Nanochannel-Assisted Perovskite Nanowires: Growth Mechanisms. to Photodetector Applications

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1 Supplementary Information: Nanochannel-Assisted Perovskite Nanowires: Growth Mechanisms to Photodetector Applications Qitao Zhou, Jun Gyu Park, Riming Nie, Ashish Kumar Thokchom, Dogyeong Ha, Jing Pan, Sang Il Seok, *, and Taesung Kim *, Department of Mechanical Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulsan 44919, Republic of Korea School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulsan 44919, Republic of Korea School of Chemical Engineering Sungkyunkwan University (SKKU), 2066, Seobu-ro, Jangan-gu, Suwon , Republic of Korea CORRESPONDENCE: Sang Il Seok Department of Chemical Engineering Ulsan National Institute of Science and Technology (UNIST) 50 UNIST-gil, Ulsan 44919, Republic of Korea Taesung Kim Department of Mechanical Engineering Ulsan National Institute of Science and Technology (UNIST) 50 UNIST-gil, Ulsan 44919, Republic of Korea Tel: Fax:

2 Supplementary Figures Figure S1. The photographic image of the micro-/nanofluidic platform made of PDMS for fabricating MAPbI 3 NWs. The platform has two separate microchannels, which have a part of inlet and outlet, and are connected with crack-nanochannels. 2

3 Figure S2. a) b) Electron diffraction patterns taken from two different positions for the same NW correspond to the entire TEM image of the MAPbI 3 NW shown in Figure 1i. 3

4 Figure S3. Time-lapse microscopic images show the temporal fabrication process of MAPbI 3 wires over 900 min. A bunch of MWs and/or NWs are generated in the two microchannels from the left to the right while a single NW is generated in the nanochannel. A glass substrate was used for observation from the bottom. 4

5 Figure S4. Three cross-sectional profiles of the AFM topographic images shown in Figure 2b. Left: 200 nm in depth and 1 µm width. Middle: 350 nm in depth and 2 µm width. Right: 500 nm depth and 4 µm width. 5

6 Figure S5. a) Schematic of the micro-/nanofluidic platform which with smaller upper microchannel and setting for MAPbI 3 DMF NW growth. b) c) The growth of MAPbI 3 DMF NWs with the help of the micro-/nanofluidic PDMS platform in which the upper microchannels (20 and 50 µm in width and 10 µm in depth) were relatively narrower than the lower microchannel (100 µm in width and 10 µm in depth). 5 μl MAI/PbI 2 /DMF solution (0.125 M) was injected into the upper PDMS microchannels and then all of four inlets at the top side remained filled. The experiment was carried out at room temperature. Scale bars are 100 μm. 6

7 Figure S6. Optical images of the needle-like PbI 2 DMF precursors growing from a droplet of PbI 2 /DMF at 298 K. Scale bars are 100 μm. 7

8 Figure S7. The switched Tauc plots of the (αhυ) 2 versus hυ curves of the MAPbI 3 DMF NW at different times. From the curves, the intersection of the tangent line with the x-axis denote the band gap energy value. Thus, the band gap energy values of the MAPbI 3 DMF NW at t = 22 min and t = 35 min are determined to be 2.87 ev and 2.06 ev, as indicated with the dash-lines, respectively. These values are higher than that of pure MAPbI 3 (ca ev) 1 because the precursors of MAPbI 3 DMF NWs can still exist. In short, the calculation is based on the equation of α = A(hυ E g ) n/2 /hυ, where α, A, h, υ, and n correspond to the absorption coefficient, a proportionality constant, the Planck s constant, the frequency of the incident light, and an index, respectively. 2 Here, n is equal to 1 because MAPbI 3 is a direct band gap semiconductor material. Therefore, the absorption edge can be estimated by the formula λ g = /E g. 3 The absorption edges of the MAPbI 3 DMF NW are obtained at the wavelengths of 432 nm (t = 22 min) and 602 nm (t = 22 min), respectively. 8

9 Figure S8. a) The in situ UV-vis absorption spectra of the PbI 2 DMF NW. b) The UV-vis absorption spectra of the components and the UV-vis absorption spectra of a MAPbI 3 NW after annealing (i.e., after complete DMF evaporation). 9

10 Figure S9. Photocurrents of a MAPbI 3 NW under 532-nm-laser illumination conditions. 10

11 Supplementary Table Table S1. Comparison of the responsivity and response time of the photodetectors. Materials Responsivity (A/W) Voltage Rising time Decay time Single MAPbI 3 NW 410-1V 0.22 ms 0.79 ms This work Ref. MAPbI 3 NWs V 0.08 ms 0.24 ms [4] MAPbI 3 NWs 120 ms 210 ms [5] MAPbI 3 NWs ms 0.25 ms [6] MAPbI 3 Film V 10 μs 41 μs [7] 11

12 Supplementary Movies Movie S1: 5 μl as prepared MAI/PbI 2 /DMF solutions (0.125 M) were injected into the right side inlets of two parallel PDMS microchannels, respectively. The experiment is carried out at room temperature. Movie S2: 5 μl as prepared MAI/PbI 2 /DMF solutions (0.125 M) were injected into the upper PDMS microchannels from all of three different inlets at the top side, respectively. The experiment is carried out at room temperature. Movie S3: 5 μl PbI 2 /DMF solutions (0.125 M) were injected into the upper PDMS microchannels from all of three different inlets at the top side, respectively. The experiment is carried out at room temperature. Movie S4: 5 μl as prepared MAI/PbI 2 /DMF solutions ( M) were injected into the upper PDMS microchannels from all of three different inlets at the top side, respectively. The experiment is carried out at room temperature. Movie S5: 5 μl as prepared MAI/PbI 2 /DMF solutions (0.125 M) were injected into the upper PDMS microchannels from both of two inlets, respectively. The experiment is carried out at room temperature. 12

13 References 1 Grätzel, M. The Light and Shade of Perovskite Solar Cells. Nat. Mater. 2014, 13, Liu, J.; Liu, Y.; Liu, N.; Han, Y.; Zhang, X.; Huang, H.; Lifshitz, Y.; Lee, S.-T.; Zhong, J.; Kang, Z. Metal-Free Efficient Photocatalyst for Stable Visible Water Splitting via a Two-Electron Pathway. Science 2015, 347, Zhang, K.; Liu, C.; Huang, F.; Zheng, C.; Wang, W. Study of the Electronic Structure and Photocatalytic Activity of the BiOCl Photocatalyst. Appl. Catal., B 2006, 68, Deng, W.; Zhang, X.; Huang, L.; Xu, X.; Wang, L.; Wang, J.; Shang, Q.; Lee, S.-T.; Jie, J. Aligned Single-Crystalline Perovskite Microwire Arrays for High-Performance Flexible Image Sensors with Long-Term Stability. Adv. Mater. 2016, 28, Zhu, P.; Gu, S.; Shen, X.; Xu, N.; Tan, Y.; Zhuang, S.; Deng, Y.; Lu, Z.; Wang, Z.; Zhu, J. Direct Conversion of Perovskite Thin Films into Nanowires with Kinetic Control for Flexible Optoelectronic Devices. Nano Lett. 2016, 16, Horváth, E.; Spina, M.; Szekrényes, Z.; Kamarás, K.; Gaal, R.; Gachet, D.; Forró, L. Nanowires of Methylammonium Lead Iodide (CH 3 NH 3 PbI 3 ) Prepared by Low Temperature Solution-Mediated Crystallization. Nano Lett. 2014, 14, Dong, R.; Fang, Y.; Chae, J.; Dai, J.; Xiao, Z.; Dong, Q.; Yuan, Y.; Centrone, A.; Zeng, X. C.; Huang, J. High-Gain and Low-Driving-Voltage Photodetectors Based on Organolead Triiodide Perovskites. Adv. Mater. 2015, 27,

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