Differential absorption of circularly polarized light by a centrosymmetric crystal
Katherine A. Parrish, Andrew Salij, Kendall R. Kamp, Evan Smith, M. Iqbal Bakti Utama, Anders J. Bergsten, R.N. Czerwinski, Mackinsey A. Smith, Mark C. Hersam, Kenneth R. Poeppelmeier, Randall H. Goldsmith, Roel Tempelaar
Abstract
Crystalline solids are governed by universal structure-property relationships derived from their crystal symmetry, leading to paradigmatic rules on what properties they can and cannot exhibit. A long-held structure-property relationship is that centrosymmetric crystals cannot differentially absorb circularly polarized light. In this study, we demonstrate the design, synthesis, and characterization of the centrosymmetric material Li 2 Co 3 (SeO 3 ) 4 , which violates this relationship not by defying symmetry-imposed selection rules but by invoking a photophysical process not previously characterized for crystalline solids. This process originates from an interference between linear dichroism and linear birefringence, referred to as LD-LB, and involves strong chiroptical signals that invert upon sample flipping. In addition to enabling a chiroptical response under centrosymmetry, this process opens up photonic engineering opportunities based on crystalline solids.