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DOE OSTI · 3015280

Strong, Yet Split Hydrogen Bonding with Ice Rules in Delafossite (H/D)RhO 2

Wright, Matthew A. [Univ. of California, Santa Barbara, CA (United States)] (ORCID:0000000306173992)·Mulligan, Anya S. [Univ. of California, Santa Barbara, CA (United States)] (ORCID:0009000576826540)·Rout, Dibyata [Univ. of California, Santa Barbara, CA (United States)] (ORCID:0000000347577221)·Hu, Jerry G. [Univ. of California, Santa Barbara, CA (United States)] (ORCID:0009000541225526)·Liu, Jue [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)] (ORCID:000000024453910X)·Behrens, Rachel L. [Univ. of California, Santa Barbara, CA (United States)] (ORCID:000900093496782X)·Chamorro, Juan R. [Carnegie Mellon Univ., Pittsburgh, PA (United States)] (ORCID:0000000204625580)·Wilson, Stephen D. [Univ. of California, Santa Barbara, CA (United States)] (ORCID:000000033733930X)·Cheetham, Anthony K. [Univ. of California, Santa Barbara, CA (United States)] (ORCID:0000000315184845)·Seshadri, Ram [Univ. of California, Santa Barbara, CA (United States)] (ORCID:0000000158584027)
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Abstract

Despite remaining enigmatic, strong hydrogen bonding provides an advanced design handle for tailoring the properties of functional materials. Here, in this study, 3 R –(H/D)RhO 2 delafossites (prepared by ion exchange of Na + from NaRhO 2 ) contain H/D in linear coordination with O, linking Rh III O 2 layers. Bragg and real-space X-ray and neutron scattering analysis, vibrational and solid-state NMR spectroscopy, and density functional theory (DFT)–based electronic structure calculations have been employed to understand the nature of the hydrogen bonding. Despite short distances between H/D and the two O to which they are bonded, a clear double-minimum corresponding to a shorter and longer (H/D)–O distance is established. The triangular lattices formed by H/D appear to display ice-like disorder, corroborated by low-temperature heat capacity measurements.

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Wright, Matthew A. [Univ. of California, Santa Barbara, CA (United States)] (ORCID:0000000306173992), Mulligan, Anya S. [Univ. of California, Santa Barbara, CA (United States)] (ORCID:0009000576826540), Rout, Dibyata [Univ. of California, Santa Barbara, CA (United States)] (ORCID:0000000347577221), Hu, Jerry G. [Univ. of California, Santa Barbara, CA (United States)] (ORCID:0009000541225526), Liu, Jue [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)] (ORCID:000000024453910X), Behrens, Rachel L. [Univ. of California, Santa Barbara, CA (United States)] (ORCID:000900093496782X), Chamorro, Juan R. [Carnegie Mellon Univ., Pittsburgh, PA (United States)] (ORCID:0000000204625580), Wilson, Stephen D. [Univ. of California, Santa Barbara, CA (United States)] (ORCID:000000033733930X), Cheetham, Anthony K. [Univ. of California, Santa Barbara, CA (United States)] (ORCID:0000000315184845), Seshadri, Ram [Univ. of California, Santa Barbara, CA (United States)] (ORCID:0000000158584027). 2025-11-03. Strong, Yet Split Hydrogen Bonding with Ice Rules in Delafossite (H/D)RhO 2. https://doi.org/10.1002/anie.202515471

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