Unhindered Brownian Motion of Individual Nanoparticles in Liquid-Phase Scanning Transmission Electron Microscopy

Yesibolati, Murat Nulati; Mortensen, Kim I.; Sun, Hongyu; Brostrøm, Anders; Tidemand-Lichtenberg, Sofie; Mølhave, Kristian

doi:10.1021/acs.nanolett.0c02352

Cited by 46 publications

(49 citation statements)

References 57 publications

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“…Rapid dynamic control over liquid thickness is of key importance, in particular in bypass liquid cell systems, as it can help to overcome confinement problems such as diffusion limitations [ 17 ] or hindered Brownian motion. [ 41 ]…”

Section: Resultsmentioning

confidence: 99%

Mapping and Controlling Liquid Layer Thickness in Liquid‐Phase (Scanning) Transmission Electron Microscopy

Joosten

et al. 2021

Small Methods

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Liquid‐Phase (Scanning) Transmission Electron Microscopy (LP‐(S)TEM) has become an essential technique to monitor nanoscale materials processes in liquids in real‐time. Due to the pressure difference between the liquid and the microscope vacuum, bending of the silicon nitride (SiNx) membrane windows generally occurs. This causes a spatially varying liquid layer thickness that makes interpretation of LP‐(S)TEM results difficult due to a locally varying achievable resolution and diffusion limitations. To mediate these difficulties, it is shown: 1) how to quantitatively map liquid layer thickness for any liquid at less than 0.01 e− Å−2 total dose; 2) how to dynamically modulate the liquid thickness by tuning the internal pressure in the liquid cell, co‐determined by the Laplace pressure and the external pressure. It is demonstrated that reproducible inward bulging of the window membranes can be realized, leading to an ultra‐thin liquid layer in the central window area for high‐resolution imaging. Furthermore, it is shown that the liquid thickness can be dynamically altered in a programmed way, thereby potentially overcoming the diffusion limitations towards achieving bulk solution conditions. The presented approaches provide essential ways to measure and dynamically adjust liquid thickness in LP‐(S)TEM experiments, enabling new experiment designs and better control of solution chemistry.

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Section: Resultsmentioning

confidence: 99%

Mapping and Controlling Liquid Layer Thickness in Liquid‐Phase (Scanning) Transmission Electron Microscopy

Joosten

et al. 2021

Small Methods

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“…It further shows that the high Z contrast of the HAADF detector can be used to image across thick layers of low-Z materials such as water. It is worth noting that the pressure difference of one atmosphere between the inside of the liquid cell and the vacuum of the TEM column leads to significant bulging of the SiN x windows [129]. Thus the cell can be 2 to 3 µm thicker in its center.…”

Section: Liquid Cellsmentioning

confidence: 99%

“…Although core-loss EELS measurements remain challenging within micrometer-thick liquid layers, low-loss EELS [134,144] and electron dispersive X-ray spectroscopy (EDS) [145] have seen promising proofs of concept. The former is effective in probing changes of the electronic structure of catalysts and important to calculate effective thicknesses through the t/λ method [129,133,146]. EDS on the other hand allows for the simultaneous mapping of multiple elements at the nanoscale in liquids.…”

Section: Liquid Cells-applicationsmentioning

confidence: 99%

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Quo Vadis Micro-Electro-Mechanical Systems for the Study of Heterogeneous Catalysts Inside the Electron Microscope?

et al. 2020

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During the last decade, modern micro-electro-mechanical systems (MEMS) technology has been used to create cells that can act as catalytic nanoreactors and fit into the sample holders of transmission electron microscopes. These nanoreactors can maintain atmospheric or higher pressures inside the cells as they seal gases or liquids from the vacuum of the TEM column and can reach temperatures exceeding 1000 °C. This has led to a paradigm shift in electron microscopy, which facilitates the local characterization of structural and morphological changes of solid catalysts under working conditions. In this review, we outline the development of state-of-the-art nanoreactor setups that are commercially available and are currently applied to study catalytic reactions in situ or operando in gaseous or liquid environments. We also discuss challenges that are associated with the use of environmental cells. In catalysis studies, one of the major challenge is the interpretation of the results while considering the discrepancies in kinetics between MEMS based gas cells and fixed bed reactors, the interactions of the electron beam with the sample, as well as support effects. Finally, we critically analyze the general role of MEMS based nanoreactors in electron microscopy and catalysis communities and present possible future directions.

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“…This understanding of how the electron beam can a ect the local environment near the membrane, which in turn governs the di usive motion of nanoparticles near the surface, can be used in applications of nanoparticles in LCTEM as nanoscale probes to study the local material properties of the fluid near the surface. Similar analysis can also be performed on undamped motion of nanoparticles in bulk in LCTEM, (41,42) to investigate the e ect of electron beam on the bulk material properties. Furthermore, the change in the local material properties of the fluid next to the surface in presence of the electron beam may play a role in other LCTEM studies such as in situ growth of nanocrystals (43)(44)(45).…”

Section: Nanoscopic Interpretationmentioning

confidence: 99%

Anomalous Nanoparticle Surface Diffusion in Liquid Cell TEM is Revealed by Deep Learning-Assisted Analysis

Jamali¹,

Hargus²,

Ben-Moshe³

et al. 2020

Preprint

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The motion of nanoparticles near surfaces is of fundamental importance in physics, biology, and chemistry. Liquid cell transmission electron microscopy (LCTEM) is a promising technique for studying motion of nanoparticles with high spatial resolution. Yet, the lack of understanding of how the electron beam of the microscope affects the particle motion has held back advancement in using LCTEM for in situ single nanoparticle and macromolecule tracking at interfaces. Here, we experimentally studied the motion of a model system of gold nanoparticles dispersed in water and moving adjacent to the silicon nitride membrane of a commercial liquid cell in a broad range of electron beam dose rates. We find that the nanoparticles exhibit anomalous diffusive behavior modulated by the electron beam dose rate. We characterized the anomalous diffusion of nanoparticles in LCTEM using a convolutional deep neural network model and canonical statistical tests. The results demonstrate that the nanoparticle motion is governed by fractional Brownian motion at low dose rates, resembling diffusion in a viscoelastic medium, and continuous time random walk at high dose rates, resembling diffusion on an energy landscape with pinning sites. Both behaviors can be explained by the presence of silanol molecular species on the surface of the silicon nitride membrane and the ionic species in solution formed by radiolysis of water in presence of the electron beam.

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Unhindered Brownian Motion of Individual Nanoparticles in Liquid-Phase Scanning Transmission Electron Microscopy

Cited by 46 publications

References 57 publications

Mapping and Controlling Liquid Layer Thickness in Liquid‐Phase (Scanning) Transmission Electron Microscopy

Mapping and Controlling Liquid Layer Thickness in Liquid‐Phase (Scanning) Transmission Electron Microscopy

Quo Vadis Micro-Electro-Mechanical Systems for the Study of Heterogeneous Catalysts Inside the Electron Microscope?

Anomalous Nanoparticle Surface Diffusion in Liquid Cell TEM is Revealed by Deep Learning-Assisted Analysis

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