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The molecular structure of compound <jats:bold>1\u2009a<\/jats:bold>, determined by X\u2010ray diffraction, showed that the local geometry around the metal center is a distorted octahedral with meridional coordination of the ligands. The structural parameters, spectroscopic data, and density functional theory (DFT) calculations on representative complex <jats:bold>1\u2009a<\/jats:bold> suggest that ligand L<jats:sup>a<\/jats:sup> is predominantly an azo\u2010anion\u2010radical\u2010type, and so the complex can be represented as [Cr<jats:sup>III<\/jats:sup>(L<jats:sup>a.\u2212<\/jats:sup>)<jats:sub>3<\/jats:sub>]. An assessment of their physicochemical and surface properties was performed with the aim of using these triple\u2010tailed metallosurfactants as precursors for redox\u2010responsive films. The surface\u2010pressure\u2013molecular\u2010area isotherm measurement for compound <jats:bold>1\u2009d<\/jats:bold> shows that the complex forms a stable Langmuir film at the air\/water interface. The monolayer and multilayers were successfully transferred onto the quartz substrate and the platinum working electrode at a surface pressure of 10\u2005mN\u2009m<jats:sup>\u22121<\/jats:sup> by the Langmuir\u2013Schaefer (LS) technique. The LS films were studied by UV\/Vis spectrometry, infrared spectroscopy, field\u2010emission scanning electron microscopy, and atomic force microscopy. A good linear relationship between the absorbance at 370\u2005nm and the thickness of the layers against the number of deposited layers indicated the uniformity and reproducibility of this transfer process. Voltammograms for platinum\u2010surface\u2010bound LS film of compound <jats:bold>1\u2009d<\/jats:bold> showed that the redox response owing to the first oxidation is stable and reproducible after many cycles (&gt;300 cycles). Spectroscopic studies and electrochemical measurements of compound <jats:bold>1\u2009d<\/jats:bold> on the LS films revealed that these complexes are potential candidates for molecular devices.<\/jats:p>","DOI":"10.1002\/chem.201102765","type":"journal-article","created":{"date-parts":[[2012,1,11]],"date-time":"2012-01-11T12:36:57Z","timestamp":1326285417000},"page":"1761-1771","source":"Crossref","is-referenced-by-count":18,"title":["Synthesis of Amphiphilic Azo\u2010Anion\u2010Radical Complexes of Chromium(III) and the Development of Ultrathin Redox\u2010Active Surfaces by the Langmuir\u2013Schaefer Technique"],"prefix":"10.1002","volume":"18","author":[{"given":"Sucheta","family":"Joy","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Prabir","family":"Pal","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tapan Kumar","family":"Mondal","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"G. 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