Jeon, Jiwon Park, Young Choon Han, Sang Soo Goddard, William A., III Lee, Yoon Sup Kim, Hyungjun 2024-01-20T08:04:45Z 2024-01-20T08:04:45Z 2021-09-04 2014-12 1948-7185 https://pubs.kist.re.kr/handle/201004/126040 During the light-harvesting process of dye-sensitized solar cells (DSSCs), the hole localized on the dye after the charge separation yields an oxidized dye, D+. The fast regeneration of D+ using the redox pair (typically the I-/I-3(-) couple) is critical for the efficient DSSCs. However, the kinetic processes of dye regeneration remain uncertain, still promoting vigorous debates. Here, we use molecular dynamics simulations to determine that the inner-sphere electron-transfer pathway provides a rapid dye regeneration route of similar to 4 ps, where penetration of I- next to D+ enables an immediate electron transfer, forming a kinetic barrier. This explains the recently reported ultrafast dye regeneration rate of a few picoseconds determined experimentally. We expect that our MD based comprehensive understanding of the dye regeneration mechanism will provide a helpful guideline in designing TiO2-dye-electrolyte interfacial systems for better performing DSSCs. English American Chemical Society Rapid Dye Regeneration Mechanism of Dye-Sensitized Solar Cells Article 10.1021/jz502197b 1 The Journal of Physical Chemistry Letters, v.5, no.24, pp.4285 - 4290 The Journal of Physical Chemistry Letters 5 24 4285 4290 N scie scopus 000346759700010 2-s2.0-84918772966 Chemistry, Physical Nanoscience & Nanotechnology Materials Science, Multidisciplinary Physics, Atomic, Molecular & Chemical Chemistry Science & Technology - Other Topics Materials Science Physics Article SPHERE ELECTRON-TRANSFER TIO2 FILMS AB-INITIO IODIDE DYNAMICS EFFICIENCY INJECTION OXIDATION COST dye regeneration dye-sensitized solar cells electron transfer multiscale simulation