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

Author(s):  
Vida Jamali ◽  
Cory Hargus ◽  
Assaf Ben Moshe ◽  
Amirali Aghazadeh ◽  
Hyun Dong Ha ◽  
...  

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.

2020 ◽  
Author(s):  
Vida Jamali ◽  
Cory Hargus ◽  
Assaf Ben Moshe ◽  
Amirali Aghazadeh ◽  
Hyun Dong Ha ◽  
...  

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.


2020 ◽  
Author(s):  
Vida Jamali ◽  
Cory Hargus ◽  
Assaf Ben Moshe ◽  
Amirali Aghazadeh ◽  
Hyun Dong Ha ◽  
...  

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.


2021 ◽  
Vol 118 (10) ◽  
pp. e2017616118
Author(s):  
Vida Jamali ◽  
Cory Hargus ◽  
Assaf Ben-Moshe ◽  
Amirali Aghazadeh ◽  
Hyun Dong Ha ◽  
...  

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 LC 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.


2014 ◽  
Vol 12 (7) ◽  
pp. 774-781 ◽  
Author(s):  
Ioan Călinescu ◽  
Diana Martin ◽  
Daniel Ighigeanu ◽  
Adina Gavrila ◽  
Adrian Trifan ◽  
...  

AbstractElectron beam (EB) irradiation is a useful method to generate stable silver nanoparticles without the interference of inherent impurities generated from chemical reactions. Our experiments were carried out using linear electron beam accelerators with two different EB absorbed dose rates: 2 kGy min−1 and 7–8 kGy s−1, and with different absorbed dose levels. The optimum conditions for silver nanoparticles (AgNPs) generation by radiolysis, or by radiolysis combined with chemical reduction, were established. In order to obtain a good yield for AgNPs synthesized by radiolysis, a high dose rate is required, resulting in a rapid production process. At low absorbed dose rates, the utilization of a stabilization agent is advisable. By modifying the experimental conditions, the ratio between the chemical and radiolytic reduction process can be adjusted, thus it is possible to obtain nanoparticles with tailored characteristics, depending on the desired application.


1993 ◽  
Vol 311 ◽  
Author(s):  
J. Liu ◽  
C. J. Barbero ◽  
J. W. Corbett ◽  
K. Rajan ◽  
H. Leary

ABSTRACTAn in situ study of electron beam irradiation induced amorphous–to–crystalline transformation of Al2O3 films on silicon substrates has been carried out using transmission electron microscopy. Trigonal α–Al2O3 crystallites can be observed for electron beam dose rates larger than 10 mA/cm2. It is found that the nucleation and growth processes dominate near the Al2O3–Si interface. The possible effect of the silicon substrate on the growth of Al2O3 crystallites is considered.


CrystEngComm ◽  
2021 ◽  
Vol 23 (16) ◽  
pp. 3002-3005
Author(s):  
Junyu Zhang ◽  
Peng Zhao

In this work, we used liquid cell TEM to observe the motion and transformation pathways of Pt3Ni nanoparticles in solution by systematically changing the electron beam dose rate.


1970 ◽  
Vol 48 (22) ◽  
pp. 3463-3472 ◽  
Author(s):  
Clive Willis ◽  
P. E. Bindner

Ozone yields have been measured in CO2–O2 mixtures irradiated with single pulses from a Febetron 705 at a dose rate of 1026 eV g−1 s−1. Low concentrations of carbon dioxide in oxygen rapidly reduce the yield from G(O3) = 12.8 to G(O3) ≈ 9. At 300 Torr total pressure, as the oxygen concentration is reduced, the ozone yield decreases from this yield of G(O3) ≈ 9 to an extrapolated yield, at zero oxygen, of close to G(O3) = 7.8. Changes of yields with composition are explained in terms of ionic reactions, the main neutralization process being[Formula: see text]At 700–1500 Torr total pressure, the ozone yields are lower than that at 300 Torr. It is proposed that clustering of the ionic species affects the products of the neutralization reaction.Sulfur hexafluoride suppresses the dissociative neutralization reaction and ozone yields from mixtures containing 1.5–2% SF6 are those predicted from direct neutral dissociation processes in the pure gases.Computer calculations are used to compare the experimental results to the proposed mechanism and, in general, a good fit is obtained.


2007 ◽  
Vol 17 (4) ◽  
pp. 227-229 ◽  
Author(s):  
Alexei V. Bludenko ◽  
Alexandr V. Ponomarev ◽  
Vladimir N. Chulkov ◽  
Ilgizar A. Yakushev ◽  
Rafinat S. Yarullin

Author(s):  
M. Isaacson ◽  
M.L. Collins ◽  
M. Listvan

Over the past five years it has become evident that radiation damage provides the fundamental limit to the study of blomolecular structure by electron microscopy. In some special cases structural determinations at very low doses can be achieved through superposition techniques to study periodic (Unwin & Henderson, 1975) and nonperiodic (Saxton & Frank, 1977) specimens. In addition, protection methods such as glucose embedding (Unwin & Henderson, 1975) and maintenance of specimen hydration at low temperatures (Taylor & Glaeser, 1976) have also shown promise. Despite these successes, the basic nature of radiation damage in the electron microscope is far from clear. In general we cannot predict exactly how different structures will behave during electron Irradiation at high dose rates. Moreover, with the rapid rise of analytical electron microscopy over the last few years, nvicroscopists are becoming concerned with questions of compositional as well as structural integrity. It is important to measure changes in elemental composition arising from atom migration in or loss from the specimen as a result of electron bombardment.


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