“…Moreover, their motions and interplay with the electronic dynamics of their parent material is a point of considerable interest as researchers aim to develop a comprehensive understanding of the molecular origins of the remarkable optoelectronic properties of HOIPs. [11][12][13][14][15][16] As such, the rotational properties of the A-site cations have been extensively studied using a battery of experimental techniques, including steady-state IR 17 and millimetre wave 18 spectroscopy, calorimetry, 17 solid-state NMR, [19][20][21] neutron scattering, [22][23][24] and most recently time-resolved ultrafast spectroscopy. 10,14,[25][26][27] From these extensive investigations, a picture of the rotational dynamics of the A-site cation within HOIPs has emerged.…”