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This technique relies on applying an electric field of approximately 0.4\u20131 V nm<jats:sup>\u22121<\/jats:sup> across the membrane to induce a current, and eventually, breakdown of the dielectric. Although previous studies have performed controlled breakdown under a range of different conditions, the mechanism of conduction and breakdown has not been fully explored. Here, electrical conduction and nanopore formation in SiN<jats:sub><jats:italic>x<\/jats:italic><\/jats:sub> membranes during controlled breakdown is studied. It is demonstrated that for Si\u2010rich SiN<jats:sub><jats:italic>x<\/jats:italic><\/jats:sub>, oxidation reactions that occur at the membrane\u2010electrolyte interface limit conduction across the dielectric. However, for stoichiometric Si<jats:sub>3<\/jats:sub>N<jats:sub>4<\/jats:sub> the effect of oxidation reactions becomes relatively small and conduction is predominately limited by charge transport across the dielectric. Several important implications resulting from understanding this process are provided which will aid in further developing controlled breakdown in the coming years, particularly for extending this technique to integrate nanopores with on\u2010chip nanostructures.<\/jats:p>","DOI":"10.1002\/smll.202102543","type":"journal-article","created":{"date-parts":[[2021,8,2]],"date-time":"2021-08-02T04:07:49Z","timestamp":1627877269000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Understanding Electrical Conduction and Nanopore Formation During Controlled Breakdown"],"prefix":"10.1002","volume":"17","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-5369-6863","authenticated-orcid":false,"given":"Jasper P.","family":"Fried","sequence":"first","affiliation":[{"name":"Department of Materials University of Oxford  Oxford OX1 3PH UK"}]},{"given":"Jacob L.","family":"Swett","sequence":"additional","affiliation":[{"name":"Department of Materials University of Oxford  Oxford OX1 3PH UK"}]},{"given":"Binoy Paulose","family":"Nadappuram","sequence":"additional","affiliation":[{"name":"Department of Chemistry Imperial College London  London W12 0BZ UK"}]},{"given":"Aleksandra","family":"Fedosyuk","sequence":"additional","affiliation":[{"name":"Department of Chemistry Imperial College London  London W12 0BZ UK"}]},{"given":"Pedro Miguel","family":"Sousa","sequence":"additional","affiliation":[{"name":"Instituto de Tecnologia Qu\u00edmica e Biol\u00f3gica Ant\u00f3nio Xavier Universidade Nova de Lisboa  Av. da Rep\u00fablica Oeiras 2780\u2010157 Portugal"}]},{"given":"Dayrl P.","family":"Briggs","sequence":"additional","affiliation":[{"name":"Center for Nanophase Materials Sciences Oak Ridge National Laboratory  Oak Ridge TN 37830 USA"}]},{"given":"Aleksandar P.","family":"Ivanov","sequence":"additional","affiliation":[{"name":"Department of Chemistry Imperial College London  London W12 0BZ UK"}]},{"given":"Joshua B.","family":"Edel","sequence":"additional","affiliation":[{"name":"Department of Chemistry Imperial College London  London W12 0BZ UK"}]},{"given":"Jan A.","family":"Mol","sequence":"additional","affiliation":[{"name":"School of Physics and Astronomy Queen Mary University London  London E1 4NS UK"}]},{"given":"James R.","family":"Yates","sequence":"additional","affiliation":[{"name":"Instituto de Tecnologia Qu\u00edmica e Biol\u00f3gica Ant\u00f3nio Xavier Universidade Nova de Lisboa  Av. da Rep\u00fablica Oeiras 2780\u2010157 Portugal"}]}],"member":"311","published-online":{"date-parts":[[2021,8]]},"reference":[{"key":"e_1_2_8_1_1","first-page":"932","volume":"5","author":"Xue L.","year":"2020","journal-title":"Nat. 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