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DOE OSTI · 2570463

Differential absorption of circularly polarized light by a centrosymmetric crystal

Parrish, Katherine A. [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0000000308149638)·Salij, Andrew [Northwestern Univ., Evanston, IL (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000195073701)·Kamp, Kendall R. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000327151514)·Smith, Evan [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0000000290907196)·Utama, M. Iqbal Bakti [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000244548348)·Bergsten, Anders J. [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0009000930842376)·Czerwinski, Rachel [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0009000339677983)·Smith, Mackinsey A. [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:000000024685316X)·Hersam, Mark C. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000341201426)·Poeppelmeier, Kenneth R. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000316559127)·Goldsmith, Randall H. [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0000000190838592)·Tempelaar, Roel [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000307867304)
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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. Here, in addition to enabling a chiroptical response under centrosymmetry, this process opens up photonic engineering opportunities based on crystalline solids.

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36 MATERIALS SCIENCE37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

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Parrish, Katherine A. [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0000000308149638), Salij, Andrew [Northwestern Univ., Evanston, IL (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)] (ORCID:0000000195073701), Kamp, Kendall R. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000327151514), Smith, Evan [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0000000290907196), Utama, M. Iqbal Bakti [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000244548348), Bergsten, Anders J. [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0009000930842376), Czerwinski, Rachel [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0009000339677983), Smith, Mackinsey A. [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:000000024685316X), Hersam, Mark C. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000341201426), Poeppelmeier, Kenneth R. [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000316559127), Goldsmith, Randall H. [Univ. of Wisconsin, Madison, WI (United States)] (ORCID:0000000190838592), Tempelaar, Roel [Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000307867304). 2025-06-12. Differential absorption of circularly polarized light by a centrosymmetric crystal. https://doi.org/10.1126/science.adr5478

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Cyclic moisture reactivation of calcium sorbents for long duration thermochemical energy storage

The transition to a flexible and reliable energy infrastructure, using electro-thermal energy generation technologies such as geothermal, concentrated solar power, and nuclear, usually demands simultaneous advancement of thermal energy storage (TES) to support on-demand electricity generation and industrial applications while mitigating the inherent intermittency of renewable energy sources and power outages from direct energy generation. Among TES technologies, thermochemical energy storage (TCES) based on calcium looping emerges as a compelling high-power energy storage candidate due to its high reaction enthalpy, compatibility with elevated operating temperatures, and abundance of low-cost materials. However, the long-term durability of calcium-based sorbents for TCES is hindered by surface sintering and particle aggregation, leading to performance degradation over repeated thermal cycles. This study explores a moisture hydration-based strategy to regenerate a degraded calcium sorbent and mitigate performance degradation for long duration TCES. The addition of moisture transforms calcium oxide into calcium hydroxide and produces intercalation water layers, associated with a regenerated surface area and reduced calcium oxide crystallite size. Both these effects are beneficial in restoring the sorbents' reactivity for carbonization. Additionally, an optimized hydration-assisted reactivation protocol balances the recovered energy storage capacity with heating penalty required for moisture removal from hydrated samples, resulting in an enhanced energy storage capacity up to 176% compared to benchmark sorbents that undergo cycling without reactivation after 60 cycles. In conclusion, these results highlight the potential of hydration-assisted reactivation to enhance the long-term performance of TCES, providing an effective pathway to advancing electro-thermal storage technologies.

36 MATERIALS SCIENCE↗