For the HTO-PA sample, the SAED-measured (008) reflection with d-spacing measuring 0.29 nm was comparable to the simulated value of 0.287 nm, and the (220) reflection at 0.19 nm also agreed with the predicted value. Similarly, for the HTO-HDA sample, the SAED-derived (40-4) reflection with d-spacing of 0.30 nm and (1-10) with d-spacing of 0.38 nm were consistent with the corresponding simulated values of 0.30 nm and 0.38 nm, respectively. Overall, the TEM and SAED analysis confirm the validity of the proposed structural models for the pillared tetratitanates. Additionally, calculated XRD pattern of the structural models of HTO-PA and HTO-HDA are given in Fig. . It should be noted that the experimental structural analysis is limited to the titanate host, while the conformation of organic pillars is indirectly concluded based on minimized free energy and previous literature reports of confined alkyl(di)amine pillars. The interaction between nanoconfined pillars within the interlayer and the HTO-based host lattice is analyzed by Raman spectroscopy. This allows to assess any organic pillaring-induced changes in bonding environment. The presence of organic pillars in HTO-PA and HTO-HDA is confirmed by signals in the C-H stretching region (2800 to 3000 cm -1 ). Moreover, the spectra of HTO, HTO-PA and HTO-HDA are highly comparable in the wavenumber region below ca. 900 cm -1 typically assigned to the Ti-O lattice vibrations, with no new major signals appearing. Shifts or broadening of certain signals can provide information about hostpillar interactions. In HTO, the band at 267 cm -1 attributed to the Ti-OH bonds blue shifts to 275 cm -1 after pillaring with either PA or HDA. The Raman signals of HTO at 394, 452, 681 and 866 cm -1 have previously been assigned to protonated tetratitanate . They are still present (394 and 452 cm -1 ), red shift (681 to ca. 661 cm -1 ) or broaden (866 cm -1 ) after organic pillaring with PA and HDA. Other peaks arising from the organic pillars are present in HTO-PA and HTO-HDA and can be attributed to different components of the organic molecules (Fig. ). The overall strong similarity of the spectra is indicative of the tetratitanate intralayer structure remaining intact after pillaring. Slight shifts/broadening of protonated titanate related signals suggests an interaction between the organic pillars and the terminal protons of the titanate layers.