DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Ultra-Fast Electron Microscopic Imaging of Single Molecules With a Direct Electron Detection Camera and Noise Reduction

Abstract

Time-resolved imaging of molecules and materials made of light elements is an emerging field of transmission electron microscopy (TEM), and the recent development of direct electron detection cameras, capable of taking as many as 1,600 fps, has potentially broadened the scope of the time-resolved TEM imaging in chemistry and nanotechnology. However, such a high frame rate reduces electron dose per frame, lowers the signal-to-noise ratio (SNR), and renders the molecular images practically invisible. Here, we examined image noise reduction to take the best advantage of fast cameras and concluded that the Chambolle total variation denoising algorithm is the method of choice, as illustrated for imaging of a molecule in the 1D hollow space of a carbon nanotube with ~1 ms time resolution. Through the systematic comparison of the performance of multiple denoising algorithms, we found that the Chambolle algorithm improves the SNR by more than an order of magnitude when applied to TEM images taken at a low electron dose as required for imaging at around 1,000 fps. Open-source code and a standalone application to apply Chambolle denoising to TEM images and video frames are available for download.

Authors:
ORCiD logo [1];  [2];  [2];  [2];  [1]
  1. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  2. Univ. of Tokyo (Japan)
Publication Date:
Research Org.:
Virginia Polytechnic Inst. and State University (Virginia Tech), Blacksburg, VA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1800341
Grant/Contract Number:  
FG02-06ER15786
Resource Type:
Accepted Manuscript
Journal Name:
Microscopy and Microanalysis
Additional Journal Information:
Journal Volume: 26; Journal Issue: 4; Journal ID: ISSN 1431-9276
Publisher:
Microscopy Society of America (MSA)
Country of Publication:
United States
Language:
English
Subject:
47 OTHER INSTRUMENTATION; materials science; microscopy; denoising; image analysis; image processing; single-molecule imaging; transmission electron microscopy

Citation Formats

Stuckner, Joshua, Shimizu, Toshiki, Harano, Koji, Nakamura, Eiichi, and Murayama, Mitsuhiro. Ultra-Fast Electron Microscopic Imaging of Single Molecules With a Direct Electron Detection Camera and Noise Reduction. United States: N. p., 2020. Web. doi:10.1017/s1431927620001750.
Stuckner, Joshua, Shimizu, Toshiki, Harano, Koji, Nakamura, Eiichi, & Murayama, Mitsuhiro. Ultra-Fast Electron Microscopic Imaging of Single Molecules With a Direct Electron Detection Camera and Noise Reduction. United States. https://doi.org/10.1017/s1431927620001750
Stuckner, Joshua, Shimizu, Toshiki, Harano, Koji, Nakamura, Eiichi, and Murayama, Mitsuhiro. Mon . "Ultra-Fast Electron Microscopic Imaging of Single Molecules With a Direct Electron Detection Camera and Noise Reduction". United States. https://doi.org/10.1017/s1431927620001750. https://www.osti.gov/servlets/purl/1800341.
@article{osti_1800341,
title = {Ultra-Fast Electron Microscopic Imaging of Single Molecules With a Direct Electron Detection Camera and Noise Reduction},
author = {Stuckner, Joshua and Shimizu, Toshiki and Harano, Koji and Nakamura, Eiichi and Murayama, Mitsuhiro},
abstractNote = {Time-resolved imaging of molecules and materials made of light elements is an emerging field of transmission electron microscopy (TEM), and the recent development of direct electron detection cameras, capable of taking as many as 1,600 fps, has potentially broadened the scope of the time-resolved TEM imaging in chemistry and nanotechnology. However, such a high frame rate reduces electron dose per frame, lowers the signal-to-noise ratio (SNR), and renders the molecular images practically invisible. Here, we examined image noise reduction to take the best advantage of fast cameras and concluded that the Chambolle total variation denoising algorithm is the method of choice, as illustrated for imaging of a molecule in the 1D hollow space of a carbon nanotube with ~1 ms time resolution. Through the systematic comparison of the performance of multiple denoising algorithms, we found that the Chambolle algorithm improves the SNR by more than an order of magnitude when applied to TEM images taken at a low electron dose as required for imaging at around 1,000 fps. Open-source code and a standalone application to apply Chambolle denoising to TEM images and video frames are available for download.},
doi = {10.1017/s1431927620001750},
journal = {Microscopy and Microanalysis},
number = 4,
volume = 26,
place = {United States},
year = {Mon Jul 20 00:00:00 EDT 2020},
month = {Mon Jul 20 00:00:00 EDT 2020}
}

Works referenced in this record:

Comparative study of Hough Transform methods for circle finding
journal, February 1990


Atomistic structures and dynamics of prenucleation clusters in MOF-2 and MOF-5 syntheses
journal, August 2019


Conformational Analysis of Single Perfluoroalkyl Chains by Single-Molecule Real-Time Transmission Electron Microscopic Imaging
journal, December 2013

  • Harano, Koji; Takenaga, Shinya; Okada, Satoshi
  • Journal of the American Chemical Society, Vol. 136, Issue 1
  • DOI: 10.1021/ja411235x

An Iterative Regularization Method for Total Variation-Based Image Restoration
journal, January 2005

  • Osher, Stanley; Burger, Martin; Goldfarb, Donald
  • Multiscale Modeling & Simulation, Vol. 4, Issue 2
  • DOI: 10.1137/040605412

Principal component analysis
journal, August 1987

  • Wold, Svante; Esbensen, Kim; Geladi, Paul
  • Chemometrics and Intelligent Laboratory Systems, Vol. 2, Issue 1-3
  • DOI: 10.1016/0169-7439(87)80084-9

Nonlinear total variation based noise removal algorithms
journal, November 1992


A matrix theory proof of the discrete convolution theorem
journal, December 1971


Electron Microscopic Observation of Selective Excitation of Conformational Change of a Single Organic Molecule
journal, March 2015

  • Gorgoll, Ricardo M.; Yücelen, Emrah; Kumamoto, Akihito
  • Journal of the American Chemical Society, Vol. 137, Issue 10
  • DOI: 10.1021/jacs.5b00511

An Algorithm for Total Variation Minimization and Applications
journal, January 2004


Real-Time Video Imaging of Mechanical Motions of a Single Molecular Shuttle with Sub-Millisecond Sub-Angstrom Precision
journal, September 2020

  • Shimizu, Toshiki; Lungerich, Dominik; Stuckner, Joshua
  • Bulletin of the Chemical Society of Japan, Vol. 93, Issue 9
  • DOI: 10.1246/bcsj.20200134

The Shannon sampling theorem—Its various extensions and applications: A tutorial review
journal, January 1977


Chambolle's Projection Algorithm for Total Variation Denoising
journal, January 2013

  • Duran, Joan; Coll, Bartomeu; Sbert, Catalina
  • Image Processing On Line, Vol. 3
  • DOI: 10.5201/ipol.2013.61

Bayesian estimation of regularization and point spread function parameters for Wiener–Hunt deconvolution
journal, January 2010

  • Orieux, François; Giovannelli, Jean-François; Rodet, Thomas
  • Journal of the Optical Society of America A, Vol. 27, Issue 7
  • DOI: 10.1364/JOSAA.27.001593

Unravelling surface and interfacial structures of a metal–organic framework by transmission electron microscopy
journal, February 2017

  • Zhu, Yihan; Ciston, Jim; Zheng, Bin
  • Nature Materials, Vol. 16, Issue 5
  • DOI: 10.1038/nmat4852

A Non-Local Algorithm for Image Denoising
conference, January 2005

  • Buades, A.; Coll, B.; Morel, J. -M.
  • 2005 IEEE Computer Society Conference on Computer Vision and Pattern Recognition (CVPR'05)
  • DOI: 10.1109/CVPR.2005.38

Facet development during platinum nanocube growth
journal, August 2014


Direct Microscopic Analysis of Individual C 60 Dimerization Events: Kinetics and Mechanisms
journal, December 2017

  • Okada, Satoshi; Kowashi, Satori; Schweighauser, Luca
  • Journal of the American Chemical Society, Vol. 139, Issue 50
  • DOI: 10.1021/jacs.7b09776

Heterogeneous nucleation of organic crystals mediated by single-molecule templates
journal, September 2012

  • Harano, Koji; Homma, Tatsuya; Niimi, Yoshiko
  • Nature Materials, Vol. 11, Issue 10
  • DOI: 10.1038/nmat3408

The size distribution, imaging and obstructing properties of C60 and higher fullerenes formed within arc-grown single walled carbon nanotubes
journal, January 2000


Point spread functions and deconvolution of ultrasonic images
journal, March 2015

  • Dalitz, Christoph; Pohle-Frohlich, Regina; Michalk, Thorsten
  • IEEE Transactions on Ultrasonics, Ferroelectrics, and Frequency Control, Vol. 62, Issue 3
  • DOI: 10.1109/TUFFC.2014.006717

Measurement of signal-to-noise ratios in MR images: Influence of multichannel coils, parallel imaging, and reconstruction filters
journal, January 2007

  • Dietrich, Olaf; Raya, José G.; Reeder, Scott B.
  • Journal of Magnetic Resonance Imaging, Vol. 26, Issue 2
  • DOI: 10.1002/jmri.20969

A Threshold Selection Method from Gray-Level Histograms
journal, January 1979


De-noising Filters for TEM (Transmission Electron Microscopy) Image of Nanomaterials
conference, January 2012

  • Kushwaha, Himmat S.; Tanwar, Sanju; Rathore, K. S.
  • Communication Technologies (ACCT), 2012 Second International Conference on Advanced Computing & Communication Technologies
  • DOI: 10.1109/ACCT.2012.41