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Article

Gold Nanoparticle Formation via X-ray Radiolysis Investigated with Time-Resolved X-ray Liquidography

by 1,2,3, 1,2,3, 1,2,3,4, 1,2,3, 1,2,3, 1,2,3, 1,2,3, 1,2,3, 1, 1,2,3, 1,2,3, 1,4 and 1,2,3,*
1
Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Korea
2
KI for the BioCentury, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Korea
3
Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS), Daejeon 34141, Korea
4
Center for Catalytic Hydrocarbon Functionalizations, Institute for Basic Science (IBS), Daejeon 34141, Korea
*
Author to whom correspondence should be addressed.
Int. J. Mol. Sci. 2020, 21(19), 7125; https://0-doi-org.brum.beds.ac.uk/10.3390/ijms21197125
Received: 29 August 2020 / Revised: 23 September 2020 / Accepted: 24 September 2020 / Published: 27 September 2020
(This article belongs to the Collection Feature Papers in Physical Chemistry and Chemical Physics)
We report the generation of gold nanoparticles (AuNPs) from the aqueous solution of chloro(2,2′,2″-terpyridine)gold(III) ion ([Au(tpy)Cl]2+) through X-ray radiolysis and optical excitation at a synchrotron. The original purpose of the experiment was to investigate the photoinduced structural changes of [Au(tpy)Cl]2+ upon 400 nm excitation using time-resolved X-ray liquidography (TRXL). Initially, the TRXL data did not show any signal that would suggest structural changes of the solute molecule, but after an induction time, the TRXL data started to show sharp peaks and valleys. In the early phase, AuNPs with two types of morphology, dendrites, and spheres, were formed by the reducing action of hydrated electrons generated by the X-ray radiolysis of water, thereby allowing the detection of TRXL data due to the laser-induced lattice expansion and relaxation of AuNPs. Along with the lattice expansion, the dendritic and spherical AuNPs were transformed into smaller, raspberry-shaped AuNPs of a relatively uniform size via ablation by the optical femtosecond laser pulse used for the TRXL experiment. Density functional theory calculations confirm that the reduction potential of the metal complex relative to the hydration potential of X-ray-generated electrons determines the facile AuNP formation observed for [Au(tpy)Cl]2+. View Full-Text
Keywords: X-ray radiolysis; gold nanoparticle; time-resolved X-ray liquidography; laser ablation X-ray radiolysis; gold nanoparticle; time-resolved X-ray liquidography; laser ablation
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MDPI and ACS Style

Ki, H.; Park, S.; Eom, S.; Gu, J.; Kim, S.; Kim, C.; Ahn, C.W.; Choi, M.; Ahn, S.; Ahn, D.-S.; Choi, J.; Baik, M.-H.; Ihee, H. Gold Nanoparticle Formation via X-ray Radiolysis Investigated with Time-Resolved X-ray Liquidography. Int. J. Mol. Sci. 2020, 21, 7125. https://0-doi-org.brum.beds.ac.uk/10.3390/ijms21197125

AMA Style

Ki H, Park S, Eom S, Gu J, Kim S, Kim C, Ahn CW, Choi M, Ahn S, Ahn D-S, Choi J, Baik M-H, Ihee H. Gold Nanoparticle Formation via X-ray Radiolysis Investigated with Time-Resolved X-ray Liquidography. International Journal of Molecular Sciences. 2020; 21(19):7125. https://0-doi-org.brum.beds.ac.uk/10.3390/ijms21197125

Chicago/Turabian Style

Ki, Hosung, Sungjun Park, Seunghwan Eom, Jain Gu, Siin Kim, Changwon Kim, Chi W. Ahn, Minseo Choi, Sena Ahn, Doo-Sik Ahn, Jungkweon Choi, Mu-Hyun Baik, and Hyotcherl Ihee. 2020. "Gold Nanoparticle Formation via X-ray Radiolysis Investigated with Time-Resolved X-ray Liquidography" International Journal of Molecular Sciences 21, no. 19: 7125. https://0-doi-org.brum.beds.ac.uk/10.3390/ijms21197125

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