{"id":24035,"date":"2021-10-06T00:00:45","date_gmt":"2021-10-05T16:00:45","guid":{"rendered":"https:\/\/www.science.nus.edu.sg\/?p=24035"},"modified":"2021-10-06T10:55:07","modified_gmt":"2021-10-06T02:55:07","slug":"modelling-nonequilibrium-nanoscale-junctions-with-steady-state-density-functional-theory-dft","status":"publish","type":"post","link":"https:\/\/www.science.nus.edu.sg\/blog\/2021\/10\/modelling-nonequilibrium-nanoscale-junctions-with-steady-state-density-functional-theory-dft\/","title":{"rendered":"Modelling nonequilibrium nanoscale junctions with steady-state density functional theory (DFT)"},"content":{"rendered":"<p><span style=\"font-family: arial, helvetica, sans-serif; font-size: 16px;\">NUS scientists have predicted a new type of nonequilibrium effects that could generally exist in nanoscale electronic devices, and successfully explained a recent puzzling experiment using the effects.<\/span><\/p>\n<p><span style=\"font-family: arial, helvetica, sans-serif; font-size: 16px;\">Understanding bias-induced nonequilibrium effects on electron transport properties of nanoscale junctions is the central issue in computational nanoscience. The standard density functional theory (DFT)-based first-principles method that combines DFT and nonequilibrium Green\u2019s functions\u2019 techniques has been widely used in modelling nonequilibrium nanoscale devices. This provides qualitative understanding of experiments by relating the measured conductance to tunnelling of electrons through \u201cmolecular\u201d orbitals of the devices.<\/span><\/p>\n<p><span style=\"font-family: arial, helvetica, sans-serif; font-size: 16px;\">A recent experiment, however, reported surprising transport phenomena through silane junctions that cannot be understood by the standard DFT method. The conductance for various silane molecules connected with two different linker groups (amine or thiol) to either gold (Au) or silver (Ag) metal electrodes were measured. It was found that, when using the amine linker, the Au electrode generates a much higher conductance when compared to an Ag electrode. With the thiol linker, this trend reverses and the Ag electrode is significantly more conducting than the Au electrode. In contrast, DFT-based calculations predict that the Au electrode is always more conducting than the Ag electrode regardless of the type of linkers. This contradiction between theoretical and experimental results presents the community of computational nanoscience with an exciting challenge.<\/span><\/p>\n<p><span style=\"font-family: arial, helvetica, sans-serif; font-size: 16px;\">To address this challenge, the research group led by Prof ZHANG Chun from the Department of Physics and the Department of Chemistry, National University of Singapore, studied the theoretical transport properties of silane junctions building on the steady-state DFT technique that was proposed by Prof Zhang himself back in 2015. The steady-state DFT considers nonequilibrium effects in full by employing nonequilibrium quantum statistics. They found that underlying the puzzling experimental observations is a novel type of nonequilibrium effects (named \u201cnonequilibrium pulling\u201d in their work) that exist in silane junctions having thiol linkers. Their theoretical calculations show that, when the junction is near equilibrium, the standard DFT method is an excellent approximation of steady state conditions. However, at low biases around the region of 0.2 volts, the \u201cnonequilibrium pulling\u201d effect drives the thiol-terminated silanes far away from equilibrium, thus resulting in the reversal of conductance values observed in experiments.<\/span><\/p>\n<p><span style=\"font-family: arial, helvetica, sans-serif; font-size: 16px;\">Prof Zhang said, \u201cFurther analysis suggests that these nonequilibrium effects could generally exist in nanoscale devices in which there are conducting channels mainly residing at the source contact and located close to the bias window. These findings significantly broaden our fundamental understanding of electron transport at the nanoscale.\u201d<\/span><\/p>\n<p><img fetchpriority=\"high\" decoding=\"async\" width=\"443\" height=\"370\" src=\"https:\/\/www.science.nus.edu.sg\/wp-content\/uploads\/2021\/10\/292._ZhangC_PHY_20210928_1.jpg\" alt=\"\" class=\"alignnone size-full wp-image-24033\" srcset=\"https:\/\/www.science.nus.edu.sg\/wp-content\/uploads\/2021\/10\/292._ZhangC_PHY_20210928_1.jpg 443w, https:\/\/www.science.nus.edu.sg\/wp-content\/uploads\/2021\/10\/292._ZhangC_PHY_20210928_1-300x251.jpg 300w\" sizes=\"(max-width: 443px) 100vw, 443px\" \/><\/p>\n<p><span style=\"font-family: arial, helvetica, sans-serif; font-size: 16px;\">The figure shows the conceptual difference between steady-state DFT (used by the research team) and the standard DFT method. In steady-state DFT, the transport state is a functional of two densities, the total electron density \u03c1t and the current-carrying electron density \u03c1<sub>n<\/sub>. The standard DFT can be considered to be \u201cone-dimensional\u201d as the transport state is only determined by \u03c1<sub>t<\/sub>. The two-dimensional (2D) colour contour represents the energy of the steady-state transport state E<sub>ss<\/sub>. Steady-state DFT searches for the most stable transport state in the 2D plane (global minimum energy state) while the standard DFT does the search along \u03c1t axis (local minimum energy state). When the system is near equilibrium, \u03c1<sub>n<\/sub> is small and the search path of the steady-state DFT is close to the \u03c1<sub>t<\/sub> axis. For such cases, the standard DFT method can be a good approximation. [Credit: Nanoscale Horizons]<\/span><\/p>\n<p><strong><span style=\"font-family: arial, helvetica, sans-serif; font-size: 16px;\">Reference<\/span><\/strong><\/p>\n<p><span style=\"font-family: arial, helvetica, sans-serif; font-size: 16px;\">Jiang Z; Yam KM; Guo N; Zhang L; Shen L; Zhang C*, \u201cProminent nonequilibrium effects beyond the standard first-principles approach in nanoscale electronic devices\u201d, NANOSCALE HORIZONS Volume: 6, Page number: 801-808 DOI: 10.1039\/d1nh00293g Published: 2021.<\/span><\/p>\n<p>&nbsp;<\/p>\n","protected":false},"excerpt":{"rendered":"<p>NUS scientists have predicted a new type of nonequilibrium effects that could generally exist in nanoscale electronic devices, and successfully&#8230;<\/p>\n","protected":false},"author":16,"featured_media":24032,"comment_status":"open","ping_status":"closed","sticky":false,"template":"","format":"standard","meta":{"_acf_changed":false,"footnotes":""},"categories":[29,13],"tags":[],"class_list":["post-24035","post","type-post","status-publish","format-standard","has-post-thumbnail","hentry","category-computational-science","category-research-news"],"acf":[],"yoast_head":"<!-- This site is optimized with the Yoast SEO Premium plugin v23.6 (Yoast SEO v23.6) - https:\/\/yoast.com\/wordpress\/plugins\/seo\/ -->\n<title>Modelling nonequilibrium nanoscale junctions with steady-state density functional theory (DFT) - NUS Faculty of Science<\/title>\n<meta name=\"robots\" content=\"index, follow, max-snippet:-1, max-image-preview:large, max-video-preview:-1\" \/>\n<link rel=\"canonical\" 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