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“Supersaturated” Self-Assembled Charge-Selective Interfacial Layers for Organic Solar Cells
To achieve densely packed charge-selective organosilane-based interfacial layers (IFLs) on the tin-doped indium oxide (ITO) anodes of organic photovoltaic (OPV) cells, a series of Ar2N-(CH2) n -SiCl3 precursors with Ar = 3,4-difluorophenyl, n = 3, 6, 10, and 18, was synthesized, characterized, and c...
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Published in: | Journal of the American Chemical Society 2014-12, Vol.136 (51), p.17762-17773 |
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creator | Song, Charles Kiseok Luck, Kyle A Zhou, Nanjia Zeng, Li Heitzer, Henry M Manley, Eric F Goldman, Samuel Chen, Lin X Ratner, Mark A Bedzyk, Michael J Chang, Robert P. H Hersam, Mark C Marks, Tobin J |
description | To achieve densely packed charge-selective organosilane-based interfacial layers (IFLs) on the tin-doped indium oxide (ITO) anodes of organic photovoltaic (OPV) cells, a series of Ar2N-(CH2) n -SiCl3 precursors with Ar = 3,4-difluorophenyl, n = 3, 6, 10, and 18, was synthesized, characterized, and chemisorbed on OPV anodes to serve as IFLs. To minimize lateral nonbonded -NAr2···Ar2N- repulsions which likely limit IFL packing densities in the resulting self-assembled monolayers (SAMs), precursor mixtures having both small and large n values are simultaneously deposited. These “heterogeneous” SAMs are characterized by a battery of techniques: contact angle measurements, X-ray reflectivity, X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy (UPS), cyclic voltammetry, and DFT computation. It is found that the headgroup densities of these “supersaturated” heterogeneous SAMs (SHSAMs) are enhanced by as much as 17% versus their homogeneous counterparts. Supersaturation significantly modifies the IFL properties including the work function (as much as 16%) and areal dipole moment (as much as 49%). Bulk-heterojunction OPV devices are fabricated with these SHSAMs: ITO/IFL/poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b′]dithiophene-2,6-diyl][2-[[(2-ethylhexyl)oxy]carbonyl]-3-fluorothieno[3,4-b]thiophenediyl]]:phenyl-C71-butyric acid methyl ester (PTB7:PC71BM)/LiF/Al. OPVs having SHSAM IFLs exhibit significantly enhanced performance (PCE by 54%; V oc by 35%) due to enhanced charge selectivity and collection, with the PCE rivaling or exceeding that of PEDOT:PSS IFL devices −7.62%. The mechanism underlying the enhanced performance involves modified hole collection and selectivity efficiency inferred from the UPS data. The ITO/SAM/SHSAM surface potential imposed by the dipolar SAMs causes band bending and favorably alters the Schottky barrier height. Thus, interfacial charge selectivity and collection are enhanced as evident in the greater OPV V oc. |
doi_str_mv | 10.1021/ja508453n |
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H ; Hersam, Mark C ; Marks, Tobin J</creator><creatorcontrib>Song, Charles Kiseok ; Luck, Kyle A ; Zhou, Nanjia ; Zeng, Li ; Heitzer, Henry M ; Manley, Eric F ; Goldman, Samuel ; Chen, Lin X ; Ratner, Mark A ; Bedzyk, Michael J ; Chang, Robert P. H ; Hersam, Mark C ; Marks, Tobin J ; Argonne National Laboratory (ANL), Argonne, IL (United States) ; Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research (ANSER)</creatorcontrib><description>To achieve densely packed charge-selective organosilane-based interfacial layers (IFLs) on the tin-doped indium oxide (ITO) anodes of organic photovoltaic (OPV) cells, a series of Ar2N-(CH2) n -SiCl3 precursors with Ar = 3,4-difluorophenyl, n = 3, 6, 10, and 18, was synthesized, characterized, and chemisorbed on OPV anodes to serve as IFLs. To minimize lateral nonbonded -NAr2···Ar2N- repulsions which likely limit IFL packing densities in the resulting self-assembled monolayers (SAMs), precursor mixtures having both small and large n values are simultaneously deposited. These “heterogeneous” SAMs are characterized by a battery of techniques: contact angle measurements, X-ray reflectivity, X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy (UPS), cyclic voltammetry, and DFT computation. It is found that the headgroup densities of these “supersaturated” heterogeneous SAMs (SHSAMs) are enhanced by as much as 17% versus their homogeneous counterparts. Supersaturation significantly modifies the IFL properties including the work function (as much as 16%) and areal dipole moment (as much as 49%). Bulk-heterojunction OPV devices are fabricated with these SHSAMs: ITO/IFL/poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b′]dithiophene-2,6-diyl][2-[[(2-ethylhexyl)oxy]carbonyl]-3-fluorothieno[3,4-b]thiophenediyl]]:phenyl-C71-butyric acid methyl ester (PTB7:PC71BM)/LiF/Al. OPVs having SHSAM IFLs exhibit significantly enhanced performance (PCE by 54%; V oc by 35%) due to enhanced charge selectivity and collection, with the PCE rivaling or exceeding that of PEDOT:PSS IFL devices −7.62%. The mechanism underlying the enhanced performance involves modified hole collection and selectivity efficiency inferred from the UPS data. The ITO/SAM/SHSAM surface potential imposed by the dipolar SAMs causes band bending and favorably alters the Schottky barrier height. 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H</creatorcontrib><creatorcontrib>Hersam, Mark C</creatorcontrib><creatorcontrib>Marks, Tobin J</creatorcontrib><creatorcontrib>Argonne National Laboratory (ANL), Argonne, IL (United States)</creatorcontrib><creatorcontrib>Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research (ANSER)</creatorcontrib><title>“Supersaturated” Self-Assembled Charge-Selective Interfacial Layers for Organic Solar Cells</title><title>Journal of the American Chemical Society</title><addtitle>J. Am. Chem. Soc</addtitle><description>To achieve densely packed charge-selective organosilane-based interfacial layers (IFLs) on the tin-doped indium oxide (ITO) anodes of organic photovoltaic (OPV) cells, a series of Ar2N-(CH2) n -SiCl3 precursors with Ar = 3,4-difluorophenyl, n = 3, 6, 10, and 18, was synthesized, characterized, and chemisorbed on OPV anodes to serve as IFLs. To minimize lateral nonbonded -NAr2···Ar2N- repulsions which likely limit IFL packing densities in the resulting self-assembled monolayers (SAMs), precursor mixtures having both small and large n values are simultaneously deposited. These “heterogeneous” SAMs are characterized by a battery of techniques: contact angle measurements, X-ray reflectivity, X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy (UPS), cyclic voltammetry, and DFT computation. It is found that the headgroup densities of these “supersaturated” heterogeneous SAMs (SHSAMs) are enhanced by as much as 17% versus their homogeneous counterparts. Supersaturation significantly modifies the IFL properties including the work function (as much as 16%) and areal dipole moment (as much as 49%). Bulk-heterojunction OPV devices are fabricated with these SHSAMs: ITO/IFL/poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b′]dithiophene-2,6-diyl][2-[[(2-ethylhexyl)oxy]carbonyl]-3-fluorothieno[3,4-b]thiophenediyl]]:phenyl-C71-butyric acid methyl ester (PTB7:PC71BM)/LiF/Al. OPVs having SHSAM IFLs exhibit significantly enhanced performance (PCE by 54%; V oc by 35%) due to enhanced charge selectivity and collection, with the PCE rivaling or exceeding that of PEDOT:PSS IFL devices −7.62%. The mechanism underlying the enhanced performance involves modified hole collection and selectivity efficiency inferred from the UPS data. The ITO/SAM/SHSAM surface potential imposed by the dipolar SAMs causes band bending and favorably alters the Schottky barrier height. Thus, interfacial charge selectivity and collection are enhanced as evident in the greater OPV V oc.</description><subject>INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY</subject><subject>SOLAR ENERGY</subject><issn>0002-7863</issn><issn>1520-5126</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2014</creationdate><recordtype>article</recordtype><recordid>eNptkMtKA0EQRRtRND4W_oAMgqCL0eqentcyBB-BgIvouqnuVMcJk5nYPSNklw_Rn_NLbIm6clXcqlOXy2XslMM1B8FvFphCIdOk2WEDngqIUy6yXTYAABHnRZYcsEPvF0FKUfB9diBSKYKQA6Y-N-_TfkXOY9c77Gj2ufmIplTbeOg9LXVNs2j0gm5OcdiS6ao3isZNR86iqbCOJrgO35FtXfTo5thUJpq2NbpoRHXtj9mexdrTyc88Ys93t0-jh3jyeD8eDScxSi67uNBaW2NlTogSyyw3UIocLMlc2mIGtqQSMi01FDpPCVKSJEtTaixSHq7JETvf-ra-q5Q3VUfmxbRNExIrnuRJKZIAXW6hlWtfe_KdWlbehJjYUNt7xTMJsuASIKBXW9S41ntHVq1ctUS3VhzUd-nqr_TAnv3Y9npJsz_yt-UAXGwBNF4t2t41oYp_jL4AKMiKIw</recordid><startdate>20141224</startdate><enddate>20141224</enddate><creator>Song, Charles Kiseok</creator><creator>Luck, Kyle A</creator><creator>Zhou, Nanjia</creator><creator>Zeng, Li</creator><creator>Heitzer, Henry M</creator><creator>Manley, Eric F</creator><creator>Goldman, Samuel</creator><creator>Chen, Lin X</creator><creator>Ratner, Mark A</creator><creator>Bedzyk, Michael J</creator><creator>Chang, Robert P. 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H</creatorcontrib><creatorcontrib>Hersam, Mark C</creatorcontrib><creatorcontrib>Marks, Tobin J</creatorcontrib><creatorcontrib>Argonne National Laboratory (ANL), Argonne, IL (United States)</creatorcontrib><creatorcontrib>Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research (ANSER)</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><collection>OSTI.GOV - Hybrid</collection><collection>OSTI.GOV</collection><jtitle>Journal of the American Chemical Society</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Song, Charles Kiseok</au><au>Luck, Kyle A</au><au>Zhou, Nanjia</au><au>Zeng, Li</au><au>Heitzer, Henry M</au><au>Manley, Eric F</au><au>Goldman, Samuel</au><au>Chen, Lin X</au><au>Ratner, Mark A</au><au>Bedzyk, Michael J</au><au>Chang, Robert P. H</au><au>Hersam, Mark C</au><au>Marks, Tobin J</au><aucorp>Argonne National Laboratory (ANL), Argonne, IL (United States)</aucorp><aucorp>Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research (ANSER)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>“Supersaturated” Self-Assembled Charge-Selective Interfacial Layers for Organic Solar Cells</atitle><jtitle>Journal of the American Chemical Society</jtitle><addtitle>J. Am. Chem. Soc</addtitle><date>2014-12-24</date><risdate>2014</risdate><volume>136</volume><issue>51</issue><spage>17762</spage><epage>17773</epage><pages>17762-17773</pages><issn>0002-7863</issn><eissn>1520-5126</eissn><abstract>To achieve densely packed charge-selective organosilane-based interfacial layers (IFLs) on the tin-doped indium oxide (ITO) anodes of organic photovoltaic (OPV) cells, a series of Ar2N-(CH2) n -SiCl3 precursors with Ar = 3,4-difluorophenyl, n = 3, 6, 10, and 18, was synthesized, characterized, and chemisorbed on OPV anodes to serve as IFLs. To minimize lateral nonbonded -NAr2···Ar2N- repulsions which likely limit IFL packing densities in the resulting self-assembled monolayers (SAMs), precursor mixtures having both small and large n values are simultaneously deposited. These “heterogeneous” SAMs are characterized by a battery of techniques: contact angle measurements, X-ray reflectivity, X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy (UPS), cyclic voltammetry, and DFT computation. It is found that the headgroup densities of these “supersaturated” heterogeneous SAMs (SHSAMs) are enhanced by as much as 17% versus their homogeneous counterparts. Supersaturation significantly modifies the IFL properties including the work function (as much as 16%) and areal dipole moment (as much as 49%). Bulk-heterojunction OPV devices are fabricated with these SHSAMs: ITO/IFL/poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b′]dithiophene-2,6-diyl][2-[[(2-ethylhexyl)oxy]carbonyl]-3-fluorothieno[3,4-b]thiophenediyl]]:phenyl-C71-butyric acid methyl ester (PTB7:PC71BM)/LiF/Al. OPVs having SHSAM IFLs exhibit significantly enhanced performance (PCE by 54%; V oc by 35%) due to enhanced charge selectivity and collection, with the PCE rivaling or exceeding that of PEDOT:PSS IFL devices −7.62%. The mechanism underlying the enhanced performance involves modified hole collection and selectivity efficiency inferred from the UPS data. The ITO/SAM/SHSAM surface potential imposed by the dipolar SAMs causes band bending and favorably alters the Schottky barrier height. Thus, interfacial charge selectivity and collection are enhanced as evident in the greater OPV V oc.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>25420044</pmid><doi>10.1021/ja508453n</doi><tpages>12</tpages><oa>free_for_read</oa></addata></record> |
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title | “Supersaturated” Self-Assembled Charge-Selective Interfacial Layers for Organic Solar Cells |
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