Supplementary Information. Bright, wind-driven white mechanoluminescence from zinc sulphide

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1 Electronic Supplementary Material (ESI) for Energy & Environmental Science. This journal is The Royal Society of Chemistry 4 Supplementary Information Bright, wind-driven white mechanoluminescence from zinc sulphide microparticles embedded in a polydimethylsiloxane elastomer Soon Moon Jeong,* a Seongkyu Song, a Kyung-Il Joo, a Joonwoo Kim, a Sung-Ho Hwang, a Jaewook Jeong a and Hyunmin Kim a a Nano & Bio Research Division, Daegu Gyeongbuk Institute of Science and Technology, 5- Sang-Ri, Hyeonpung-Myeon, Dalseong-Gun, Daegu 7-873, Republic of Korea *Corresponding author: smjeong@dgist.ac.kr These authors contributed equally to this work

2 Brightness (cd/m ) 5 5 B+PDMS G+PDMS B'+PDMS G'+PDMS O'+PDMS 7% 3% 3% cycle/min Fig. S. ML brightness of various samples. The samples compared are the B+, G+, and samples (blue, GG64; green, GG45; and orange, GG3, purchased from Osram Sylvania Inc.) and the B, G, and O materials from previous studies (blue, GGS6; green, GGS4; and orange, GGS, purchased from Osram Sylvania Inc.). Note that the current materials are approximately 3% brighter at the 5-cpm S-R rate.

Sample preparation for S-R measurement (a) (b) (c) Phosphor (B/G/O colour) PDMS Phosphor : PDMS = 7: 3 (weight ratio) Mixing

Initial Stretching Releasing.5 cm 3.5 cm.5 cm cm cm cm Fig. S. Schematic illustration of the sample preparation and measurement conditions for the S- R test.

(c) This mixed solution was poured into a steel mould, which acted as a template.

(f) The ML composites for the S-R measurement were prepared by separating the ML from the steel mould.

3 Sample preparation for S-R measurement (a) (b) (c) Phosphor (B/G/O colour) PDMS Phosphor : PDMS = 7: 3 (weight ratio) Mixing Pouring to steel mould (d) (e) (f) 7, 3min curing Separation Squeeze Thickness: ~7 μm S-R measurement condition (g) (h) (i) Initial Stretching Releasing.5 cm 3.5 cm.5 cm cm cm cm Fig. S. Schematic illustration of the sample preparation and measurement conditions for the S- R test. (a) Mixed or unmixed (i.e., pure) phosphors were poured into a PDMS solution and (b) mixed well. (c) This mixed solution was poured into a steel mould, which acted as a template. After (d) squeezing, (e) the solution was cured at 7 C for 3 min. (f) The ML composites for the S-R measurement were prepared by separating the ML from the steel mould. To take the S-R measurement, (g) the sample was mounted onto the S-R system without any deformation (.5 cm). The sample was then (h) mechanical stretched (3.5 cm) and (i) released (.5 cm). The S-R process shown in (h) and (i) is defined as cycle.

4 (a) Solvent : Toluene 95wt% + Trichloro(octadecyl)silane 5wt% 6, h stirring SAM treatment Toluene 5min dipping N gas blowing Rotating magnetic bar Hole patterned Al mould (b) (c) Prepare SAM treated Al mould Inject green (G+PDMS) paste into the holes with ML logo and then pour it to make thick plate (e) Photograph (d) 7, 3 min curing Detach PDMS from Al mould Fig. S3. Schematic of the fabrication process used to produce the wind-driven patterned ML sample with only a green ML. (a) SAM surface treatment of the Al mould with ML patterned holes using a mixed solvent of toluene (95 wt%) and trichloro(octadecyl)silane (5 wt%). (b c) Injection of green (G+PDMS) paste into the holes defining the ML logo, followed by pouring to make a thick plate. (d e) After curing (at 7 C for 3 minutes), the PDMS is separated from the Al mould.

5 (a) Solvent : Toluene 95wt% + Trichloro(octadecyl)silane 5wt% 6, h stirring SAM treatment Toluene 5min dipping N gas blowing Rotating magnetic bar Hole patterned Al mould (b) tape (c) 7, 3 min curing Inject green paste (G+PDMS) into the holes with ML logo Inject white (O+B+PDMS; ) paste into other holes and then pour it to make thick plate (e) Photograph (d) 7, 3 min curing Detach PDMS from Al mould Fig. S4. Schematic of the fabrication process used to produce the wind-driven patterned ML sample with a green ML and white background. (a) SAM surface treatment of the Al mould with ML patterned holes using a mixed solvent of toluene (95 wt%) and trichloro(octadecyl)silane (5 wt%). (b) Injection of green (G+PDMS) paste into the holes defining the ML logo. (c) Injection of white (O+B+PDMS; ) paste into the remaining holes, followed by pouring to make a thick plate. (d e) After curing (at 7 C for 3 minutes), the PDMS is separated from the Al mould.

6 (a) Hz (b) Hz (c) 5 Hz O:G=9: O:G=8: O:G=7:3 O:G=6:4 O:G=5:5 O:G=9: O:G=8: O:G=7:3 O:G=6:4 O:G=5:5 O:G=9: O:G=8: O:G=7:3 O:G=6:4 O:G=5:5 G+PDMS G+PDMS G+PDMS (d) Hz (e) Hz (f) O:B=9: O:B=8: O:B=9: O:B=8: 5 Hz O:B=9: O:B=8: B+PDMS B+PDMS B+PDMS Fig. S5. EL spectra of the O+G+PDMS and O+B+PDMS samples with various mixing ratios at (a, d) Hz, (b, e) Hz, and (c, f) 5 Hz.

7 5 Hz Hz Hz 5 Hz O:G=8: 5 Hz Hz Hz 5 Hz O:G=9: 5 Hz Hz Hz 5 Hz O:G=7:3 5 Hz Hz Hz 5 Hz O:G=6:4 5 Hz Hz Hz 5 Hz 3 O:G=5:5 5 Hz Hz Hz 5 Hz 5 G+PDMS 5 Hz Hz Hz 5 Hz Fig. S6. Calculated EL intensity normalised to 586 nm in the O+G+PDMS ACEL samples with various mixing ratios.

8 5 Hz Hz Hz 5 Hz O:B=9: 5 Hz Hz Hz 5 Hz O:B=8: 5 Hz Hz Hz 5 Hz 3 5 Hz Hz Hz 5 Hz 5 Hz Hz Hz 5 Hz Hz Hz Hz 5 Hz 3 B+PDMS 5 Hz Hz Hz 5 Hz Fig. S7. Calculated EL intensity normalised to 586 nm in the O+B+PDMS ACEL samples with various mixing ratios.

9 (a) (b) (c) O:G=9: cpm cpm 3 cpm 4 cpm 5 cpm O:G=8: cpm cpm 3 cpm 4 cpm 5 cpm O:G=7:3 cpm cpm 3 cpm 4 cpm 5 cpm (d) O:G=6:4 cpm cpm 3 cpm 4 cpm 5 cpm (e) O:G=5:5 cpm cpm 3 cpm 4 cpm 5 cpm cpm (f) O:B=9: (g) O:B=8: (h) cpm cpm 3 cpm 4 cpm 5 cpm cpm 3 cpm 4 cpm 5 cpm cpm cpm 3 cpm 4 cpm 5 cpm (i) cpm cpm 3 cpm 4 cpm 5 cpm (j) cpm cpm 3 cpm 4 cpm 5 cpm Fig. S8. ML spectra obtained from O+G+PDMS (a-e) and O+B+PDMS (f-j) samples with various mixing ratios. The S-R rates were varied from to 5 cpm in -cpm increments.

10 (a) (c) (e) (g) (i) O:B=9: O:B=8: (b) (d) (f) (h) (j) O:B=9: O:B=8: Fig. S9. Wind-driven ML spectra obtained from O+B+PDMS. (a, c, e, g, i) Intensity plotted as a function of wavelength. (b, d, f, h, j) Intensity normalised to 586 nm plotted as a function of wavelength.

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