Supplementary Information Multi-layering of a Nanopatterned TiO2 Layer for Highly Efficient Solid-State Solar Cells Jongbeom Na, Younghoon Kim, Chihyun Park and Eunkyoung Kim* Active Polymer Center for Pattern Integration, Department of Chemical and Biomolecular Engineering, Yonsei University, 50 Yonsei-ro, Seodaemun-gu, Seoul 120-749, South Korea E-mail: eunkim@yonsei.kr Homepage: http://web.yonsei.ac.kr/eunkim Keywords: multi-layered, nanopatterned TiO2, light harvesting, solid-state solar cells, photoanode. 1 Supplementary Figure S1. SEM image of multi-layered nanopatterned photoanodes (MNPs) with top view; (a) 2-layered nanopatterned photoanode (2NP) (scale bar: 2 μm), (b) 3-layered nanopatterned photoanode (3NP) (scale bar: 5 μm), (c) 4-layered nanopatterned photoanode (4NP) (scale bar: 7 μm). Cross view of MNPs at the (d) nanopatterned TiO2 layer (scale bar: 300 nm), (e) nanopattern interface (scale bar: 500 nm) and f) magnified image of e) (scale bar: 100 nm). Supplementary Figure S2. SEM image of nanopatterned TiO2 layer with top view; (a) before spin-coating polystyrene (PS) solution, (b) after spin-coating PS of 0.1 wt% solution, (c) 0.5 wt%, (d) 1 wt%, (e) 3 wt% and (f) 5 wt%. (scale bar: 200 nm) Supplementary Figure S3. The Fourier transform infrared spectroscopy (FT-IR) of polystyrene (PS) and MNPs. Commercially available PS (black line), MNPs after spin-coating PS (red line) and MNPs after calcination. (blue line) Supplementary Figure S4. The EDS analysis of nanopatterned TiO2 layer. (a, b, c) The SEM image and (b, d, f) EDS mapping image of nanopatterned TiO2 layer (a,b) before spin-coating polystyrene (PS) solution, (c, d) after spin-coating PS solution (5 wt%), and (e, f) after calcination at 500 °C for 30 min. The element color (Ti: green, O: blue, C: red) (scale bar: 1 μm). Supplementary Figure S5. The light transmittance characteristic of MNPs after N719 dye loading. Flat (black), 1NP (red), 2NP (blue), 3NP (magenta), and 4NP (green). Supplementary Figure S6. The absorption spectra of desorbed N719 dye from the MNPs in a solution of NaOH (5 mM) in an ethanol/water (1:1 v/v) mixture. Flat (black), 1NP (red), 2NP (blue), 3NP (magenta), and 4NP (green). Supplementary Figure S7. (a) The electron lifetime (τr), (b) diffusion coefficient (Dn), and (c) diffusion length (Ln) of the ssDSSCs fabricated with multi-nanopatterned photoanodes (MNPs) as determined from the IMPS / IMVS measurement. Flat (black), 1NP (red), 2NP (blue), 3NP (magenta), and 4NP (green). 2 Supplementary Table S1. The atomic percent of elements in the MNPs by EDS analysis. a) Sample Atomic percent (%) of titanium (Ti) Atomic percent (%) of oxygen (O) Atomic percent (%) of carbon (C) Total atomic percent (%) Before PS coating 33.3 66.7 - 100 After PS coating a) 7.2 4.6 88.2 100 After calcination (500°C, 30 min) 33.1 66.9 - 100 The 5 wt% of PS solution was spin-coated on the nanopatterned TiO2 film. Supplementary Table S2. Relative absorption, transmittance and reflectance data of different number of nanopatterned layer of MNPs. Relative Relative Relative absorption b) transmittance b) reflectance b) (400 nm ~ 700 nm) (400 nm ~ 700 nm) (400 nm ~ 700 nm) Flat 1 1 1 1NP 1.16 0.81 1.29 2NP 1.24 0.65 1.37 3NP 1.26 0.57 1.43 4NP 1.27 0.53 1.51 Sample a) a) Relative absorption, transmittance and reflectance of samples were calculated by integrating UV-vis spectrum. b) Relative optical data with reference to the absorption of flat, characterized by UV-vis spectroscopy. 3 Supplementary Table S3. The weight percent of TiO2 paste for fabricating MNPs and amount of dye loading of MNPs. Weight percent of TiO2 paste b) Dye loading c) (wt %) (nmol cm-2) Flat 100 86.1 1NP 100 85.7 2NP 80 85.5 3NP 65 85.9 4NP 50 85.4 Sample a) The thickness of MNPs was 12 μm. b) The TiO2 paste were diluted by organic solvent (terpineol) with vigorous stirring. c) The concentration of desorbed dye solution was analyzed by using a UV/Vis spectrophotometer. a) 4