The Experts below are selected from a list of 1542 Experts worldwide ranked by ideXlab platform
Paul A Alivisatos - One of the best experts on this subject based on the ideXlab platform.
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elucidating the role of halides and iron during radiolysis driven oxidative etching of Gold Nanocrystals using liquid cell transmission electron microscopy and pulse radiolysis
Journal of the American Chemical Society, 2021Co-Authors: Michelle F Crook, Christian Laube, Ivan A Morenohernandez, Axel Kahnt, Stefan Zahn, Justin C Ondry, Aijia Liu, Paul A AlivisatosAbstract:Graphene liquid cell transmission electron microscopy (TEM) has enabled the observation of a variety of nanoscale transformations. Yet understanding the chemistry of the liquid cell solution and its impact on the observed transformations remains an important step toward translating insights from liquid cell TEM to benchtop chemistry. Gold Nanocrystal etching can be used as a model system to probe the reactivity of the solution. FeCl3 has been widely used to promote Gold oxidation in bulk and liquid cell TEM studies, but the roles of the halide and iron species have not been fully elucidated. In this work, we observed the etching trajectories of Gold Nanocrystals in different iron halide solutions. We observed an increase in Gold Nanocrystal etch rate going from Cl-- to Br-- to I--containing solutions. This is consistent with a mechanism in which the dominant role of halides is as complexation agents for oxidized Gold species. Additionally, the mechanism through which FeCl3 induces etching in liquid cell TEM remains unclear. Ground-state bleaching of the Fe(III) absorption band observed through pulse radiolysis indicates that iron may react with Cl2·- radicals to form an oxidized transient species under irradiation. Complete active space self-consistent field (CASSCF) calculations indicate that the FeCl3 complex is oxidized to an Fe species with an OH radical ligand. Together our data indicate that an oxidized Fe species may be the active oxidant, while halides modulate the etch rate by tuning the reduction potential of Gold Nanocrystals.
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Gold Nanocrystal etching as a means of probing the dynamic chemical environment in graphene liquid cell electron microscopy
Journal of the American Chemical Society, 2019Co-Authors: Matthew R Hauwiller, Justin C Ondry, Cindy M. Chan, Prachi Khandekar, Paul A AlivisatosAbstract:Graphene liquid cell electron microscopy has the necessary temporal and spatial resolution to enable the in situ observation of nanoscale dynamics in solution. However, the chemistry of the solution in the liquid cell during imaging is as yet poorly understood due to the generation of a complex mixture of radiolysis products by the electron beam. In this work, the etching trajectories of Nanocrystals were used as a probe to determine the effect of the electron beam dose rate and preloaded etchant, FeCl3, on the chemistry of the liquid cell. Initially, illuminating the sample at a low electron beam dose rate generates hydrogen bubbles, providing a reservoir of sacrificial reductant. Increasing the electron beam dose rate leads to a constant etching rate that varies linearly with the electron beam dose rate. Comparing these results with the oxidation potentials of the species in solution, the electron beam likely controls the total concentration of oxidative species in solution and FeCl3 likely controls the relative ratio of oxidative species, independently determining the etching rate and chemical potential of the reaction, respectively. Correlating these liquid cell etching results with the ex situ oxidative etching of Gold Nanocrystals using FeCl3 provides further insight into the liquid cell chemistry while corroborating the liquid cell dynamics with ex situ synthetic behavior. This understanding of the chemistry in the liquid cell will allow researchers to better control the liquid cell electron microscopy environment, allowing new nanoscale materials science experiments to be conducted systematically in a reproducible manner.
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Gold Nanocrystal Etching as a Means of Probing the Dynamic Chemical Environment in Graphene Liquid Cell Electron Microscopy
2019Co-Authors: Matthew R. Hauwiller, Justin C Ondry, Cindy M. Chan, Prachi Khandekar, Paul A AlivisatosAbstract:Graphene liquid cell electron microscopy has the necessary temporal and spatial resolution to enable the in situ observation of nanoscale dynamics in solution. However, the chemistry of the solution in the liquid cell during imaging is as yet poorly understood due to the generation of a complex mixture of radiolysis products by the electron beam. In this work, the etching trajectories of Nanocrystals were used as a probe to determine the effect of the electron beam dose rate and preloaded etchant, FeCl3, on the chemistry of the liquid cell. Initially, illuminating the sample at a low electron beam dose rate generates hydrogen bubbles, providing a reservoir of sacrificial reductant. Increasing the electron beam dose rate leads to a constant etching rate that varies linearly with the electron beam dose rate. Comparing these results with the oxidation potentials of the species in solution, the electron beam likely controls the total concentration of oxidative species in solution and FeCl3 likely controls the relative ratio of oxidative species, independently determining the etching rate and chemical potential of the reaction, respectively. Correlating these liquid cell etching results with the ex situ oxidative etching of Gold Nanocrystals using FeCl3 provides further insight into the liquid cell chemistry while corroborating the liquid cell dynamics with ex situ synthetic behavior. This understanding of the chemistry in the liquid cell will allow researchers to better control the liquid cell electron microscopy environment, allowing new nanoscale materials science experiments to be conducted systematically in a reproducible manner
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unraveling kinetically driven mechanisms of Gold Nanocrystal shape transformations using graphene liquid cell electron microscopy
Nano Letters, 2018Co-Authors: Matthew R Hauwiller, Justin C Ondry, Layne B Frechette, Matthew R Jones, Grant M Rotskoff, Phillip L Geissler, Paul A AlivisatosAbstract:Mechanisms of kinetically driven Nanocrystal shape transformations were elucidated by monitoring single particle etching of Gold Nanocrystals using in situ graphene liquid cell transmission electron microscopy (TEM). By systematically changing the chemical potential of the oxidative etching and then quantifying the facets of the Nanocrystals, nonequilibrium processes of atom removal could be deduced. Etching at sufficiently high oxidation potentials, both cube and rhombic dodecahedra (RDD)-shaped Gold Nanocrystals transform into kinetically stable tetrahexahedra (THH)-shaped particles. Whereas {100}-faceted cubes adopt an { hk0}-faceted THH intermediate where h/ k depends on chemical potential, {110}-faceted RDD adopt a {210}-faceted THH intermediate regardless of driving force. For cube reactions, Monte Carlo simulations show that removing 6-coordinate edge atoms immediately reveals 7-coordinate interior atoms. The rate at which these 6- and 7-coordinate atoms are etched is sensitive to the chemical potential, resulting in different THH facet structures with varying driving force. Conversely, when RDD are etched to THH, removal of 6-coordinate edge atoms reveals 6-coordinate interior atoms. Thus, changing the driving force for oxidation does not change the probability of edge atom versus interior atom removal, leading to a negligible effect on the kinetically stabilized intermediate shape. These fundamental insights, facilitated by single-particle liquid-phase TEM imaging, provide important atomic-scale mechanistic details regarding the role of kinetics and chemical driving force in dictating shape transformations at the nanometer length scale.
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Unraveling Kinetically-Driven Mechanisms of Gold Nanocrystal Shape Transformations Using Graphene Liquid Cell Electron Microscopy
2018Co-Authors: Matthew R Hauwiller, Justin C Ondry, Layne B Frechette, Matthew R Jones, Grant M Rotskoff, Phillip Geissler, Paul A AlivisatosAbstract:Mechanisms of kinetically driven Nanocrystal shape transformations were elucidated by monitoring single particle etching of Gold Nanocrystals using in situ graphene liquid cell transmission electron microscopy (TEM). By systematically changing the chemical potential of the oxidative etching and then quantifying the facets of the Nanocrystals, nonequilibrium processes of atom removal could be deduced. Etching at sufficiently high oxidation potentials, both cube and rhombic dodecahedra (RDD)-shaped Gold Nanocrystals transform into kinetically stable tetrahexahedra (THH)-shaped particles. Whereas {100}-faceted cubes adopt an {hk0}-faceted THH intermediate where h/k depends on chemical potential, {110}-faceted RDD adopt a {210}-faceted THH intermediate regardless of driving force. For cube reactions, Monte Carlo simulations show that removing 6-coordinate edge atoms immediately reveals 7-coordinate interior atoms. The rate at which these 6- and 7-coordinate atoms are etched is sensitive to the chemical potential, resulting in different THH facet structures with varying driving force. Conversely, when RDD are etched to THH, removal of 6-coordinate edge atoms reveals 6-coordinate interior atoms. Thus, changing the driving force for oxidation does not change the probability of edge atom versus interior atom removal, leading to a negligible effect on the kinetically stabilized intermediate shape. These fundamental insights, facilitated by single-particle liquid-phase TEM imaging, provide important atomic-scale mechanistic details regarding the role of kinetics and chemical driving force in dictating shape transformations at the nanometer length scale
S O Hruszkewycz - One of the best experts on this subject based on the ideXlab platform.
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three dimensional variable wavelength x ray bragg coherent diffraction imaging
Physical Review Letters, 2016Co-Authors: Andrew Ulvestad, Marc Allain, Virginie Chamard, Ross Harder, Steven J Leake, Jorg Maser, P H Fuoss, S O HruszkewyczAbstract:We present and demonstrate a formalism by which three dimensional (3D) Bragg x-ray coherent diffraction imaging (BCDI) can be implemented without moving the sample by scanning the energy of the incident x-ray beam. This capability is made possible by introducing a 3D Fourier transform that accounts for x-ray wavelength variability. We demonstrate the approach by inverting coherent Bragg diffraction patterns from a Gold Nanocrystal measured with an x-ray energy scan. Variable-wavelength BCDI will expand the breadth of feasible in situ 3D strain imaging experiments towards more diverse materials environments, especially where sample manipulation is difficult.
Yuji C. Sasaki - One of the best experts on this subject based on the ideXlab platform.
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x ray observation of novel nucleation factor in protein supersaturated solution
Biophysical Journal, 2016Co-Authors: Yufuku Matsushita, Hiroshi Sekiguchi, Noboru Ohta, Keigo Ikezaki, Yuji Goto, Yuji C. SasakiAbstract:Recently, Protein solution and the micro scale structure are receiving a lot of attention in diverse protein study. Protein crystal observation In particular, protein aggregation process is a typical micro scale phenomenon of protein solution. Moreover, it is a one of the unclear mechanism of protein characteristics.In this study, we approached to observe the time resolved micro scale dynamics of protein solution by Diffracted X-ray Tracking (DXT) as known as single molecule measurement method. This method is able to direct observation of local solution dynamics for Target solution by detecting angular rotational displacement of a coexisted and dispersed single Gold Nanocrystal (approximately 100 nm) with pico-meter scale positional accuracy and micro-second time resolution. For target sample, we choose a crystal precursor metastable state of lysozyme solution.From detailed DXT analysis, we observed as crystal precursor state solution of lysozyme are containing slow and fast dynamics and the fast diffusion corresponded relaxation process of metastable state of nano scale clusters which is a important factor of maintenance of metastable supersaturated condition, driving force of morphology determination of final product from crystallization and nucleation process from supersaturation. From this study, DXT measurement results and detailed analysis process for a protein solution such as crystal precursor metastable state of lysozyme solution are concerned that this technique is a powerful tool for observing nano-scale protein structures and its local dynamics in bulk solution. For next work, we will planning to tackle research in order to observe morphology control factor discovery inhibitation techniques of supersaturated condition, and approaching for elucidation of protein abnormal aggregation process.
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cooperative motion of a multi subunit protein visualized by x ray single molecule tracking
Biophysical Journal, 2013Co-Authors: Hiroshi Sekiguchi, Kouhei Ichiyanagi, Naoto Yagi, Yohei Yamamoto, Ayumi Nakagawa, Kazuki Moriya, Mayuno Arita, Masafumi Yohda, Yuji C. SasakiAbstract:Most of proteins or enzymes are multimeric proteins, such as dimer, trimer, or higher-order structures (Goodsell et al. Annu Rev Biophys Biomol Struct, 2000). Usually, these proteins have multiple biding sites for ligands, such as ATP, peptide and others, that induce protein's conformational change. The function of the protein is regulated by such conformational changes that may give rise to cooperativity. Therefore, assessment of the cooperativity between subunits of proteins is important to understand the function of complex proteins.We have previously reported that the diffracted X-ray tracking (DXT) method could trace ATP-induced twisting motion of group II chaperonin ring at a single molecule level with high accuracy. In DXT, a Gold Nanocrystal immobilized on one side of chaperonin-ring is used as tracer for structural change of chaperonin. Our analyses clearly showed that the chaperonin ring partially closed within 1 s of ATP binding, the closed ring subsequently twisted counterclockwise within 2-6 s, as viewed from the top to bottom of the chaperonin, and the twisted ring reverted to the original open-state with a clockwise motion. In this study, we checked how ATPase deficient mutant subunits modulate the speed or frequency of twisting motion. We controlled the number of ATPase deficient mutant within one chaperonin ring, constructed the ATP deficient hetero-ring using circular permutated connected mutants, and evaluated the effects of those mutants to chaperonin-ring's twisting motion. We found that the equivalent twisting motion was observed in hetero-ring chaperonin and inter-ring communication is dispensable for the function of group II chaperonin3.
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Atto-Newton X-Ray Radiation Pressure Force on Gold Nanocrystal in Aqueous Solution
Biophysical Journal, 2012Co-Authors: Kentaro Hoshisashi, Hiroshi Sekiguchi, Kouhei Ichiyanagi, Yasuhito Suzuki, Naoto Yagi, Tatsuhito Matsuo, Noboru Oota, Yuji C. SasakiAbstract:In micro-sized force field, radiation pressure forces acting on an object surface have been widely applied as a tool for laser trapping and cooling of the visible light. In the region of short-wavelength, we confirmed the existence of atto-Newton (aN) level's radiation pressure force measured by using Diffracted X-ray Tracking (DXT) which is tracing the X-ray diffraction spots from the Gold Nanocrystal was labeled on the protein molecule at single molecular level [1].In this study, we succeeded in measuring the modified dynamic rotational Brownian behaviors of the Gold Nanocrystal in an aqueous solution at micro-sec. levels by varying the wavelength and flux of the incident X-ray probe. As a result, we observed a clear energy-dependent radiation pressure in the X-ray axial direction (2 theta) by comparing with a concentric circle direction (chi: no-pressure direction). And the observed pressures were able to be estimated from the X-ray wavelengths and flux. Furthermore, we found the presence of the resultant forces of X-ray radiation pressure on several diffracted crystal planes from analyzing the angular distributions of accelerated motions. This phenomenon expects to open a new application of X-ray science.For example, we can utilize this X-ray resultant force for the trapping of nano-probe and the crystal growth azimuth control during crystal growths. In addition, we proved that the ultra-fast DXT using protein molecules labeled the Gold Nanocrystal [2] can detect aN level's force field in functional protein molecules. In the future, we can detect dynamic structural changes of functional surface induced by an ultra-small force field that cannot be detected by STM and AFM.[1] Y. C. Sasaki et al., Appl. Phys. Lett., 89, 053121(2006).[2] H. Shimizu et al., Cell, 132, 67–78 (2008).
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Global Twisting Motion of Single Molecular KcsA Potassium Channel upon Gating
Cell, 2008Co-Authors: Hirofumi Shimizu, Yuji C. Sasaki, Masayuki Iwamoto, Takashi Konno, Amiko Nihei, Shigetoshi OikiAbstract:Ion channels are signal transduction molecules that switch ion permeation pathways on and off (gating). Crystal structures of several kinds of potassium channels have revealed open and closed conformations, which provide static pictures of gating status. Here we studied KcsA potassium channels undergoing conformational changes at the single-molecule level. A KcsA channel with a Gold Nanocrystal attached was irradiated by white X-rays and motions of the diffraction spot from the Nanocrystal were tracked in real time. Upon gating, the KcsA channels twisted around the axis of the pore. These conformational changes were prevented by an open-channel blocker, tetrabuthylammonium. Random clockwise and counterclockwise twisting in the range of several tens of degrees originated in the transmembrane domain and was transmitted to the cytoplasmic domain. This coupling suggests a mechanical interplay between the transmembrane and cytoplasmic domains.
Paul Mulvaney - One of the best experts on this subject based on the ideXlab platform.
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Electrochemical charging of single Gold nanorods
Journal of the American Chemical Society, 2009Co-Authors: Carolina Novo, Ann K. Gooding, Alison M Funston, Paul MulvaneyAbstract:Metal Nanocrystals are commonly used to mediate important chemical reactions such as water splitting and CO oxidation. To investigate such redox reactions in detail, it would be useful to be able to carry out electrochemistry on single metal Nanocrystals. We report here that the surface plasmon resonance of a single Gold Nanocrystal can be reversibly and rapidly tuned by tens of nanometers electrochemically. The spectral shifts are more sensitive for elongated morphologies such as rods and lead to color changes perceptible by eye.
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direct observation of chemical reactions on single Gold Nanocrystals using surface plasmon spectroscopy
Nature Nanotechnology, 2008Co-Authors: Carolina Novo, Alison M Funston, Paul MulvaneyAbstract:Heterogeneous catalysts have been pivotal to the development of the modern chemical industry and are essential for catalysing many industrial reactions. However, reaction rates are different for every individual catalyst particle and depend upon each particle's morphology and size, crystal structure and composition. Measuring the rates of reaction on single Nanocrystals will enable the role of catalyst structure to be quantified. Here, using surface plasmon spectroscopy, we have directly observed the kinetics of atomic deposition onto a single Gold Nanocrystal and also monitored electron injection and extraction during a redox reaction involving the oxidation of ascorbic acid on a Gold Nanocrystal surface. These results constitute the first direct measurement of the rates of redox catalysis on single Nanocrystals.
Justin C Ondry - One of the best experts on this subject based on the ideXlab platform.
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elucidating the role of halides and iron during radiolysis driven oxidative etching of Gold Nanocrystals using liquid cell transmission electron microscopy and pulse radiolysis
Journal of the American Chemical Society, 2021Co-Authors: Michelle F Crook, Christian Laube, Ivan A Morenohernandez, Axel Kahnt, Stefan Zahn, Justin C Ondry, Aijia Liu, Paul A AlivisatosAbstract:Graphene liquid cell transmission electron microscopy (TEM) has enabled the observation of a variety of nanoscale transformations. Yet understanding the chemistry of the liquid cell solution and its impact on the observed transformations remains an important step toward translating insights from liquid cell TEM to benchtop chemistry. Gold Nanocrystal etching can be used as a model system to probe the reactivity of the solution. FeCl3 has been widely used to promote Gold oxidation in bulk and liquid cell TEM studies, but the roles of the halide and iron species have not been fully elucidated. In this work, we observed the etching trajectories of Gold Nanocrystals in different iron halide solutions. We observed an increase in Gold Nanocrystal etch rate going from Cl-- to Br-- to I--containing solutions. This is consistent with a mechanism in which the dominant role of halides is as complexation agents for oxidized Gold species. Additionally, the mechanism through which FeCl3 induces etching in liquid cell TEM remains unclear. Ground-state bleaching of the Fe(III) absorption band observed through pulse radiolysis indicates that iron may react with Cl2·- radicals to form an oxidized transient species under irradiation. Complete active space self-consistent field (CASSCF) calculations indicate that the FeCl3 complex is oxidized to an Fe species with an OH radical ligand. Together our data indicate that an oxidized Fe species may be the active oxidant, while halides modulate the etch rate by tuning the reduction potential of Gold Nanocrystals.
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Gold Nanocrystal etching as a means of probing the dynamic chemical environment in graphene liquid cell electron microscopy
Journal of the American Chemical Society, 2019Co-Authors: Matthew R Hauwiller, Justin C Ondry, Cindy M. Chan, Prachi Khandekar, Paul A AlivisatosAbstract:Graphene liquid cell electron microscopy has the necessary temporal and spatial resolution to enable the in situ observation of nanoscale dynamics in solution. However, the chemistry of the solution in the liquid cell during imaging is as yet poorly understood due to the generation of a complex mixture of radiolysis products by the electron beam. In this work, the etching trajectories of Nanocrystals were used as a probe to determine the effect of the electron beam dose rate and preloaded etchant, FeCl3, on the chemistry of the liquid cell. Initially, illuminating the sample at a low electron beam dose rate generates hydrogen bubbles, providing a reservoir of sacrificial reductant. Increasing the electron beam dose rate leads to a constant etching rate that varies linearly with the electron beam dose rate. Comparing these results with the oxidation potentials of the species in solution, the electron beam likely controls the total concentration of oxidative species in solution and FeCl3 likely controls the relative ratio of oxidative species, independently determining the etching rate and chemical potential of the reaction, respectively. Correlating these liquid cell etching results with the ex situ oxidative etching of Gold Nanocrystals using FeCl3 provides further insight into the liquid cell chemistry while corroborating the liquid cell dynamics with ex situ synthetic behavior. This understanding of the chemistry in the liquid cell will allow researchers to better control the liquid cell electron microscopy environment, allowing new nanoscale materials science experiments to be conducted systematically in a reproducible manner.
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Gold Nanocrystal Etching as a Means of Probing the Dynamic Chemical Environment in Graphene Liquid Cell Electron Microscopy
2019Co-Authors: Matthew R. Hauwiller, Justin C Ondry, Cindy M. Chan, Prachi Khandekar, Paul A AlivisatosAbstract:Graphene liquid cell electron microscopy has the necessary temporal and spatial resolution to enable the in situ observation of nanoscale dynamics in solution. However, the chemistry of the solution in the liquid cell during imaging is as yet poorly understood due to the generation of a complex mixture of radiolysis products by the electron beam. In this work, the etching trajectories of Nanocrystals were used as a probe to determine the effect of the electron beam dose rate and preloaded etchant, FeCl3, on the chemistry of the liquid cell. Initially, illuminating the sample at a low electron beam dose rate generates hydrogen bubbles, providing a reservoir of sacrificial reductant. Increasing the electron beam dose rate leads to a constant etching rate that varies linearly with the electron beam dose rate. Comparing these results with the oxidation potentials of the species in solution, the electron beam likely controls the total concentration of oxidative species in solution and FeCl3 likely controls the relative ratio of oxidative species, independently determining the etching rate and chemical potential of the reaction, respectively. Correlating these liquid cell etching results with the ex situ oxidative etching of Gold Nanocrystals using FeCl3 provides further insight into the liquid cell chemistry while corroborating the liquid cell dynamics with ex situ synthetic behavior. This understanding of the chemistry in the liquid cell will allow researchers to better control the liquid cell electron microscopy environment, allowing new nanoscale materials science experiments to be conducted systematically in a reproducible manner
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unraveling kinetically driven mechanisms of Gold Nanocrystal shape transformations using graphene liquid cell electron microscopy
Nano Letters, 2018Co-Authors: Matthew R Hauwiller, Justin C Ondry, Layne B Frechette, Matthew R Jones, Grant M Rotskoff, Phillip L Geissler, Paul A AlivisatosAbstract:Mechanisms of kinetically driven Nanocrystal shape transformations were elucidated by monitoring single particle etching of Gold Nanocrystals using in situ graphene liquid cell transmission electron microscopy (TEM). By systematically changing the chemical potential of the oxidative etching and then quantifying the facets of the Nanocrystals, nonequilibrium processes of atom removal could be deduced. Etching at sufficiently high oxidation potentials, both cube and rhombic dodecahedra (RDD)-shaped Gold Nanocrystals transform into kinetically stable tetrahexahedra (THH)-shaped particles. Whereas {100}-faceted cubes adopt an { hk0}-faceted THH intermediate where h/ k depends on chemical potential, {110}-faceted RDD adopt a {210}-faceted THH intermediate regardless of driving force. For cube reactions, Monte Carlo simulations show that removing 6-coordinate edge atoms immediately reveals 7-coordinate interior atoms. The rate at which these 6- and 7-coordinate atoms are etched is sensitive to the chemical potential, resulting in different THH facet structures with varying driving force. Conversely, when RDD are etched to THH, removal of 6-coordinate edge atoms reveals 6-coordinate interior atoms. Thus, changing the driving force for oxidation does not change the probability of edge atom versus interior atom removal, leading to a negligible effect on the kinetically stabilized intermediate shape. These fundamental insights, facilitated by single-particle liquid-phase TEM imaging, provide important atomic-scale mechanistic details regarding the role of kinetics and chemical driving force in dictating shape transformations at the nanometer length scale.
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Unraveling Kinetically-Driven Mechanisms of Gold Nanocrystal Shape Transformations Using Graphene Liquid Cell Electron Microscopy
2018Co-Authors: Matthew R Hauwiller, Justin C Ondry, Layne B Frechette, Matthew R Jones, Grant M Rotskoff, Phillip Geissler, Paul A AlivisatosAbstract:Mechanisms of kinetically driven Nanocrystal shape transformations were elucidated by monitoring single particle etching of Gold Nanocrystals using in situ graphene liquid cell transmission electron microscopy (TEM). By systematically changing the chemical potential of the oxidative etching and then quantifying the facets of the Nanocrystals, nonequilibrium processes of atom removal could be deduced. Etching at sufficiently high oxidation potentials, both cube and rhombic dodecahedra (RDD)-shaped Gold Nanocrystals transform into kinetically stable tetrahexahedra (THH)-shaped particles. Whereas {100}-faceted cubes adopt an {hk0}-faceted THH intermediate where h/k depends on chemical potential, {110}-faceted RDD adopt a {210}-faceted THH intermediate regardless of driving force. For cube reactions, Monte Carlo simulations show that removing 6-coordinate edge atoms immediately reveals 7-coordinate interior atoms. The rate at which these 6- and 7-coordinate atoms are etched is sensitive to the chemical potential, resulting in different THH facet structures with varying driving force. Conversely, when RDD are etched to THH, removal of 6-coordinate edge atoms reveals 6-coordinate interior atoms. Thus, changing the driving force for oxidation does not change the probability of edge atom versus interior atom removal, leading to a negligible effect on the kinetically stabilized intermediate shape. These fundamental insights, facilitated by single-particle liquid-phase TEM imaging, provide important atomic-scale mechanistic details regarding the role of kinetics and chemical driving force in dictating shape transformations at the nanometer length scale