Molecular Dynamics of Flexible Polar Cations in a Variable Confined Space: Toward Exceptional Two‐Step Nonlinear Optical Switches

The changeable molecular dynamics of flexible polar cations in the variable confined space between inorganic chains brings about a new type of two-step nonlinear optical (NLO) switch with genuine "off-on-off" second harmonic generation (SHG) conversion between one NLO-active state and two NLO-inactive states.