bio-mof-1 DMASM Wavenumber (cm -1 ) Supplementary Figure S1 FTIR spectra of bio-mof-1, DMASMI, and bio-mof-1 DMASM.

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1 bio-mof-1 Transmittance bio-mof-1 DMASM DMASMI Wavenumber (cm -1 ) Supplementary Figure S1 FTIR spectra of bio-mof-1, DMASMI, and bio-mof-1 DMASM. Intensity (a.u.) bio-mof-1 DMASM as synthesized bio-mof-1 simulated bio-mof (degree) Supplementary Figure S2 PXRD patterns of bio-mof-1 and bio-mof-1 DMASM.

2 0.9 c in MOFs (mmol/cm 3 ) c in solution (mmol/ml) Supplementary Figure S3 Loaded content of DMASM cations in bio-mof-1 as a function of the concentration of DMASMI solution that used for ion-exchange. Supplementary Figure S4 1 H NMR spectra (600 MHz) of dye DMASMI and bio-mof-1 DMASM dissolved in DMSO-d6, D2O and DCl.

3 Supplementary Figure S5 CIE chromaticity diagram of bio-mof-1 DMASM composite with different DMASM contents under UV light excitation at 340 nm. Intensity (a.u.) bio-mof % 0.071% 0.34% 1.8% 8.7% 39% 91% Supplementary Figure S6 Emission spectra of bio-mof-1 and bio-mof-1 DMASM powder with different DMASM contents excited at 365 nm.

4 (a) Fluorescence intensity (a.u.) moni = 412 nm ex = 365 nm (10 4 mol -1 L cm -1 ) (b) Intensity (a.u.) bio-mof-1 DMASM-0.97% moni = 622 nm DMASMI powder moni = 682 nm in DMF moni = 628 nm Supplementary Figure S7 Fluorescence properties of bio-mof-1, DMASMI and bio-mof-1 DMASM. (a) Excitation (black) and emission (blue) spectra of bio-mof-1, and UV-vis absorption spectrum of DMASMI in DMF solution (red). (b) Excitation spectra of DMASMI powder (blue), DMASMI in DMF solution (pink) and bio-mof-1 DMASM (red). λmoni is the monitoring wavelength.

5 (a) (b) Supplementary Figure S8 Simulated morphology of bio-mof-1. (a) viewed along the c-axis direction of bio-mof-1, which corresponds to the longitudinal direction of a single crystal. (b) viewed along a-axis direction. Supplementary Figure S9 Confocal images of bio-mof-1 DMASM at different depths recorded on an Olympus FV1000 laser scanning confocal microscope. Excitation wavelength, 488 nm; scale bar, 100 μm.

6 (a) (b) Intensity (a.u.) Supplementary Figure S10 Dye distribution in bio-mof-1. (a) Fluorescence microscopy images of bio-mof-1 DMASM; (b) Emission spectra of selected regions in bio-mof-1 DMASM crystals recorded on a laser scanning confocal microscope. Supplementary Figure S11 Fluorescence anisotropy of bio-mof-1 DMASM crystal. (a, b) Fluorescence images of a bio-mof-1 DMASM crystal with a dye concentration of 0.054% under linearly polarized light excitation. Scale bar, 100 μm. (c) Fluorescence intensity of the crystal with response to polarization light at a wavelength of 470 nm. The intensity of excitation light at different polarization directions was corrected.

7 Normalized intensity (degree) 300 Supplementary Figure S12 Fluorescence intensity of a bio-mof-1 DMASM crystal with a dye concentration of 0.97% in response to linear polarization excitation, showing less significant emission anisotropy than that with a lower dye concentration (0.054%). SHG intensity (a.u.) bio-mof-1 DMASM DMASMI bio-mof Supplementary Figure S13 SHG spectra of bio-mof-1, DMASMI powder, and bio-mof-1 DMASM measured by Kurtz powder technique using a Q-switched Nd:YAG pulse laser at 1064 nm as fundamental frequency laser.

8 100 bio-mof R (%) bio-mof-1 DMASM Normalized intensity Supplementary Figure S14 Diffuse reflectance UV-vis spectra of bio-mof-1 (red) and bio-mof-1 DMASM (orange), and emission spectrum of bio-mof-1 DMASM (blue) at an excitation wavelength of 365 nm. 100 R (%) % 4.8% 7.9% 20% 55% Supplementary Figure S15 Diffuse reflectance UV-vis spectra of DMASM dye included bio-mof-1 (bio-mof-1 DMASM) with different dye contents. These spectra were recorded on a Hitachi U-4100 spectrometer that has equipped with an integral sphere. The red shift of absorption maximal peak suggests the presence of J-aggregation in bio-mof-1 DMASM composite at high DMASM concentrations.

9 Intensity (a.u.) Pulse Energy 2 (mj 2 ) Supplementary Figure S16 Two-photon excited fluorescence intensity (λex = 1064 nm) of bio-mof-1 DMASM versus excitation pulse energy. Error bars are the standard deviation of uncertainty for each point. Supplementary Figure S17 Schematic illustration of TPP lasing spectra measurement setup.

10 3 (nm) /L ( m -1 ) Supplementary Figure S18 Mode spacing Δλ around λ = 640 nm versus 1/L of bio-mof-1 DMASM crystals, showing clearly a linear relationship. L is the thickness of the bio-mof-1 DMASM crystals. 1.0 Normalized intensity irradiated at 365 nm irradiated at 1064 nm Time (s) Supplementary Figure S19 Photostability of bio-mof-1 DMASM irradiated at 365 and 1064 nm.

11 Supplementary Figure S20 1 H NMR spectra (500 MHz) of pure dye DMASMI. Excitation light Emission light Intensity (a.u.) Without sample With sample A ex, without sample Aem A ex, with sample Supplementary Figure S21 Measurement of the quantum yield using the absolute method. Aex, with sample and Aex, without sample are the integrated intensity of the excitation light source peaked at 468 nm with and without sample, respectively, and Aem is the integrated intensity of emission light of the sample (Ref. 55).

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