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The outcomes presented in this work, obtained with ab initio<\/jats:italic> methods of exceptional predictive capabilities, offer strong evidences that sizable hyperpolarizability contrasts between neutral and charged alkali metal doped cluster forms might be simultaneously accomplished. The observed switching procedure involves redox polyatomic clusters formed by Si atoms. These centers function as electron acceptors at the ground state and as electron donors at the excited states facilitating low energy charge transfer transitions upon electronic excitation. \u00a9 2014 Wiley Periodicals, Inc.<\/jats:p>","DOI":"10.1002\/jcc.23549","type":"journal-article","created":{"date-parts":[[2014,2,12]],"date-time":"2014-02-12T12:30:19Z","timestamp":1392208219000},"page":"829-838","source":"Crossref","is-referenced-by-count":12,"title":["Significant nonlinear\u2010optical switching capacity in atomic clusters built from silicon and lithium: A combined ab initio<\/i> and density functional study"],"prefix":"10.1002","volume":"35","author":[{"given":"Panaghiotis","family":"Karamanis","sequence":"first","affiliation":[{"name":"Equipe de Chimie Physique IPREM Institut des Sciences Analytiques et de Physico\u2010chimie pour l'Environnement et les Mat\u00e9riaux (IPREM) UMR 5254. 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