Niu, Chengwang | Engineering Papers

DOE OSTI2025

Pyrochlore NaYbO2: A Potential Quantum Spin Liquid Candidate

The search for quantum spin liquids (QSL) and chemical doping in such materials to explore superconductivity have continuously attracted intense interest. Here, we report the discovery of a potential QSL candidate, pyrochlore-lattice β-NaYbO2. Colorless and transparent NaYbO2 single crystals, layered α-NaYbO2 (∼250 μm on edge) and octahedral β-NaYbO2 (∼50 μm on edge), were grown for the first time. Synchrotron X-ray single-crystal diffraction unambiguously determined that the newfound β-NaYbO2 belongs to the three-dimensional pyrochlore structure characterized by the R3̅m space group, corroborated by synchrotron X-ray and neutron powder diffraction and pair distribution function. Magnetic measurements revealed no long-range magnetic order or spin glass behavior down to 0.4 K with a low boundary spin frustration factor of 17.5, suggesting a potential QSL ground state. Under high magnetic fields, the potential QSL state was broken and spins order. Our findings reveal that NaYbO2 is a fertile playground for studying novel quantum states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Tailoring the Electronic Structures and Spectral Properties of ZnO with Irradiation Defects Generated Under Intense Electronic Excitation: A Combined Experimental and DFT Approach

Here, the relationship between the composition of the internal defect states, spectral properties, and correlated electronic structures of wurtzite zinc oxide (ZnO) crystals under 645 MeV Xe 35+ irradiation is systematically investigated, employing experimental characterizations combined with first-principle calculations. Based on the ion irradiation-induced thermal expansion and relaxation processes, the high concentration of vacancy/interstitial defects produced from the transient disordered phase in molten track states trigger photoelectric changes, as follows: i) the generation of internal defect states effectively reduces the intrinsic bandgap (3.25 eV → 2.66 eV); ii) a large number of defective active sites inhibits the recombination between electron–hole pairs, causing dark conductance and photoconductance to increase with increasing damage levels until optimal fluence is achieved. Based on the density functional theory (DFT) with the GGA + U (GGA = generalized gradient approximation) method, the defective models associated with the different electronic structures, density of states, formation energy, and the nature of the chemical bonding are established. The narrowing of the bandgap observed experimentally and the enhancement of carrier concentration originating from the internal electron defect states are qualitatively verified, therefore laying the foundation for designing future nanoscale photoelectronic devices and microelectronics applications.

36 MATERIALS SCIENCE↗