Figure 1

Crystal structure of croconic acid and optical probes on its polarization, π-electrons, and protons. (a) Molecular and crystal structure of croconic acid. The pink-shaded circles show unbalanced π-electron distributions, which are responsible for the ferroelectric polarization. (b–d) Optical probes used in this study: (b) terahertz-pulse-pump SHG-probe measurement for the detection of the polarization change, (c) terahertz-pulse-pump visible-reflectivity-probe spectroscopy for the detection of the π-electron wavefunction change, and (d) mid-IR reflection spectroscopy under static electric fields for the detection of the proton displacements.