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      Elimination of Interface Energy Barriers Using Dendrimer Polyelectrolytes with Fractal Geometry

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          Abstract

          In this work we study conjugated polyelectrolyte (CPE) films based on polyamidoamine (PAMAM) dendrimers of generations G1 and G3. These fractal macromolecules are compared to branched polyethylenimine (b-PEI) polymer using methanol as the solvent. All of these materials present a high density of amino groups, which protonated by methoxide counter-anions create strong dipolar interfaces. The vacuum level shift associated to these films on n-type silicon was 0.93 eV for b-PEI, 0.72 eV for PAMAM G1 and 1.07 eV for PAMAM G3. These surface potentials were enough to overcome Fermi level pinning, which is a typical limitation of aluminium contacts on n-type silicon. A specific contact resistance as low as 20 mΩ·cm 2 was achieved with PAMAM G3, in agreement with the higher surface potential of this material. Good electron transport properties were also obtained for the other materials. Proof-of-concept silicon solar cells combining vanadium oxide as a hole-selective contact with these new electron transport layers have been fabricated and compared. The solar cell with PAMAM G3 surpassed 15% conversion efficiency with an overall increase of all the photovoltaic parameters. The performance of these devices correlates with compositional and nanostructural studies of the different CPE films. Particularly, a figure-of-merit ( V σ) for CPE films that considers the number of protonated amino groups per macromolecule has been introduced. The fractal geometry of dendrimers leads to a geometric increase in the number of amino groups per generation. Thus, investigation of dendrimer macromolecules seems a very good strategy to design CPE films with enhanced charge-carrier selectivity.

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          Theory of Surface States

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            Dendrimers: synthesis, applications, and properties

            Dendrimers are nano-sized, radially symmetric molecules with well-defined, homogeneous, and monodisperse structure that has a typically symmetric core, an inner shell, and an outer shell. Their three traditional macromolecular architectural classes are broadly recognized to generate rather polydisperse products of different molecular weights. A variety of dendrimers exist, and each has biological properties such as polyvalency, self-assembling, electrostatic interactions, chemical stability, low cytotoxicity, and solubility. These varied characteristics make dendrimers a good choice in the medical field, and this review covers their diverse applications.
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              A New Class of Polymers: Starburst-Dendritic Macromolecules

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                Author and article information

                Journal
                ACS Appl Mater Interfaces
                ACS Appl Mater Interfaces
                am
                aamick
                ACS Applied Materials & Interfaces
                American Chemical Society
                1944-8244
                1944-8252
                03 June 2023
                14 June 2023
                : 15
                : 23
                : 28705-28715
                Affiliations
                []Departament d’Enginyeria Electrònica, Universitat Politècnica de Catalunya (UPC) , Barcelona 08034, Spain
                []Departament de Física Aplicada, Universitat de Barcelona , Martí i Franquès 1, 08028 Barcelona, Spain
                [§ ]Institute of Nanoscience and Nanotechnology (IN2UB), Universitat de Barcelona , Barcelona 08028, Spain
                Author notes
                Author information
                https://orcid.org/0000-0002-1952-6614
                https://orcid.org/0000-0001-8833-9057
                https://orcid.org/0000-0002-1834-2565
                https://orcid.org/0000-0002-0320-9606
                Article
                10.1021/acsami.3c01930
                10802975
                37269290
                e887fffd-9643-463c-8846-a7f406800bb8
                © 2023 American Chemical Society

                Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained ( https://creativecommons.org/licenses/by/4.0/).

                History
                : 10 February 2023
                : 19 May 2023
                Funding
                Funded by: H2020 European Research Council, doi 10.13039/100010663;
                Award ID: 866018
                Funded by: European Regional Development Fund, doi 10.13039/501100008530;
                Award ID: NA
                Funded by: European Social Fund, doi 10.13039/501100004895;
                Award ID: 2019 FI_B 00456
                Funded by: Ministerio de Ciencia e Innovación, doi 10.13039/501100004837;
                Award ID: TED2021-131778B
                Funded by: Ministerio de Ciencia e Innovación, doi 10.13039/501100004837;
                Award ID: PID2020-116719RB-C41
                Funded by: Ministerio de Ciencia e Innovación, doi 10.13039/501100004837;
                Award ID: PID2020-115719RB-C21
                Funded by: Ministerio de Ciencia e Innovación, doi 10.13039/501100004837;
                Award ID: PID2019-109215RB-C43
                Funded by: Ministerio de Ciencia e Innovación, doi 10.13039/501100004837;
                Award ID: PID2019-109215RB-C41
                Funded by: Institució Catalana de Recerca i Estudis Avançats, doi 10.13039/501100003741;
                Award ID: NA
                Funded by: Generalitat de Catalunya, doi 10.13039/501100002809;
                Award ID: NA
                Funded by: European Commission, doi 10.13039/501100000780;
                Award ID: TED2021-131778B
                Categories
                Research Article
                Custom metadata
                am3c01930
                am3c01930

                Materials technology
                dipole,dipole film,conjugated polyelectrolytes,dendrimer,solar cells,fermi-level pinning,electronic transport

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