Improved Models for Metallic Nanoparticle Cores from Atomic Pair Distribution Function (PDF) Analysis
Abstract
X-ray atomic pair distribution functions (PDFs) were collected from a range of canonical metallic nanomaterials, both elemental and alloyed, prepared using different synthesis methods and exhibiting drastically different morphological properties. Widely applied shape-tuned attenuated crystal (AC) fcc models proved inadequate, yielding structured, coherent, and correlated fit residuals. However, equally simple discrete cluster models could account for the largest amplitude features in these difference signals. A hypothesis testing based approach to nanoparticle structure modeling systematically ruled out effects from crystallite size, composition, shape, and surface faceting as primary factors contributing to the AC misfit. On the other hand, decahedrally twinned cluster cores were found to be the origin of the AC structure misfits for a majority of the nanomaterials reported here. It is further motivated that the PDF can readily differentiate between the arrangement of domains in these multiply twinned motifs. Most of the nanomaterials surveyed also fall within the sub-5 nm size regime where traditional electron microscopy cannot easily detect and quantify domain structures, with sampling representative of the average nanocrystal synthesized. Here, the results demonstrate that PDF analysis is a powerful method for understanding internal atomic interfaces in small noble metallic nanomaterials. Such core cluster models, easily built algorithmically,more »
- Authors:
-
- Columbia Univ., New York, NY (United States)
- Univ. of Pennsylvania, Philadelphia, PA (United States)
- Univ. of Copenhagen, Copenhagen (Denmark)
- Univ. of Duisburg-Essen, Essen (Germany)
- State Univ. of New York at Stony Brook, Stony Brook, NY (United States); Fordham Univ., Bronx, NY (United States)
- State Univ. of New York at Stony Brook, Stony Brook, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Catalysis Center for Energy Innovation (CCEI); Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1487255
- Report Number(s):
- BNL-209757-2018-JAAM
Journal ID: ISSN 1932-7447
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 122; Journal Issue: 51; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Citation Formats
Banerjee, Soham, Liu, Chia -Hao, Lee, Jennifer D., Kovyakh, Anton, Grasmik, Viktoria, Prymak, Oleg, Koenigsmann, Christopher, Liu, Haiqing, Wang, Lei, Abeykoon, A. M. Milinda, Wong, Stanislaus S., Epple, Matthias, Murray, Christopher B., and Billinge, Simon J. L. Improved Models for Metallic Nanoparticle Cores from Atomic Pair Distribution Function (PDF) Analysis. United States: N. p., 2018.
Web. doi:10.1021/acs.jpcc.8b05897.
Banerjee, Soham, Liu, Chia -Hao, Lee, Jennifer D., Kovyakh, Anton, Grasmik, Viktoria, Prymak, Oleg, Koenigsmann, Christopher, Liu, Haiqing, Wang, Lei, Abeykoon, A. M. Milinda, Wong, Stanislaus S., Epple, Matthias, Murray, Christopher B., & Billinge, Simon J. L. Improved Models for Metallic Nanoparticle Cores from Atomic Pair Distribution Function (PDF) Analysis. United States. https://doi.org/10.1021/acs.jpcc.8b05897
Banerjee, Soham, Liu, Chia -Hao, Lee, Jennifer D., Kovyakh, Anton, Grasmik, Viktoria, Prymak, Oleg, Koenigsmann, Christopher, Liu, Haiqing, Wang, Lei, Abeykoon, A. M. Milinda, Wong, Stanislaus S., Epple, Matthias, Murray, Christopher B., and Billinge, Simon J. L. Mon .
"Improved Models for Metallic Nanoparticle Cores from Atomic Pair Distribution Function (PDF) Analysis". United States. https://doi.org/10.1021/acs.jpcc.8b05897. https://www.osti.gov/servlets/purl/1487255.
@article{osti_1487255,
title = {Improved Models for Metallic Nanoparticle Cores from Atomic Pair Distribution Function (PDF) Analysis},
author = {Banerjee, Soham and Liu, Chia -Hao and Lee, Jennifer D. and Kovyakh, Anton and Grasmik, Viktoria and Prymak, Oleg and Koenigsmann, Christopher and Liu, Haiqing and Wang, Lei and Abeykoon, A. M. Milinda and Wong, Stanislaus S. and Epple, Matthias and Murray, Christopher B. and Billinge, Simon J. L.},
abstractNote = {X-ray atomic pair distribution functions (PDFs) were collected from a range of canonical metallic nanomaterials, both elemental and alloyed, prepared using different synthesis methods and exhibiting drastically different morphological properties. Widely applied shape-tuned attenuated crystal (AC) fcc models proved inadequate, yielding structured, coherent, and correlated fit residuals. However, equally simple discrete cluster models could account for the largest amplitude features in these difference signals. A hypothesis testing based approach to nanoparticle structure modeling systematically ruled out effects from crystallite size, composition, shape, and surface faceting as primary factors contributing to the AC misfit. On the other hand, decahedrally twinned cluster cores were found to be the origin of the AC structure misfits for a majority of the nanomaterials reported here. It is further motivated that the PDF can readily differentiate between the arrangement of domains in these multiply twinned motifs. Most of the nanomaterials surveyed also fall within the sub-5 nm size regime where traditional electron microscopy cannot easily detect and quantify domain structures, with sampling representative of the average nanocrystal synthesized. Here, the results demonstrate that PDF analysis is a powerful method for understanding internal atomic interfaces in small noble metallic nanomaterials. Such core cluster models, easily built algorithmically, should serve as starting structures for more advanced models able to capture atomic positional disorder, ligand induced or otherwise, near nanocrystal surfaces.},
doi = {10.1021/acs.jpcc.8b05897},
journal = {Journal of Physical Chemistry. C},
number = 51,
volume = 122,
place = {United States},
year = {Mon Nov 26 00:00:00 EST 2018},
month = {Mon Nov 26 00:00:00 EST 2018}
}
Web of Science
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