Supporting Information S.1 Investigation of SD Structure by 13C-1H cross polarized MAS NMR 13 C-1H CPMAS NMR spectra were collected on a BRUKER Avance DSX 400 spectrometer (B = 9.4 T) at resonance frequencies of 100.65 MHz (13C) and 400.287 MHz (1H) using a 4 mm MAS probe with a spinning speed of 10 kHz. Adamantane was used as the external chemical shift reference (38.5 ppm of methylene C for 13C and 1.78 ppm for 1H). A 3 ms contact time was used for cross polarization. 6.5 μs π/2 1H excitation pulses with 5 s recycle delay were applied while 5076 scans were collected. The power of the contact pulses was varied by using a ramp. The 13C-1H cross polarized MAS NMR reveals two main peaks in the spectra in Figure S1. Peak I in the high field at 6.66 ppm is assigned to the carbon atom in the methyl group (see Table S1). Peak III from the methylene group in the TEA+ is downfield at 52.46 ppm. We note that cross-polarization leads to 13C peak areas that are not correlated to composition. An unexpected line is present also at 29.9 ppm in the spectra of Al-TEA+ zeolite beta (L = 0.07). This may be from the rf and could be tested by collecting an NMR spectrum with a different center resonance frequency. The 13C-1H cross polarized MAS spectra show that the TEA+ does not decompose during the synthesis of zeolite beta. S.2 Investigation of SD Occluded in Zeolite Beta by Raman Spectroscopy Raman spectra of as-prepared zeolite beta samples were measured using LabRAM spectrometer (Horiba Jobin Yvon GmbH) equipped with a Nd-YAG laser (532 nm). The spectra were measured at 180 ° scattering angle with a hole diameter of 1000 µm and slit width of 100 µm. In the spectra of the both of the samples in Figure S.2 C-H stretching bands appear at 2910, 2956, and 3008 cm-1. Several more bands due to C-H bending and C-C skeletal vibration modes are observed between 400 and 1500 cm-1. There is no effect of the Al concentration (or of the [[≡SiO]– TEA+] ion pairs) on the Raman spectra in contrast to the FTIR spectra which exhibited reduced peak intensity from the C-H bending and stretching modes at higher [[≡SiO]– TEA+] ion pair concentrations. Supporting Tables Table S1. Peak parameters from 13C-1H CP MAS NMR of the Al-TEA+ zeolite beta. Supporting Figures Figure S1. 13C-1H CP MAS NMR of the Al-TEA+ zeolite beta (L = 0.01) in the bottom layer and of the Al-TEA+ zeolite beta (L = 0.07) in the top layer. Figure S2. Raman spectra of Al-TEA+ zeolite beta (L = 0.01) in the bottom layer and of Al-TEA+ zeolite beta (L = 0.07) in the top layer. Figure S3. Correlation between the signal at peak IV in the FTIR spectra and the effective surface area of the samples as measured by N2 adsorption.