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Direct measurement of thicknesses, volumes or compositions of nanomaterials by quantitative atomic number contrast in high-angle annular dark-field scanning transmission electron microscopy

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Date Issued:
2012
Abstract/Description:
The sizes, shapes, volumes and compositions of nanoparticles are very important parameters determining many of their properties. Efforts to measure these parameters for individual nanoparticles and to obtain reliable statistics for a large number of nanoparticles require a fast and reliable method for 3-D characterization. In this dissertation, a direct measurement method for thicknesses, volumes or compositions of nanomaterials by quantitative atomic number contrast in High-Angle Annular Dark-Field (HAADF) Scanning Transmission Electron Microscopy (STEM) is presented. A HAADF detector collects electrons scattered incoherently to high angles. The HAADF signal intensity is in first-order approximation proportional to the sample thickness and increases with atomic number. However, for larger sample thicknesses this approach fails. A simple description for the thickness dependence of the HAADF-STEM contrast has been developed in this dissertation. A new method for the calibration of the sensitivity of the HAADF detector for a FEI F30 transmission electron microscope (TEM) is developed in this dissertation. A nearly linear relationship of the HAADF signal with the electron current is confirmed. Cross sections of multilayered samples provided by TriQuint Semiconductors in Apopka, FL, for contrast calibration were obtained by focused ion-beam (FIB) preparation yielding data on the interaction cross section per atom.To obtain an absolute intensity calibration of the HAADF-STEM intensity, Convergent Beam Electron Diffraction (CBED) was performed on Si single crystals. However, for samples prepared by the focused ion beam technique, CBED often significantly underestimates the sample thickness. Multislice simulations from Dr. Kirkland's C codes are used for comparison with experimental results. TEM offers high lateral resolution, but contains little or no information on the thickness of samples. Thickness maps in energy-filtered TEM (EFTEM), CBED and tilt series are so far the only methods to determine thicknesses of particles in TEM. In this work I have introduced the use of wedge-shaped multilayer samples prepared by FIB for the calibration of HAADF-STEM contrasts. This method yields quantitative contrast data as a function of sample thickness. A database with several pure elements and compounds has been compiled, containing experimental data on the fraction of electrons scattered onto the HAADF detector for each nanometer of sample thickness. The use of thick samples reveals an increased signal at the interfaces of high- and low-density materials. This effect can be explained by the transfer of scattered electrons from the high density material across the interface into the less-absorbing low-density material. The calibrations were used to determine concentration gradients in nanoscale Fe-Pt multilayers as well as thicknesses and volumes of individual Au-Fe, Pt, and Ag nanoparticles. Volumes of nanoparticles with known composition can be determined with accuracy better than 15%. Porosity determination of materials becomes available with this method as shown in an example of porous Silicon.?
Title: Direct measurement of thicknesses, volumes or compositions of nanomaterials by quantitative atomic number contrast in high-angle annular dark-field scanning transmission electron microscopy.
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Name(s): Yuan, Biao, Author
Heinrich, Helge, Committee Chair
Sohn, Yongho, Committee CoChair
Coffey, Kevin, Committee Member
Fang, Jiyu, Committee Member
Roldan Cuenya, Beatriz, Committee Member
University of Central Florida, Degree Grantor
Type of Resource: text
Date Issued: 2012
Publisher: University of Central Florida
Language(s): English
Abstract/Description: The sizes, shapes, volumes and compositions of nanoparticles are very important parameters determining many of their properties. Efforts to measure these parameters for individual nanoparticles and to obtain reliable statistics for a large number of nanoparticles require a fast and reliable method for 3-D characterization. In this dissertation, a direct measurement method for thicknesses, volumes or compositions of nanomaterials by quantitative atomic number contrast in High-Angle Annular Dark-Field (HAADF) Scanning Transmission Electron Microscopy (STEM) is presented. A HAADF detector collects electrons scattered incoherently to high angles. The HAADF signal intensity is in first-order approximation proportional to the sample thickness and increases with atomic number. However, for larger sample thicknesses this approach fails. A simple description for the thickness dependence of the HAADF-STEM contrast has been developed in this dissertation. A new method for the calibration of the sensitivity of the HAADF detector for a FEI F30 transmission electron microscope (TEM) is developed in this dissertation. A nearly linear relationship of the HAADF signal with the electron current is confirmed. Cross sections of multilayered samples provided by TriQuint Semiconductors in Apopka, FL, for contrast calibration were obtained by focused ion-beam (FIB) preparation yielding data on the interaction cross section per atom.To obtain an absolute intensity calibration of the HAADF-STEM intensity, Convergent Beam Electron Diffraction (CBED) was performed on Si single crystals. However, for samples prepared by the focused ion beam technique, CBED often significantly underestimates the sample thickness. Multislice simulations from Dr. Kirkland's C codes are used for comparison with experimental results. TEM offers high lateral resolution, but contains little or no information on the thickness of samples. Thickness maps in energy-filtered TEM (EFTEM), CBED and tilt series are so far the only methods to determine thicknesses of particles in TEM. In this work I have introduced the use of wedge-shaped multilayer samples prepared by FIB for the calibration of HAADF-STEM contrasts. This method yields quantitative contrast data as a function of sample thickness. A database with several pure elements and compounds has been compiled, containing experimental data on the fraction of electrons scattered onto the HAADF detector for each nanometer of sample thickness. The use of thick samples reveals an increased signal at the interfaces of high- and low-density materials. This effect can be explained by the transfer of scattered electrons from the high density material across the interface into the less-absorbing low-density material. The calibrations were used to determine concentration gradients in nanoscale Fe-Pt multilayers as well as thicknesses and volumes of individual Au-Fe, Pt, and Ag nanoparticles. Volumes of nanoparticles with known composition can be determined with accuracy better than 15%. Porosity determination of materials becomes available with this method as shown in an example of porous Silicon.?
Identifier: CFE0004464 (IID), ucf:49355 (fedora)
Note(s): 2012-08-01
Ph.D.
Engineering and Computer Science, Mechanical, Materials and Aerospace Engineering
Doctoral
This record was generated from author submitted information.
Subject(s): HAADF-STEM -- HAADF -- STEM -- TEM -- Nano -- Nanomaterials -- Thickness -- Quantitative -- Atomic number contrast -- Characterization
Persistent Link to This Record: http://purl.flvc.org/ucf/fd/CFE0004464
Restrictions on Access: public 2012-08-15
Host Institution: UCF

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