Combined Experimental and Theoretical Investigation on Formation of Size-Controlled Silver Nanoclusters under Gas Phase
Metallic nanoclusters (NCs) have been predicted to achieve the best Surface-Enhanced Raman Scattering (SERS) due to the controllable amount of atoms and structures in NCs. The Local Surface Plasmon Resonance (LSPR) effect on silver metal NCs (Ag<inline-formula><math xmlns="http://www.w...
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MDPI AG
2022-04-01
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| author | Chuhang Zhang |
| author_facet | Chuhang Zhang |
| author_sort | Chuhang Zhang |
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| description | Metallic nanoclusters (NCs) have been predicted to achieve the best Surface-Enhanced Raman Scattering (SERS) due to the controllable amount of atoms and structures in NCs. The Local Surface Plasmon Resonance (LSPR) effect on silver metal NCs (Ag<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mi>n</mi></msub></semantics></math></inline-formula>) enables it to be a promising candidate for manipulating the LSPR peak by controlling the size of NCs, which in turn demands a full understanding of the formation mechanism of Ag<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mi>n</mi></msub></semantics></math></inline-formula>. Here, we apply an extended Smoluchowski rate equation coupled with a fragmentation scheme to investigate the growth of size-selected silver NCs generated via a modulated pulsed power magnetron sputtering (MPP-MSP). A temperature-dependent fragmentation coefficient <i>D</i> is proposed and integrated into the rate equations. The consistency between the computational and experimental results shows that in relative low peak power (<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msub><mi>P</mi><mi>p</mi></msub><mo>≤</mo><mn>800</mn></mrow></semantics></math></inline-formula> W), the recombination of cation and anion species are the dominant mechanism for NC growth. However, in the higher <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mi>P</mi><mi>p</mi></msub></semantics></math></inline-formula> region (≥800 W), the fragmentation mechanism becomes more impactful, leading to the formation of smaller NCs. The scanning electron microscopy observation shows the Ag<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>36</mn></msub></semantics></math></inline-formula> is successfully soft-landed and immobilized on a strontium titanate crystal, which facilitates the application of the Ag<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mi>n</mi></msub></semantics></math></inline-formula>/STO to the SERS research. |
| first_indexed | 2024-03-10T03:15:17Z |
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| language | English |
| last_indexed | 2024-03-10T03:15:17Z |
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| spelling | doaj.art-29879258ad8045a1bce6c0bc7e07f4912023-11-23T10:15:14ZengMDPI AGBiosensors2079-63742022-04-0112528210.3390/bios12050282Combined Experimental and Theoretical Investigation on Formation of Size-Controlled Silver Nanoclusters under Gas PhaseChuhang Zhang0Physics Department, Zhejiang University of Science and Technology, 318 Liuhe Road, Xihu District, Hangzhou 310008, ChinaMetallic nanoclusters (NCs) have been predicted to achieve the best Surface-Enhanced Raman Scattering (SERS) due to the controllable amount of atoms and structures in NCs. The Local Surface Plasmon Resonance (LSPR) effect on silver metal NCs (Ag<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mi>n</mi></msub></semantics></math></inline-formula>) enables it to be a promising candidate for manipulating the LSPR peak by controlling the size of NCs, which in turn demands a full understanding of the formation mechanism of Ag<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mi>n</mi></msub></semantics></math></inline-formula>. Here, we apply an extended Smoluchowski rate equation coupled with a fragmentation scheme to investigate the growth of size-selected silver NCs generated via a modulated pulsed power magnetron sputtering (MPP-MSP). A temperature-dependent fragmentation coefficient <i>D</i> is proposed and integrated into the rate equations. The consistency between the computational and experimental results shows that in relative low peak power (<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msub><mi>P</mi><mi>p</mi></msub><mo>≤</mo><mn>800</mn></mrow></semantics></math></inline-formula> W), the recombination of cation and anion species are the dominant mechanism for NC growth. However, in the higher <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mi>P</mi><mi>p</mi></msub></semantics></math></inline-formula> region (≥800 W), the fragmentation mechanism becomes more impactful, leading to the formation of smaller NCs. The scanning electron microscopy observation shows the Ag<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mn>36</mn></msub></semantics></math></inline-formula> is successfully soft-landed and immobilized on a strontium titanate crystal, which facilitates the application of the Ag<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mrow></mrow><mi>n</mi></msub></semantics></math></inline-formula>/STO to the SERS research.https://www.mdpi.com/2079-6374/12/5/282silver nanoclusterformation mechanismSmoluchowski equationfragmentation |
| spellingShingle | Chuhang Zhang Combined Experimental and Theoretical Investigation on Formation of Size-Controlled Silver Nanoclusters under Gas Phase Biosensors silver nanocluster formation mechanism Smoluchowski equation fragmentation |
| title | Combined Experimental and Theoretical Investigation on Formation of Size-Controlled Silver Nanoclusters under Gas Phase |
| title_full | Combined Experimental and Theoretical Investigation on Formation of Size-Controlled Silver Nanoclusters under Gas Phase |
| title_fullStr | Combined Experimental and Theoretical Investigation on Formation of Size-Controlled Silver Nanoclusters under Gas Phase |
| title_full_unstemmed | Combined Experimental and Theoretical Investigation on Formation of Size-Controlled Silver Nanoclusters under Gas Phase |
| title_short | Combined Experimental and Theoretical Investigation on Formation of Size-Controlled Silver Nanoclusters under Gas Phase |
| title_sort | combined experimental and theoretical investigation on formation of size controlled silver nanoclusters under gas phase |
| topic | silver nanocluster formation mechanism Smoluchowski equation fragmentation |
| url | https://www.mdpi.com/2079-6374/12/5/282 |
| work_keys_str_mv | AT chuhangzhang combinedexperimentalandtheoreticalinvestigationonformationofsizecontrolledsilvernanoclustersundergasphase |