Laser illuminated gold nanoparticles (AuNPs) efficiently absorb light and heat up the surrounding medium, leading to versatile applications ranging from plasmonic catalysis to cancer photothermal therapy. Therefore, an in-depth understanding of the thermal, optical, and electron induced reaction pathways is required. Here, the electrophilic DNA nucleobase analog 5-Bromouracil (BrU) has been used as a model compound to study its decomposition in the vicinity of AuNPs illuminated with intense ns laser pulses under various conditions. The plasmonic response of the AuNPs and the concentration of BrU and resulting photoproducts have been tracked by ultraviolet and visible (UV–Vis) spectroscopy as a function of the irradiation time. A kinetic model has been developed to determine the reaction rates of two parallel fragmentation pathways of BrU, and their dependency on laser fluence and adsorption on the AuNP have been evaluated. In addition, the size and the electric field enhancement of the decomposed AuNPs have been determined by atomic force microscopy and finite domain time difference calculations, respectively. A minor influence of the direct photoreaction and a strong effect of the heating of the AuNPs have been revealed. However, due to the size reduction of the irradiated AuNPs, a trade-off between laser fluence and plasmonic response of the AuNPs has been observed. Hence, the decomposition of the AuNPs might be limiting the achievable temperatures under irradiation with several laser pulses. These findings need to be considered for an efficient design of catalytic plasmonic systems.
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31 March 2020
Research Article|
March 26 2020
Kinetics of molecular decomposition under irradiation of gold nanoparticles with nanosecond laser pulses—A 5-Bromouracil case study Available to Purchase
Special Collection:
Emerging Directions in Plasmonics
Telma S. Marques
;
Telma S. Marques
1
School of Physical Sciences, The Open University
, Walton Hall, MK7 6AA, Milton Keynes, United Kingdom
2
CEFITEC, Departamento de Física, Faculdade de Ciências e Tecnologia, Universidade Nova de Lisboa
, 2829-516 Caparica, Portugal
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Robin Schürmann
;
Robin Schürmann
3
Physical Chemistry, Institute of Chemistry, University of Potsdam
, Karl-Liebknecht-Str. 24-25, 14476 Potsdam-Golm, Germany
4
Department of Analytical Chemistry BAM, Federal Institute of Material Research and Testing
, Richard-Willstätter-Str. 11, 12489 Berlin, Germany
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Kenny Ebel;
Kenny Ebel
3
Physical Chemistry, Institute of Chemistry, University of Potsdam
, Karl-Liebknecht-Str. 24-25, 14476 Potsdam-Golm, Germany
4
Department of Analytical Chemistry BAM, Federal Institute of Material Research and Testing
, Richard-Willstätter-Str. 11, 12489 Berlin, Germany
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Christian Heck
;
Christian Heck
3
Physical Chemistry, Institute of Chemistry, University of Potsdam
, Karl-Liebknecht-Str. 24-25, 14476 Potsdam-Golm, Germany
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Małgorzata A. Śmiałek
;
Małgorzata A. Śmiałek
1
School of Physical Sciences, The Open University
, Walton Hall, MK7 6AA, Milton Keynes, United Kingdom
5
Department of Control and Power Engineering, Faculty of Ocean Engineering and Ship Technology, Gdansk University of Technology
, Gabriela Narutowicza 11/12, 80-233 Gdansk, Poland
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Sam Eden
;
Sam Eden
1
School of Physical Sciences, The Open University
, Walton Hall, MK7 6AA, Milton Keynes, United Kingdom
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Nigel Mason
;
Nigel Mason
1
School of Physical Sciences, The Open University
, Walton Hall, MK7 6AA, Milton Keynes, United Kingdom
6
School of Physical Sciences, University of Kent
, Canterbury CT2 7NH, United Kingdom
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Ilko Bald
Ilko Bald
a)
3
Physical Chemistry, Institute of Chemistry, University of Potsdam
, Karl-Liebknecht-Str. 24-25, 14476 Potsdam-Golm, Germany
4
Department of Analytical Chemistry BAM, Federal Institute of Material Research and Testing
, Richard-Willstätter-Str. 11, 12489 Berlin, Germany
a)Author to whom correspondence should be addressed: [email protected]
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Telma S. Marques
1,2
Robin Schürmann
3,4
Kenny Ebel
3,4
Christian Heck
3
Małgorzata A. Śmiałek
1,5
Sam Eden
1
Nigel Mason
1,6
Ilko Bald
3,4,a)
1
School of Physical Sciences, The Open University
, Walton Hall, MK7 6AA, Milton Keynes, United Kingdom
2
CEFITEC, Departamento de Física, Faculdade de Ciências e Tecnologia, Universidade Nova de Lisboa
, 2829-516 Caparica, Portugal
3
Physical Chemistry, Institute of Chemistry, University of Potsdam
, Karl-Liebknecht-Str. 24-25, 14476 Potsdam-Golm, Germany
4
Department of Analytical Chemistry BAM, Federal Institute of Material Research and Testing
, Richard-Willstätter-Str. 11, 12489 Berlin, Germany
5
Department of Control and Power Engineering, Faculty of Ocean Engineering and Ship Technology, Gdansk University of Technology
, Gabriela Narutowicza 11/12, 80-233 Gdansk, Poland
6
School of Physical Sciences, University of Kent
, Canterbury CT2 7NH, United Kingdom
a)Author to whom correspondence should be addressed: [email protected]
Note: This paper is part of the JCP Special Topic on Emerging Directions in Plasmonics.
J. Chem. Phys. 152, 124712 (2020)
Article history
Received:
November 13 2019
Accepted:
February 21 2020
Citation
Telma S. Marques, Robin Schürmann, Kenny Ebel, Christian Heck, Małgorzata A. Śmiałek, Sam Eden, Nigel Mason, Ilko Bald; Kinetics of molecular decomposition under irradiation of gold nanoparticles with nanosecond laser pulses—A 5-Bromouracil case study. J. Chem. Phys. 31 March 2020; 152 (12): 124712. https://doi.org/10.1063/1.5137898
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