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1. Wide‐Bandgap R Ba ₃ (B ₃ O ₆ ) ₃ ( R = Nd, Sm, Tb, Dy, and Er) Single Crystals for Ultraviolet Nonlinear Optics

   https://doi.org/10.1002/adom.202401437  

   Sarker, Saugata; Wang, Yu; Benyacko, Caeli; Guan, Yingdong; Yoshida, Suguru; Yennawar, Hemant; He, Jingyang; Mao, Zhiqiang; Gopalan, Venkatraman (August 2024, Advanced Optical Materials)

   Abstract Discovery of new materials with enhanced optical properties in the visible and UV‐C range can impact applications in lasers, nonlinear optics, and quantum optics. Here, the optical floating zone growth of a family of rare earth borates,RBa₃(B₃O₆)₃(R= Nd, Sm, Tb, Dy, and Er), with promising linear and nonlinear optical (NLO) properties is reported. Although previously identified to be centrosymmetric, the X‐ray analysis combined with optical second harmonic generation (SHG) assigns the noncentrosymmetricPspace group to these crystals. Characterization of linear optical properties reveals a direct bandgap of ≈5.61–5.72 eV and strong photoluminescence in both the visible and mid‐IR regions. Anisotropic linear and nonlinear optical characterization reveals both Type‐I and Type‐II SHG phase matchability, with the highest effective phase‐matched SHG coefficient of 1.2 pm V⁻¹at 800‐nm fundamental wavelength (for DyBa₃(B₃O₆)₃), comparable to β‐BaB₂O₄(phase‐matchedd₂₂≈ 1.9 pm V⁻¹). Laser‐induced surface damage threshold for these environmentally stable crystals is 650–900 GW cm⁻², which is four to five times higher than that of β‐BaB₂O₄, thus providing an opportunity to pump with significantly higher power to generate about six to seven times stronger SHG light. Since the SHG arises from disorder on the Ba‐site, significantly larger SHG coefficients may be realized by “poling” the crystals to align the Ba displacements. These properties motivate further development of this crystal family for laser and wide bandgap NLO applications. 

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2. Structural transitions, octahedral rotations, and electronic properties of A3Ni2O7 rare-earth nickelates under high pressure

   https://doi.org/10.1038/s41535-024-00648-0  

   Geisler, Benjamin; Hamlin, James_J; Stewart, Gregory_R; Hennig, Richard_G; Hirschfeld, P_J (April 2024, npj Quantum Materials)

   Abstract Motivated by the recent observation of superconductivity withT_c ~ 80 K in pressurized La₃Ni₂O₇¹, we explore the structural and electronic properties ofA₃Ni₂O₇bilayer nickelates (A = La-Lu, Y, Sc) as a function of pressure (0–150 GPa) from first principles including a Coulomb repulsion term. At ~ 20 GPa, we observe an orthorhombic-to-tetragonal transition in La₃Ni₂O₇at variance with x-ray diffraction data, which points to so-far unresolved complexities at the onset of superconductivity, e.g., charge doping by variations in the oxygen stoichiometry. We compile a structural phase diagram that establishes chemical and external pressure as distinct and counteracting control parameters. We find unexpected correlations betweenT_cand thein-planeNi-O-Ni bond angles for La₃Ni₂O₇. Moreover, two structural phases with significantc⁺octahedral rotations and in-plane bond disproportionations are uncovered forA = Nd-Lu, Y, Sc that exhibit a pressure-driven electronic reconstruction in the Nie_gmanifold. By disentangling the involvement of basal versus apical oxygen states at the Fermi surface, we identify Tb₃Ni₂O₇as an interesting candidate for superconductivity at ambient pressure. These results suggest a profound tunability of the structural and electronic phases in this novel materials class and are key for a fundamental understanding of the superconductivity mechanism. 

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3. Local structure of Sr ₂ CuO _3.3 , a 95 K cuprate superconductor without CuO ₂ planes

   https://doi.org/10.1073/pnas.1918890117  

   Conradson, Steven D.; Geballe, Theodore H.; Jin, Changqing; Cao, Lipeng; Baldinozzi, Gianguido; Jiang, Jack M.; Latimer, Matthew J.; Mueller, Oliver (February 2020, Proceedings of the National Academy of Sciences)

   The local structure of the highly “overdoped” 95 K superconductor Sr₂CuO_3.3determined by Cu K X-ray absorption fine structure (XAFS) at 62 K in magnetically oriented samples shows that 1) the magnetization is perpendicular to thecaxis; 2) at these levels of precision the Cu sublattice is tetragonal in agreement with the crystal structure; the O sublattice has 3) continuous -Cu-O- chains that orient perpendicular to an applied magnetic field; 4) approximately half-filled -Cu-O- chains that orient parallel to this field; 5) a substantial number of apical O vacancies; 6) O ions at some apical positions with expanded Cu-O distances; and 7) interstitial positions that imply highly displaced Sr ions. These results contradict the universally accepted features of cuprates that require intact CuO₂planes, magnetization along thecaxis, and a termination of the superconductivity when the excess charge on the CuO₂Cu ions exceeds 0.27. These radical differences in charge and structure demonstrate that this compound constitutes a separate class of Cu-O–based superconductors in which the superconductivity originates in a different, more complicated structural unit than CuO₂planes while retaining exceptionally high transition temperatures. 

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4. Designing multicomponent hydrides with potential high T _c superconductivity

   https://doi.org/10.1073/pnas.2413096121  

   Denchfield, Adam; Park, Hyowon; Hemley, Russell J (November 2024, Proceedings of the National Academy of Sciences)

   While hydrogen-rich materials have been demonstrated to exhibit high T_csuperconductivity at high pressures, there is an ongoing search for ternary, quaternary, and more chemically complex hydrides that achieve such high critical temperatures at much lower pressures. First-principles searches are impeded by the computational complexity of solving the Eliashberg equations for large, complex crystal structures. Here, we adopt a simplified approach using electronic indicators previously established to be correlated with superconductivity in hydrides. This is used to study complex hydride structures, which are predicted to exhibit promisingly high critical temperatures for superconductivity. In particular, we propose three classes of hydrides inspired by the Fm $\overline{3}$m RH ${}_3$structures that exhibit strong hydrogen network connectivity, as defined through the electron localization function. The first class [RH ${}_{11}$X ${}_3$Y] is based on a Pm $\overline{3}$m structure showing moderately high T_c, where the T_cestimate from electronic properties is compared with direct Eliashberg calculations and found to be surprisingly accurate. The second class of structures [(RH ${}_{11}$) ${}_2$X ${}_6$YZ] improves on this with promisingly high density of states with dominant hydrogen character at the Fermi energy, typically enhancing T_c. The third class [(R ${}^1$H ${}_{11}$)(R ${}^2$H ${}_{11}$)X ${}_6$YZ] improves the strong hydrogen network connectivity by introducing anisotropy in the hydrogen network through a specific doping pattern. These design principles and associated model structures provide flexibility to optimize both T_cand the structural stability of complex hydrides. 

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5. Epitaxial AlBN/β‐Nb ₂ N Ferroelectric/Superconductor Heterostructures

   https://doi.org/10.1002/pssr.202400157  

   Savant, Chandrashekhar; Nguyen, Thai‐Son; Vishwakarma, Saurabh; Lee, Joongwon; Ithepalli, Anand; Chen, Yu‐Hsin; Nomoto, Kazuki; Rana, Farhan; Smith, David J; Xing, Huili Grace; et al (November 2024, physica status solidi (RRL) – Rapid Research Letters)

   We report the growth of AlBN/β‐Nb₂N nitride epitaxial heterostructures in which the AlBN is ferroelectric, and β‐Nb₂N with metallic resistivity ≈40 μ at 300 K becomes superconducting belowT_C ≈ 0.5 K. Using nitrogen plasma molecular beam epitaxy, we grow hexagonal β‐Nb₂N films on c‐plane Al₂O₃substrates, followed by wurtzite AlBN. The AlBN is in epitaxial registry and rotationally aligned with the β‐Nb₂N, and the hexagonal lattices of both nitride layers make angles of 30° with the hexagonal lattice of the Al₂O₃substrate. The B composition of the AlBN layer is varied from 0 to 14.7%. It is found to depend weakly on the B flux, but increases strongly with decreasing growth temperature, indicating a reaction rate‐controlled growth. The increase in B content causes a non‐monotonic change in the a‐lattice constant and a monotonic decrease in the c‐lattice constant of AlBN. Sharp, abrupt epitaxial AlBN/β‐Nb₂N/Al₂O₃heterojunction interfaces and close symmetry matching are observed by transmission electron microscopy. The observation of ferroelectricity and superconductivity in epitaxial nitride heterostructures opens avenues for novel electronic and quantum devices. 

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