{"id":357,"date":"2021-09-02T12:00:00","date_gmt":"2021-09-02T16:00:00","guid":{"rendered":"https:\/\/sciences.ucf.edu\/physics\/rahman-group\/?p=357"},"modified":"2024-05-02T14:15:36","modified_gmt":"2024-05-02T18:15:36","slug":"gakiya-teruya-et-al-2021","status":"publish","type":"post","link":"https:\/\/sciences.ucf.edu\/physics\/rahman-group\/gakiya-teruya-et-al-2021\/","title":{"rendered":"Asymmetric\u00a0Design\u00a0of\u00a0Spin-Crossover\u00a0Complexes\u00a0to\u00a0Increase\u00a0the\u00a0Volatility\u00a0for\u00a0Surface\u00a0Deposition"},"content":{"rendered":"\n<p><\/p>\n\n\n<div class=\"wp-block-image\">\n<figure class=\"aligncenter size-full is-resized\"><img decoding=\"async\" width=\"999\" height=\"541\" data-src=\"https:\/\/sciences.ucf.edu\/physics\/rahman-group\/wp-content\/uploads\/sites\/40\/2024\/05\/images_large_ja1c04598_0008.jpeg\" alt=\"\" class=\"wp-image-358 lazyload\" style=\"--smush-placeholder-width: 999px; --smush-placeholder-aspect-ratio: 999\/541;width:auto;height:300px\" data-srcset=\"https:\/\/sciences.ucf.edu\/physics\/rahman-group\/wp-content\/uploads\/sites\/40\/2024\/05\/images_large_ja1c04598_0008.jpeg 999w, https:\/\/sciences.ucf.edu\/physics\/rahman-group\/wp-content\/uploads\/sites\/40\/2024\/05\/images_large_ja1c04598_0008-300x162.jpeg 300w, https:\/\/sciences.ucf.edu\/physics\/rahman-group\/wp-content\/uploads\/sites\/40\/2024\/05\/images_large_ja1c04598_0008-768x416.jpeg 768w\" data-sizes=\"(max-width: 999px) 100vw, 999px\" src=\"data:image\/svg+xml;base64,PHN2ZyB3aWR0aD0iMSIgaGVpZ2h0PSIxIiB4bWxucz0iaHR0cDovL3d3dy53My5vcmcvMjAwMC9zdmciPjwvc3ZnPg==\" \/><\/figure>\n<\/div>\n\n\n<p><\/p>\n\n\n\n<p>A mononuclear complex [Fe(<em>t<\/em>Bu<sub>2<\/sub>qsal)<sub>2<\/sub>] has been obtained by a reaction between an Fe(II) precursor salt and a tridentate ligand 2,4-di(<em>tert<\/em>-butyl)-6-((quinoline-8-ylimino)methyl)phenol (<em>t<\/em>Bu<sub>2<\/sub>qsalH) in the presence of triethylamine. The complex exhibits a hysteretic spin transition at 117 K upon cooling and 129 K upon warming, as well as light-induced excited spin-state trapping at lower temperatures. Although the strongly cooperative spin transition suggests substantial intermolecular interactions, the complex is readily sublimable, as evidenced by the growth of its single crystals by sublimation at 573 \u2192 373 K and \u223c10<sup>\u20133<\/sup>\u00a0mbar. This seemingly antagonistic behavior is explained by the asymmetric coordination environment, in which the\u00a0<em>t<\/em>Bu substituents and quinoline moieties appear on opposite sides of the complex. As a result, the structure is partitioned in well-defined layers separated by van der Waals interactions between the\u00a0<em>t<\/em>Bu groups, while the efficient cooperative interactions within the layer are provided by the quinoline-based moieties. The abrupt spin transition is preserved in a 20 nm thin film prepared by sublimation, as evidenced by abrupt and hysteretic changes in the dielectric properties in the temperature range comparable to the one around which the spin transition is observed for the bulk material. The changes in the dielectric response are in excellent agreement with differences in the dielectric tensor of the low-spin and high-spin crystal structures evaluated by density functional theory calculations. The substantially higher volatility of [Fe(<em>t<\/em>Bu<sub>2<\/sub>qsal)<sub>2<\/sub>], as compared to a similar complex without\u00a0<em>t<\/em>Bu substituents, suggests that asymmetric molecular shapes offer an efficient design strategy to achieve sublimable complexes with strongly cooperative spin transitions.<br><br>This work was published in Journal\u00a0of\u00a0the\u00a0American\u00a0Chemical\u00a0Society.<br>[M.\u00a0Gakiya-Teruya,\u00a0X.\u00a0Jiang,\u00a0D.\u00a0Le,\u00a0\u00d6.\u00a0\u00dcng\u00f6r,\u00a0A. J.\u00a0Durrani,\u00a0J. J.\u00a0Koptur-Palenchar,\u00a0J.\u00a0Jiang,\u00a0T.\u00a0Jiang,\u00a0M. W.\u00a0Meisel,\u00a0H.-P.\u00a0Cheng,\u00a0X.-G.\u00a0Zhang,\u00a0X.-X.\u00a0Zhang,\u00a0<strong>T. S.\u00a0Rahman<\/strong>,\u00a0A. F.\u00a0Hebard,\u00a0and\u00a0M.\u00a0Shatruk,\u00a0&#8220;Asymmetric\u00a0Design\u00a0of\u00a0Spin-Crossover\u00a0Complexes\u00a0to\u00a0Increase\u00a0the\u00a0Volatility\u00a0for\u00a0Surface\u00a0Deposition,&#8221;\u00a0Journal\u00a0of\u00a0the\u00a0American\u00a0Chemical\u00a0Society\u00a0143,\u00a014563-14572\u00a0(2021).\u00a0<a href=\"https:\/\/doi.org\/10.1021\/jacs.1c04598\">https:\/\/doi.org\/10.1021\/jacs.1c04598<\/a>]<\/p>\n","protected":false},"excerpt":{"rendered":"<p>A mononuclear complex [Fe(tBu2qsal)2] has been obtained by a reaction between an Fe(II) precursor salt and a tridentate ligand 2,4-di(tert-butyl)-6-((quinoline-8-ylimino)methyl)phenol (tBu2qsalH) in the presence of triethylamine. The complex exhibits a hysteretic spin transition at 117 K upon cooling and 129 K upon warming, as well as light-induced excited spin-state trapping at lower temperatures. Although the &#8230; <a title=\"Asymmetric\u00a0Design\u00a0of\u00a0Spin-Crossover\u00a0Complexes\u00a0to\u00a0Increase\u00a0the\u00a0Volatility\u00a0for\u00a0Surface\u00a0Deposition\" class=\"read-more\" href=\"https:\/\/sciences.ucf.edu\/physics\/rahman-group\/gakiya-teruya-et-al-2021\/\" aria-label=\"Read more about Asymmetric\u00a0Design\u00a0of\u00a0Spin-Crossover\u00a0Complexes\u00a0to\u00a0Increase\u00a0the\u00a0Volatility\u00a0for\u00a0Surface\u00a0Deposition\">Read more<\/a><\/p>\n","protected":false},"author":92,"featured_media":0,"comment_status":"off","ping_status":"off","sticky":false,"template":"","format":"standard","meta":{"footnotes":"","_links_to":"","_links_to_target":""},"categories":[4],"tags":[],"class_list":["post-357","post","type-post","status-publish","format-standard","hentry","category-home-slider"],"yoast_head":"<!-- This site is optimized with the Yoast SEO plugin v27.2 - https:\/\/yoast.com\/product\/yoast-seo-wordpress\/ -->\n<title>Asymmetric\u00a0Design\u00a0of\u00a0Spin-Crossover\u00a0Complexes\u00a0to\u00a0Increase\u00a0the\u00a0Volatility\u00a0for\u00a0Surface\u00a0Deposition - Professor Talat S. Rahman<\/title>\n<meta name=\"robots\" content=\"index, follow, max-snippet:-1, max-image-preview:large, max-video-preview:-1\" \/>\n<link rel=\"canonical\" href=\"https:\/\/sciences.ucf.edu\/physics\/rahman-group\/gakiya-teruya-et-al-2021\/\" \/>\n<meta property=\"og:locale\" content=\"en_US\" \/>\n<meta property=\"og:type\" content=\"article\" \/>\n<meta property=\"og:title\" content=\"Asymmetric\u00a0Design\u00a0of\u00a0Spin-Crossover\u00a0Complexes\u00a0to\u00a0Increase\u00a0the\u00a0Volatility\u00a0for\u00a0Surface\u00a0Deposition - Professor Talat S. Rahman\" \/>\n<meta property=\"og:description\" content=\"A mononuclear complex [Fe(tBu2qsal)2] has been obtained by a reaction between an Fe(II) precursor salt and a tridentate ligand 2,4-di(tert-butyl)-6-((quinoline-8-ylimino)methyl)phenol (tBu2qsalH) in the presence of triethylamine. 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