Paraquinoid rings are introduced in the pi-conjugation of all-organic donor-pi-acceptor dyes as sensitizer in dye sensitized solar cells, to drastically shift optical response from violet-blue to near-infrared and to significantly enhance photoabsorption. Taking Y1 as a model, real time electron dynamics simulations based on time-dependent density functional theory confirm that paraquinoid conjugation maintains high thermal stability and ultrafast electron-hole separation at ambient temperature. (C) 2013 Elsevier B.V. All rights reserved.