with variable and/or poor performance. Up to date, the evolutionary pathways associated with printing have largely remained unaddressed, mainly owing to the difficulty to study the transformations induced in the material during processing. Time-resolved coherent X-ray scattering techniques, such as X-ray photon correlation spectroscopy, enable the in situ study of transient nanoscale and mesoscale states in a large variety of materials, including amorphous ones, by directly accessing the most relevant timescales and length scales of their nanoscale and mesoscale dynamics, self-assembly, and mesostructure evolution. In this work, we conduct in operando studies of continuous-flow direct writing with colloidal inks, focusing on how the ink formulation and ink-substrate interactions affect the processes that determine the macroscopic properties of the printed materials. We find fundamental differences in the ink structural relaxations emerging from the primary colloid properties (monodisperse versus aggregated colloids) and the substrates surface energy and mechanical properties. Our work helps to reveal and quantify the basic science governing the evolution of 3D-printed materials during processing, ultimately improving engineering criteria for the design of printable materials.

36 MATERIALS SCIENCE↗

Local structure of temperature and pH-sensitive colloidal microgels

The temperature dependence of the local intra-particle structure of colloidal microgel particles, composed of interpenetrated polymer networks, has been investigated by small-angle neutron scattering at different pH and concentrations, in the range (299÷315) K, where a volume phase transition from a swollen to a shrunken state takes place. Data are well described by a theoretical model that takes into account the presence of both interpenetrated polymer networks and cross-linkers. Two different behaviors are found across the volume phase transition. At neutral pH and T ≈ 307 K, a sharp change of the local structure from a water rich open inhomogeneous interpenetrated polymer network to a homogeneous porous solid-like structure after expelling water is observed. Differently, at acidic pH, the local structure changes almost continuously. These findings demonstrate that a fine control of the pH of the system allows to tune the sharpness of the volume-phase transition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Experimental setup combining in situ hard X-ray photoelectron spectroscopy and real-time surface X-ray diffraction for characterizing atomic and electronic structure evolution during complex oxide heterostructure growth

We describe the next-generation system for in situ characterization of a complex oxide thin film and heterostructure growth by pulsed laser deposition (PLD) using synchrotron hard X-rays. The system consists of a PLD chamber mounted on a diffractometer allowing both real-time surface X-ray diffraction (SXRD) and in situ hard X-ray photoelectron spectroscopy (HAXPES). HAXPES is performed in the incident X-ray energy range from 4 to 12 keV using a Scienta EW4000 electron energy analyzer mounted on the PLD chamber fixed parallel with the surface normal. In addition to the standard application mode of HAXPES for disentangling surface from bulk properties, the increased penetration depth of high energy photoelectrons is used for investigation of the electronic structure changes through thin films grown deliberately as variable thickness capping layers. Such heterostructures represent model systems for investigating a variety of critical thickness and dead layer phenomena observed at complex oxide interfaces. In this new mode of operation, in situ HAXPES is used to determine the electronic structure associated with unique structural features identified by real-time SXRD during thin film growth. The system is configured for using both laboratory excitation sources off-line and on-line operation at beamline 33-ID-D at the Advanced Photon Source. We illustrate the performance of the system by preliminary scattering and spectroscopic data on oxygen vacancy ordering induced perovskite-to-brownmillerite reversible phase transformation in La 2/3 Sr 1/3 MnO 3 films capped with oxygen deficient SrTiO 3–δ (100) layers of varying thickness.

47 OTHER INSTRUMENTATION↗

CONTIN XPCS : software for inverse transform analysis of X-ray photon correlation spectroscopy dynamics

X-ray photon correlation spectroscopy (XPCS) and dynamic light scattering (DLS) reveal materials dynamics using coherent scattering, with XPCS permitting the investigation of dynamics in a more diverse array of materials than DLS. Heterogeneous dynamics occur in many material systems. The authors' recent work has shown how classic tools employed in the DLS analysis of heterogeneous dynamics can be extended to XPCS, revealing additional information that conventional Kohlrausch exponential fitting obscures. The present work describes the software implementation of inverse transform analysis of XPCS data. This software, called CONTIN XPCS , is an extension of traditional CONTIN analysis and accommodates the various dynamics encountered in equilibrium XPCS measurements.

36 MATERIALS SCIENCE↗

Heteroepitaxial chemistry of zinc chalcogenides on InP nanocrystals for defect-free interfaces with atomic uniformity

Heteroepitaxy on colloidal semiconductor nanocrystals is an essential strategy for manipulating their optoelectronic functionalities. However, their practical synthesis typically leads to scattered and unexpected outcomes due to the intervention of multiple reaction pathways associated with complicated side products of reactants. Here, the heteroepitaxy mechanism of zinc chalcogenide initiated on indium phosphide (InP) colloidal nanocrystals is elucidated using the precursors, zinc carboxylate and trialkylphosphine selenide. The high magnetic receptivity of 77 Se and the characteristic longitudinal optical phonon mode of ZnSe allowed for monitoring the sequence of epilayer formation at the molecular level. The investigation revealed the sterically hindered acyloxytrialkylphosphonium and diacyloxytrialkylphosphorane to be main intermediates in the surface reaction, which retards the metal ion adsorption by a large steric hindrance. The transformation of adsorbates to the crystalline epilayer was disturbed by surface oxides. Raman scattering disclosed the pathway of secondary surface oxidation triggered by carboxylate ligands migrated from zinc carboxylate. The surface-initiated heteroepitaxy protocol is proposed to fabricate core/shell heterostructured nanocrystals with atomic-scale uniformity of epilayers. Despite the large lattice mismatch of ZnS to InP, we realised a uniform and interface defect-free ZnS epilayer (~0.3 nm thickness) on InP nanocrystals, as evidenced by a high photoluminescence quantum yield of 97.3%.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

RECOZ data reduction and analysis: Programs and procedures

The RECOZ data reduction programs transform data from the RECOZ photometer to ozone number density and overburden as a function of altitude. Required auxiliary data are the altitude profile versus time and for appropriate corrections to the ozone cross sections and scattering effects, air pressure and temperature profiles. Air temperature and density profiles may also be used to transform the ozone density versus geometric altitude to other units, such as to ozone partial pressure or mixing ratio versus pressure altitude. There are seven programs used to accomplish this: RADAR, LISTRAD, RAW OZONE, EDIT OZONE, MERGE, SMOOTH, and PROFILE.

Reed, E. I.↗

Precise relative locations for earthquakes in the northeast Pacific region

We report that double-difference methods applied to cross-correlation measured Rayleigh wave time shifts are an effective tool to improve epicentroid locations and relative origin time shifts in remote regions. We apply these methods to seismicity offshore of southwestern Canada and the U.S. Pacific Northwest, occurring along the boundaries of the Pacific and Juan de Fuca (including the Explorer Plate and Gorda Block) Plates. The Blanco, Mendocino, Revere-Dellwood, Nootka, and Sovanco fracture zones host the majority of this seismicity, largely consisting of strike-slip earthquakes. The Explorer, Juan de Fuca, and Gorda spreading ridges join these fracture zones and host normal faulting earthquakes. Our results show that at least the moderate-magnitude activity clusters along fault strike, supporting suggestions of large variations in seismic coupling along oceanic transform faults. Our improved relative locations corroborate earlier interpretations of the internal deformation in the Explorer and Gorda Plates. North of the Explorer Plate, improved locations support models that propose northern extension of the Revere-Dellwood fault. Relocations also support interpretations that favor multiple parallel active faults along the Blanco Transform Fault Zone. Seismicity of the western half of the Blanco appears more scattered and less collinear than the eastern half, possibly related to fault maturity. We use azimuthal variations in the Rayleigh wave cross-correlation amplitude to detect and model rupture directivity for a moderate size earthquake along the eastern Blanco Fault. Lastly, the observations constrain the seismogenic zone geometry and suggest a relatively narrow seismogenic zone width of 2 to 4 km.

58 GEOSCIENCES↗

PVDF-based backsheet cracking: Mapping in situ phase evolution by X-ray scattering

One of the most common polymers used in commercial photovoltaic backsheets is polyvinylidene fluoride (PVDF). However, recent reports have shown the potential for PVDF-based backsheets to crack and fail prematurely. Previous work has suggested that polymer phase changes play a role in the failure mechanism. Here, in situ wide-angle X-ray scattering maps are used to show that α- to β-phase transformations occur at crack tips in aged PVDF-based backsheets under stretching. Substantial β-phase formation is shown to be associated with strain hardening. In addition, our work demonstrates that β-phase formation is not required for crack growth and only occurs at crack tips when plastic deformation of the PVDF polymer has occurred. In conclusion, the anisotropy in the strength of aged PVDF-based backsheets is linked to the lack of β-phase formation when strain is applied to aged backsheets in the transverse direction.

14 SOLAR ENERGY↗

Statistical Hauser-Feshbach theory with width-fluctuation correction including direct reaction channels for neutron-induced reactions at low energies

Here, a model to calculate particle-induced reaction cross sections with statistical Hauser-Feshbach theory including direct reactions is given. The energy average of the scattering matrix from the coupled-channels optical model is diagonalized by the transformation proposed by Engelbrecht and Weidenmüller [C. A. Engelbrecht and H. A. Weidenmüller, Phys. Rev. C 8, 859 (1973)]. The ensemble average of S -matrix elements in the diagonalized channel space is approximated by a model of Moldauer [P. A. Moldauer, Phys. Rev. C 12, 744 (1975)] using the newly parametrized channel degree-of-freedom ν a to better describe the Gaussian orthogonal ensemble (GOE) reference calculations. The Moldauer approximation is confirmed by a Monte Carlo study using a randomly generated S matrix, as well as the GOE threefold integration formula. Lastly, the method proposed is applied to the 238U(n,n') cross-section calculation in the fast-energy range, showing an enhancement in the inelastic scattering cross sections.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Photometric redshifts for the S-PLUS Survey: Is machine learning up to the task?

The Southern Photometric Local Universe Survey (S-PLUS) is a novel project that aims to map the Southern Hemisphere using a twelve filter system, comprising five broad-band SDSS-like filters and seven narrow-band filters optimized for important stellar features in the local universe. In this paper we use the photometry and morphological information from the first S-PLUS data release (S-PLUS DR1) cross-matched to unWISE data and spectroscopic redshifts from Sloan Digital Sky Survey DR15. We explore three different machine learning methods (Gaussian Processes with GPz and two Deep Learning models made with TensorFlow) and compare them with the currently used template-fitting method in the S-PLUS DR1 to address whether machine learning methods can take advantage of the twelve filter system for photometric redshift prediction. Using tests for accuracy for both single-point estimates such as the calculation of the scatter, bias, and outlier fraction, and probability distribution functions (PDFs) such as the Probability Integral Transform (PIT), the Continuous Ranked Probability Score (CRPS) and the Odds distribution, we conclude that a deep-learning method using a combination of a Bayesian Neural Network and a Mixture Density Network offers the most accurate photometric redshifts for the current test sample. In conclusion, it achieves single-point photometric redshifts with scatter (σ NMAD ) of 0.023, normalized bias of -0.001, and outlier fraction of 0.64% for galaxies with r_auto magnitudes between 16 and 21.

79 ASTRONOMY AND ASTROPHYSICS↗

A flexible neutron spectrometer concept with a new ultra-high field steady-state vertical-bore magnet

The proposed facility explores materials under ultra-high magnetic fields. By combining the power of high fields to tune materials and of neutron scattering to probe the resulting changes down to the atomic scale, this facility will enable transformative progress in the study of quantum materials and is named for the “TITAN” subset of Greek gods to reflect this transformation. TITAN will offer DC magnetic fields up to at least 20 T. Exploiting the record brightness and bandwidth of the Second Target Station at the Spallation Neutron Source, TITAN will probe atomic-scale responses through high efficiency neutron spectroscopy up to 80 meV energy transfer, high resolution diffraction, and small angle neutron scattering. Focusing neutron optics will maximize flux on accurately positioned samples, while radial collimation and optimized shielding and detection strategies will minimize backgrounds.

47 OTHER INSTRUMENTATION↗

Measurement of the Fast Neutron Response for {sup 4}He Scintillation Detectors Using a Coincidence Scattering Method

Previous work has measured the neutron response of pressurized {sup 4}He scintillation detectors, however these studies only examine the response as a function of incident neutron energy. Since the detection mechanism in {sup 4}He detectors is elastic scattering, and the interacting neutron will only deposit a fraction of its incident kinetic energy in the detector gas, an examination of the response of the detector output to deposited energy is necessary to transform these detectors into instruments for neutron spectrometry. Using a combined time-of-flight (TOF) and coincidence scattering method, this paper further characterizes the {sup 4}He light response to fast neutrons by examining the scintillation light yield as a function of deposited energy, measuring the light response up to 5 MeV. These {sup 4}He detectors are simple in design, and are manufactured by Arktis Radiation Detectors in several sizes. The specific model used in this experiment had an active volume 20 cm long with an inner diameter of 4.4 cm, giving a total active volume of 304 cm{sup 3}. The key components include the active volume, filled with 150 bar of helium-4 gas, and photomultiplier tubes (PMTs) mounted at either end of the active volume. The detector body is made of stainless steel. The detector response was experimentally measured using a two-detector coincidence arrangement with a {sup 252}Cf source. Two {sup 4}He detectors were vertically mounted, and the source was placed at a horizontal distance from the center of the bottom detector, forming a right angle. By requiring coincidence between the two detectors, it was confirmed that each neutron interacting in the second (top) detector must first have undergone a scattering interaction in the first (bottom) detector, and the time-of-flight (TOF) technique could then be used to determine the energy of the neutron as it traveled between the two detectors by the difference in time between the two detector events. More importantly, with the scattering angle known, the amount of energy deposited by the neutron in the bottom detector (ER) was also calculated using kinematic scattering equations. This deposited recoil energy was then compared to the corresponding light output for each event to form a deposited energy scintillation light response matrix. Similarly, the system's insensitivity to gammas and its ability to reject gammas by pulse shape discrimination (PSD) are often cited as an important advantage, although a detailed analysis of these capabilities has not yet been performed. This work therefore quantified these parameters in order to further characterize these detectors for future mixed radiation field measurements. Gamma sources were measured spanning a range of gamma-ray energies from 0.122 MeV to 1.332 MeV, including {sup 57}Co, {sup 137}Cs, {sup 54}Mn, and {sup 60}Co. Each source was counted by the {sup 4}He detector and the background subtracted. Taking the ratio of the number of events detected during the experimental source measurement to the number of gammas predicted by MCNPX to pass through the detector volume yields the detector's intrinsic gamma efficiency. The difference between this fraction and unity is therefore a measure of the detector's ability to ignore interfering gamma rays, defined as its inherent gamma rejection rate. The ability of post-processing PSD algorithms to further reduce the number of gammas is also investigated and quantified. Finally, it has been noted that the scintillation signal from a single neutron event can be separated in time into two components: the fast component is a sharp peak that exists on the order of nanoseconds; the slow component is a series of smaller pulses, stretched out over four microseconds. Whereas previous research has exclusively focused on the energy information contained in the slow component, this work demonstrates that the fast component is also sensitive to neutron energy, and the entire scintillation signal can therefore be used. In conclusion, the relationship of fast neutron {sup 4}He scintillation detectors to deposited neutron energy was explored, and will be combined with previous works that measured the scintillation response to incident neutron energy in order to develop a neutron spectrometer. Similarly, the ability of these {sup 4}He detectors to reject interfering gamma rays was also quantified, and so will enable this spectrometer to be deployed in mixed radiation field measurements. Finally, while previous works with these detectors have focused on an analysis of the slow scintillation component, it was demonstrated in this work that the fast component also contains significant energy information.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Searching for an Enhanced Signal of the Onset of Color Transparency in Baryons with D(e,e′p)n Scattering

Observation of the onset of color transparency in baryons would provide a new means of studying the nuclear strong force and would be the first clear evidence of baryons transforming into a color-neutral point-like size in the nucleus as predicted by quantum chromodynamics. Recent C(e,e′p) results from electron-scattering did not observe the onset of color transparency (CT) in protons up to spacelike four-momentum transfers squared, Q2=14.2 GeV2. The traditional methods of searching for CT in (e,e′p) scattering use heavy targets favoring kinematics with already initially reduced final state interactions (FSIs) such that any CT effect that further reduces FSIs will be small. The reasoning behind this choice is the difficulty in accounting for all FSIs. D(e,e′p)n, on the other hand, has well-understood FSI contributions from double scattering with a known dependence on the kinematics and can show an increased sensitivity to hadrons in point-like configurations. Double scattering is the square of the re-scattering amplitude in which the knocked-out nucleon interacts with the spectator nucleon, a process that is suppressed in the presence of point-like configurations and is particularly well-studied for the deuteron. This suppression yields a quadratic sensitivity to CT effects and is strongly dependent on the choice of kinematics. Here, we describe a possible Jefferson National Accelerator Facility (JLab) electron-scattering experiment that utilizes these kinematics and explores the potential signal for the onset of CT with enhanced sensitivity as compared to recent experiments.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Optical modeling of plasma-deposited ZnO films: Electron scattering at different length scales

In this work, an optical modeling study on electron scattering mechanisms in plasma-deposited ZnO layers is presented. Because various applications of ZnO films pose a limit on the electron carrier density due to its effect on the film transmittance, higher electron mobility values are generally preferred instead. Hence, insights into the electron scattering contributions affecting the carrier mobility are required. In optical models, the Drude oscillator is adopted to represent the free-electron contribution and the obtained optical mobility can be then correlated with the macroscopic material properties. However, the influence of scattering phenomena on the optical mobility depends on the considered range of photon energy. For example, the grain-boundary scattering is generally not probed by means of optical measurements and the ionized-impurity scattering contribution decreases toward higher photon energies. To understand this frequency dependence and quantify contributions from different scattering phenomena to the mobility, several case studies were analyzed in this work by means of spectroscopic ellipsometry and Fourier transform infrared (IR) spectroscopy. The obtained electrical parameters were compared to the results inferred by Hall measurements. For intrinsic ZnO (i-ZnO), the in-grain mobility was obtained by fitting reflection data with a normal Drude model in the IR range. For Al-doped ZnO (Al:ZnO), besides a normal Drude fit in the IR range, an Extended Drude fit in the UV-vis range could be used to obtain the in-grain mobility. Scattering mechanisms for a thickness series of Al:ZnO films were discerned using the more intuitive parameter “scattering frequency” instead of the parameter “mobility”. The interaction distance concept was introduced to give a physical interpretation to the frequency dependence of the scattering frequency. This physical interpretation furthermore allows the prediction of which Drude models can be used in a specific frequency range.

36 MATERIALS SCIENCE↗

Modular Approach for the Synthesis of Bottlebrush Diblock Copolymers from Poly(Glycidyl Methacrylate)-block-Poly(Vinyldimethylazlactone) Backbones

A strategy that enables the facile synthesis of bottlebrush block copolymers with flexible backbones was developed. A demonstration of the strategy’s utility was carried out by grafting end-functionalized polymethylmethacrylate (PMMA) and polystyrene (PS) to the dually reactive block copolymer, poly(glycidyl methacrylate)-block-poly(vinyldimethylazlactone) (PGMA-b-PVDMA). Five different bottlebrush diblock copolymers were investigated by size-exclusion chromatography (SEC), 1H NMR, Fourier transform infrared (FT-IR), differential scanning calorimetry (DSC), X-ray scattering methods, atomic force microscopy (AFM), rheology and computational simulations using molecular dynamics (MD), and self-consistent field theory (SCFT). A relationship between the glass transition temperature and the fraction of chain ends was demonstrated by DSC and highlights the potential of this synthetic method to tailor polymer properties. All five samples were found to be in a disordered phase exhibiting multiscale structures revealed by two broad peaks in small-angle X-ray scattering (SAXS) that can be attributed to graft-to-graft and backbone-to-backbone density correlations using MD simulations. The SCFT-based simulations justify the observation of a disordered phase due to its stabilization by the grafts. Additionally, this modular approach can be easily extended to other grafts, including responsive, conducting, and charged polymers with the prerequisite end groups. The versatility and ease of assembling these functional bottlebrushes constitute a powerful “toolbox” method for the rapid and scalable synthesis of novel bottlebrush block copolymers with desired properties.

36 MATERIALS SCIENCE↗

Gallstone-Formation-Inspired Bimetallic Supra-nanostructures for Computed-Tomography-Image-Guided Radiation Therapy

Inspired by the gallstone formation mechanism, we report here a fast one-pot synthesis of high-surface-area bimetallic hierarchical supra-nanostructures. As gallstones are generated from metal cholate complexes, cholate bile acid molecules with Au/Ag metal precursors formed stable nanocomplexes aggregated with metal Au ions and preformed ~2 nm silver halide nanoparticles before reduction. When a reducing agent was added, the metal cholate nanocomplexes quickly formed noble bimetallic hierarchical supra-nanostructures. The morphology of bimetallic supra-nanostructures could be tailored by changing the feeding ratio of each metal precursor. In situ synchrotron small-angle X-ray scattering measurement with a custom-designed reaction cell showed two-step growth and attachment behavior toward hierarchical supra-nanostructures from the gallstone-formation-inspired metal cholate nanocomplexes in a 60 s reaction. Additional wide-angle X-ray scattering, X-ray absorption near-edge structure, in situ Fourier transform infrared, and high-resolution scanning transmission electron microscopy investigations subsequently revealed the mechanism for the evolution of bimetallic hierarchical supra-nanostructures. The gallstone-formation-inspired synthesis mechanism can be universally applied to other metals, for example, Pt–Ag and Pd–Ag bimetallic nanostructures. The synthesized high-surface-area bimetallic supra-nanostructures demonstrated significantly enhanced X-ray computed tomography imaging contrast and radiosensitizing effect for a potential image-guided nanomedicine application. We believe that our synthetic method inspired by gallstone formation and understanding represents an important step toward the development of hierarchical nanoparticles for various applications.

62 RADIOLOGY AND NUCLEAR MEDICINE↗