The N3/TiO2 interfacial structure is dependent on the pH conditions during sensitization
The electronic structure of the N3/TiO2 interface can directly influence the performance of a dye sensitized solar cell (DSSC). Therefore, it is crucial to understand the parameters that control the dye’s orientation on the semiconductor’s surface. A typical step in DSSC fabrication is to submerge t...
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Veröffentlicht in: | The Journal of chemical physics 2022-07, Vol.157 (4), p.044702-044702 |
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creator | Farah, Yusef R. Krummel, Amber T. |
description | The electronic structure of the N3/TiO2 interface can directly influence the performance of a dye sensitized solar cell (DSSC). Therefore, it is crucial to understand the parameters that control the dye’s orientation on the semiconductor’s surface. A typical step in DSSC fabrication is to submerge the nanoparticulate semiconductor film in a solution containing the dye, the sensitizing solution. The pH of the N3 sensitizing solution determines the distribution of the N3 protonation states that exist in solution. Altering the pH of the sensitizing solution changes the N3 protonation states that exist in solution and, subsequently, the N3 protonation states that anchor to the TiO2 substrate. We utilize the surface specific technique of heterodyne detected vibrational sum frequency generation spectroscopy to determine the binding geometry of N3 on a TiO2 surface as a function of the sensitizing solution pH conditions. It is determined that significant reorientation of the dye occurs in pH ≤2.0 conditions due to the lack of N3-dye carboxylate anchoring groups participating in adsorption to the TiO2 substrate. Consequently, the change in molecular geometry is met with a change in the interfacial electronic structure that can hinder electron transfer in DSSC architectures. |
doi_str_mv | 10.1063/5.0099543 |
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Therefore, it is crucial to understand the parameters that control the dye’s orientation on the semiconductor’s surface. A typical step in DSSC fabrication is to submerge the nanoparticulate semiconductor film in a solution containing the dye, the sensitizing solution. The pH of the N3 sensitizing solution determines the distribution of the N3 protonation states that exist in solution. Altering the pH of the sensitizing solution changes the N3 protonation states that exist in solution and, subsequently, the N3 protonation states that anchor to the TiO2 substrate. We utilize the surface specific technique of heterodyne detected vibrational sum frequency generation spectroscopy to determine the binding geometry of N3 on a TiO2 surface as a function of the sensitizing solution pH conditions. It is determined that significant reorientation of the dye occurs in pH ≤2.0 conditions due to the lack of N3-dye carboxylate anchoring groups participating in adsorption to the TiO2 substrate. Consequently, the change in molecular geometry is met with a change in the interfacial electronic structure that can hinder electron transfer in DSSC architectures.</description><identifier>ISSN: 0021-9606</identifier><identifier>EISSN: 1089-7690</identifier><identifier>DOI: 10.1063/5.0099543</identifier><identifier>CODEN: JCPSA6</identifier><language>eng</language><publisher>Melville: American Institute of Physics</publisher><subject>Dye-sensitized solar cells ; Dyes ; Electron transfer ; Electronic structure ; Physics ; Protonation ; Sensitizing ; Substrates ; Titanium dioxide</subject><ispartof>The Journal of chemical physics, 2022-07, Vol.157 (4), p.044702-044702</ispartof><rights>Author(s)</rights><rights>2022 Author(s). 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Therefore, it is crucial to understand the parameters that control the dye’s orientation on the semiconductor’s surface. A typical step in DSSC fabrication is to submerge the nanoparticulate semiconductor film in a solution containing the dye, the sensitizing solution. The pH of the N3 sensitizing solution determines the distribution of the N3 protonation states that exist in solution. Altering the pH of the sensitizing solution changes the N3 protonation states that exist in solution and, subsequently, the N3 protonation states that anchor to the TiO2 substrate. We utilize the surface specific technique of heterodyne detected vibrational sum frequency generation spectroscopy to determine the binding geometry of N3 on a TiO2 surface as a function of the sensitizing solution pH conditions. It is determined that significant reorientation of the dye occurs in pH ≤2.0 conditions due to the lack of N3-dye carboxylate anchoring groups participating in adsorption to the TiO2 substrate. Consequently, the change in molecular geometry is met with a change in the interfacial electronic structure that can hinder electron transfer in DSSC architectures.</description><subject>Dye-sensitized solar cells</subject><subject>Dyes</subject><subject>Electron transfer</subject><subject>Electronic structure</subject><subject>Physics</subject><subject>Protonation</subject><subject>Sensitizing</subject><subject>Substrates</subject><subject>Titanium dioxide</subject><issn>0021-9606</issn><issn>1089-7690</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><recordid>eNqd0U1LBCEYAGCJgratQ_9A6lLBtK86o-Mxlr4g2ssG3WTWccrY1UmdoH59brsQdOwkvj7q-4HQMYFLApxNqksAKauS7aARgVoWgkvYRSMASgrJge-jgxjfAIAIWo7Q8_zV4Ec2mdsZxdYlE7pG22aJYwqDTkMw2Ebcmt641riEvcMp3-jvsPautcl6l4-HYN0LjsbFHPlq1tFDtNc1y2iOtusYPd1cz6d3xcPs9n569VBoRmgqCNE1yM6UVFPGRJP3HWcll3XNKwmSMFK29YKKugLdEcMbSlsBrWR0wStgbIxONu_6mKyK2iajX3NuzuikSC0kIXVGZxvUB_8-mJjUykZtlsvGGT9ERfN_nFEQNNPTP_TND8HlEtZKECEpQFbnG6WDjzGYTvXBrprwqQio9SBUpbaDyPZiY9fJ_fTmf_jDh1-o-rZj377xk5g</recordid><startdate>20220728</startdate><enddate>20220728</enddate><creator>Farah, Yusef R.</creator><creator>Krummel, Amber T.</creator><general>American Institute of Physics</general><scope>AAYXX</scope><scope>CITATION</scope><scope>8FD</scope><scope>H8D</scope><scope>L7M</scope><scope>7X8</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0003-3973-1575</orcidid><orcidid>https://orcid.org/0000000339731575</orcidid></search><sort><creationdate>20220728</creationdate><title>The N3/TiO2 interfacial structure is dependent on the pH conditions during sensitization</title><author>Farah, Yusef R. ; Krummel, Amber T.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c312t-11c809fe42c2337a11cf6346988659091314d8b27850cf1e6a22d70d932b65033</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2022</creationdate><topic>Dye-sensitized solar cells</topic><topic>Dyes</topic><topic>Electron transfer</topic><topic>Electronic structure</topic><topic>Physics</topic><topic>Protonation</topic><topic>Sensitizing</topic><topic>Substrates</topic><topic>Titanium dioxide</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Farah, Yusef R.</creatorcontrib><creatorcontrib>Krummel, Amber T.</creatorcontrib><collection>CrossRef</collection><collection>Technology Research Database</collection><collection>Aerospace Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>MEDLINE - Academic</collection><collection>OSTI.GOV</collection><jtitle>The Journal of chemical physics</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Farah, Yusef R.</au><au>Krummel, Amber T.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>The N3/TiO2 interfacial structure is dependent on the pH conditions during sensitization</atitle><jtitle>The Journal of chemical physics</jtitle><date>2022-07-28</date><risdate>2022</risdate><volume>157</volume><issue>4</issue><spage>044702</spage><epage>044702</epage><pages>044702-044702</pages><issn>0021-9606</issn><eissn>1089-7690</eissn><coden>JCPSA6</coden><abstract>The electronic structure of the N3/TiO2 interface can directly influence the performance of a dye sensitized solar cell (DSSC). Therefore, it is crucial to understand the parameters that control the dye’s orientation on the semiconductor’s surface. A typical step in DSSC fabrication is to submerge the nanoparticulate semiconductor film in a solution containing the dye, the sensitizing solution. The pH of the N3 sensitizing solution determines the distribution of the N3 protonation states that exist in solution. Altering the pH of the sensitizing solution changes the N3 protonation states that exist in solution and, subsequently, the N3 protonation states that anchor to the TiO2 substrate. We utilize the surface specific technique of heterodyne detected vibrational sum frequency generation spectroscopy to determine the binding geometry of N3 on a TiO2 surface as a function of the sensitizing solution pH conditions. It is determined that significant reorientation of the dye occurs in pH ≤2.0 conditions due to the lack of N3-dye carboxylate anchoring groups participating in adsorption to the TiO2 substrate. 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source | AIP Journals Complete; Alma/SFX Local Collection |
subjects | Dye-sensitized solar cells Dyes Electron transfer Electronic structure Physics Protonation Sensitizing Substrates Titanium dioxide |
title | The N3/TiO2 interfacial structure is dependent on the pH conditions during sensitization |
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