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However, conventional spectroelectrochemistry (SEC) may yield results that deviate from practical device operation because it typically relies on gradual potential scans. Here, we investigate mixed-phase and pure wurtzite CdSe\/CdS core\/shell nanocrystals using potentiostatic polarization SEC. Mixed-phase nanocrystals exhibit spectral recovery under both biases, originating from self-elimination of excess electrons (negative bias) and photo-assisted elimination of trap states, whose rapid charging\/discharging induces local electric field fluctuations that cause asymmetric spectral broadening (positive bias). In contrast, pure wurtzite nanocrystals allow additional hole injection, causing a reversible spectral blueshift. Under negative bias, they exhibit slow photoluminescence quenching and redshift from gradual electron injection. These differences stem from the lack of conduction band intermediate levels and a valence band barrier due to zinc blende stacking faults, suggesting microstructural engineering may enable balanced carrier injection.<\/jats:p>","DOI":"10.1021\/acs.jpclett.6c02515","type":"journal-article","created":{"date-parts":[[2026,9,30]],"date-time":"2026-09-30T03:02:18Z","timestamp":1790737338000},"page":"11869-11877","source":"Crossref","is-referenced-by-count":0,"title":["Decoupling Electron\nand Hole Injection Dynamics in\nColloidal Nanocrystals via Potentiostatic Polarization Spectroelectrochemistry"],"prefix":"10.1021","volume":"17","author":[{"given":"Junkai","family":"Wang","sequence":"first","affiliation":[{"name":"Hangzhou Dianzi University , , , ,","place":["Hangzhou, China, 310018"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2779-5419","authenticated-orcid":true,"given":"Huichao","family":"Zhang","sequence":"additional","affiliation":[{"name":"Hangzhou Dianzi University , , , ,","place":["Hangzhou, China, 310018"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bo","family":"Huang","sequence":"additional","affiliation":[{"name":"Hangzhou Dianzi University , , , ,","place":["Hangzhou, China, 310018"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chenyu","family":"Du","sequence":"additional","affiliation":[{"name":"Hangzhou Dianzi University , , , ,","place":["Hangzhou, China, 310018"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shiji","family":"Chen","sequence":"additional","affiliation":[{"name":"Hangzhou Dianzi University , , , ,","place":["Hangzhou, China, 310018"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,29]]},"reference":[{"issue":"6555","key":"2026101508221250600_cit1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aaz8541","article-title":"Semiconductor Quantum Dots: Technological\nProgress and Future Challenges","volume":"373","author":"de Arquer","year":"2021","journal-title":"Science"},{"issue":"6","key":"2026101508221250600_cit2","doi-asserted-by":"publisher","first-page":"412","DOI":"10.1038\/s44287-024-00059-0","article-title":"Advances in Understanding Quantum\nDot Light-Emitting Diodes","volume":"1","author":"Li","year":"2024","journal-title":"Nat. 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Nanotechnol."},{"issue":"8","key":"2026101508221250600_cit6","doi-asserted-by":"publisher","first-page":"548","DOI":"10.1038\/s41928-021-00632-7","article-title":"Colloidal Quantum Dot Electronics","volume":"4","author":"Liu","year":"2021","journal-title":"Nat. Electron."},{"issue":"8","key":"2026101508221250600_cit7","doi-asserted-by":"publisher","first-page":"4663","DOI":"10.1021\/acs.chemrev.2c00695","article-title":"Review: Quantum Dot\nLight-Emitting Diodes","volume":"123","author":"Jang","year":"2023","journal-title":"Chem. Rev."},{"issue":"7","key":"2026101508221250600_cit8","doi-asserted-by":"publisher","first-page":"1777","DOI":"10.1021\/acs.jpclett.3c00070","article-title":"Quantitative\nDetermination of Charge Accumulation and\nRecombination in Operational Quantum Dots Light Emitting Diodes via\nTime-Resolved Electroluminescence Spectroscopy","volume":"14","author":"Bao","year":"2023","journal-title":"J. Phys. Chem. 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Mater."},{"issue":"33","key":"2026101508221250600_cit15","doi-asserted-by":"publisher","first-page":"14001","DOI":"10.1039\/D0NR09189H","article-title":"Evidence of Band Filling in PbS Colloidal Quantum Dot Square Superstructures","volume":"13","author":"Liu","year":"2021","journal-title":"Nanoscale"},{"issue":"1","key":"2026101508221250600_cit16","doi-asserted-by":"publisher","first-page":"377","DOI":"10.1021\/acsnano.0c07365","article-title":"Quantitative Electrochemical\nControl over Optical Gain in Quantum-Dot Solids","volume":"15","author":"Geuchies","year":"2021","journal-title":"ACS Nano"},{"issue":"7","key":"2026101508221250600_cit17","doi-asserted-by":"publisher","first-page":"2519","DOI":"10.1021\/acsenergylett.1c00970","article-title":"Electrochemical\nP-Doping of CsPbBr3 Perovskite Nanocrystals","volume":"6","author":"Mulder","year":"2021","journal-title":"ACS Energy Lett."},{"issue":"4","key":"2026101508221250600_cit18","doi-asserted-by":"publisher","first-page":"1353","DOI":"10.1021\/acs.chemmater.0c04416","article-title":"Spectroelectrochemistry\nof Colloidal CdSe Quantum Dots","volume":"33","author":"Ashokan","year":"2021","journal-title":"Chem. 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Adv."},{"issue":"7372","key":"2026101508221250600_cit26","doi-asserted-by":"publisher","first-page":"203","DOI":"10.1038\/nature10569","article-title":"Two Types\nof Luminescence Blinking\nRevealed by Spectroelectrochemistry of Single Quantum Dots","volume":"479","author":"Galland","year":"2011","journal-title":"Nature"},{"issue":"5","key":"2026101508221250600_cit27","doi-asserted-by":"publisher","first-page":"200","DOI":"10.1364\/PRJ.3.000200","article-title":"Laser-Annealing-Made\nAmplified Spontaneous Emission\nof \u201cGiant\u201d CdSe\/CdS Core\/Shell Nanocrystals Transferred\nfrom Bulk-like Shell to Quantum-Confined Core","volume":"3","author":"Liao","year":"2015","journal-title":"Photonics Res."},{"issue":"7","key":"2026101508221250600_cit28","doi-asserted-by":"publisher","first-page":"3855","DOI":"10.1021\/nl501026r","article-title":"Electrochemical\nControl of Two-Color Emission from Colloidal Dot-in-Bulk Nanocrystals","volume":"14","author":"Brovelli","year":"2014","journal-title":"Nano Lett."},{"issue":"9","key":"2026101508221250600_cit29","doi-asserted-by":"publisher","first-page":"9011","DOI":"10.1021\/acsnano.8b02493","article-title":"The Impact of Core\/Shell\nSizes on the Optical Gain Characteristics of CdSe\/CdS Quantum Dots","volume":"12","author":"Bisschop","year":"2018","journal-title":"ACS Nano"},{"issue":"3","key":"2026101508221250600_cit30","doi-asserted-by":"publisher","first-page":"399","DOI":"10.1021\/acs.jpclett.8b03211","article-title":"Giant-Shell CdSe\/CdS\nNanocrystals: Exciton Coupling to Shell Phonons Investigated by Resonant\nRaman Spectroscopy","volume":"10","author":"Lin","year":"2019","journal-title":"J. Phys. Chem. Lett."},{"issue":"26","key":"2026101508221250600_cit31","doi-asserted-by":"publisher","first-page":"12619","DOI":"10.1039\/C9NR03061A","article-title":"Quantum-Confined\nStark Effect in the Ensemble of Phase-Pure CdSe\/CdS Quantum Dots","volume":"11","author":"Zhang","year":"2019","journal-title":"Nanoscale"},{"issue":"11","key":"2026101508221250600_cit32","doi-asserted-by":"publisher","first-page":"10013","DOI":"10.1021\/nn303719m","article-title":"Single Molecule\nQuantum-Confined Stark Effect Measurements of Semiconductor Nanoparticles\nat Room Temperature","volume":"6","author":"Park","year":"2012","journal-title":"ACS Nano"},{"issue":"22","key":"2026101508221250600_cit33","doi-asserted-by":"publisher","first-page":"3946","DOI":"10.1063\/1.1580632","article-title":"Single-Electron Charging\nof a Self-Assembled II\u2013VI\nQuantum Dot","volume":"82","author":"Seufert","year":"2003","journal-title":"Appl. Phys. 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Lett."},{"issue":"24","key":"2026101508221250600_cit37","doi-asserted-by":"publisher","first-page":"4968","DOI":"10.1021\/acs.jpclett.6b02465","article-title":"Ultralow-Threshold\nSingle-Mode Lasing from Phase-Pure CdSe\/CdS Core\/Shell Quantum Dots","volume":"7","author":"Liao","year":"2016","journal-title":"J. Phys. Chem. Lett."},{"issue":"5","key":"2026101508221250600_cit38","doi-asserted-by":"publisher","first-page":"445","DOI":"10.1038\/nmat3539","article-title":"Compact High-Quality\nCdSe\u2013CdS\nCore\u2013Shell Nanocrystals with Narrow Emission Linewidths and\nSuppressed Blinking","volume":"12","author":"Chen","year":"2013","journal-title":"Nat. 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