Synthesis and crystal growth

Abstract:

Understanding how light modifies long-range order in quantum materials is key to improving our ability to control functionality. However, this is challenging if the response is heterogeneous. Here we address the most common form of light-induced heterogeneity-surface melting-and measure the dynamics of orbital order in the layered manganite La_0.5Sr_1.5MnO₄. We isolate the surface dynamics from the bulk by measuring the orbital truncation rod and orbital Bragg peak. After photoexcitation, the orbital Bragg peak shows an unusual narrowing, which suggests an increase in correlation length of the probed volume. By contrast, the correlation length at the surface decreases. These differences can be reconciled if the material is heterogeneous, and light melts a less ordered surface. By isolating the surface response, we determine that the loss of long-range order is an incoherent process, which is probably accompanied by the formation of local polarons.

Abstract:

Ultrafast switching of ferroic phases is an active research area with technological potential. Yet, some key challenges remain, ranging from limited speeds in ferromagnets to intrinsic volatility of switched domains owing to depolarizing fields in ferroelectrics. Unlike these ferroic systems, ferroaxial materials host bistable states that preserve spatial-inversion and time-reversal symmetry and are therefore immune to depolarizing fields but also difficult to manipulate with conventional methods. We demonstrate photo-induced switching of ferroaxial order by engineering an effective axial field composed of circularly driven terahertz phonon modes. A switched ferroaxial domain remains stable for many hours and can be reversed back with a second terahertz pulse of opposite helicity. The effects demonstrated in this work may lead to the development of a robust platform for ultrafast information storage.

Abstract:

Photocatalytic ammonia decomposition offers a sustainable route for hydrogen production, but its development is limited by low catalytic efficiency and poorly understood mechanisms. Here, a protonated layered perovskite, HPrNb2O7 (HPNO), is reported as an efficient catalyst for ammonia decomposition under mild photo‐thermal conditions. Upon exposure to NH3 at elevated temperatures, HPNO promotes the in situ formation and intercalation of hydrazine intermediates within its interlayer galleries, enabled by thermally generated oxygen vacancies and hydrogen bonding. Advanced characterization techniques have been applied to confirm the formation and stabilization of hydrazine. It is also shown that thermal energy prolongs charge carrier lifetimes and enhances oxygen vacancy formation, contributing to a strong photo‐thermal synergy. The stabilization of hydrazine intermediate promotes the associative mechanism, lowering the activation barrier, thus leading to an enhanced hydrogen evolution rate of 1311.2 µmol·g−1·h−1 at 200 °C under simulated solar irradiation without any noble metal co‐catalyst. This work reveals a distinct, hydrazine‐mediated reaction pathway and positions layered protonated perovskites as promising materials for efficient, solar‐driven ammonia decomposition and sustainable hydrogen generation.

Abstract:

${\text{YbZn}}_2{\mathrm{GaO}}_5$ is a promising candidate for realizing a quantum spin liquid (QSL) state, particularly owing to its lack of significant site disorder. Pulsed-field magnetometry at 0.5 K shows magnetization saturating near 15 T, with a corrected saturation moment of $2.1(1){\mu }_{\mathrm{B}}$ after subtracting the van Vleck contribution. Our zero-field $\mathrm{\mu }\mathrm{SR}$ measurements down to milliKelvin temperatures provide evidence for a dynamic ground state and the absence of magnetic order. To probe fluctuations in the local magnetic field at the muon site, we performed longitudinal field $\mathrm{\mu }\mathrm{SR}$ experiments. These results provide evidence for spin dynamics with a field dependence that is consistent with a U1A01 Dirac quantum spin liquid as a plausible description of the ground state.

Abstract:

${\text{CoTi}}_2{\mathrm{O}}_5$ has the paradox that low temperature static magnetic order is incompatible with the crystal structure owing to a mirror plane that exactly frustrates magnetic interactions. Despite no observable structural distortion with diffraction, ${\text{CoTi}}_2{\mathrm{O}}_5$ does magnetically order below $T_N\sim 25\mathrm{K}$ with the breaking of spin ground state degeneracy proposed to be a realization of the spin Jahn-Teller effect in analogy to the celebrated orbital Jahn-Teller transition. We apply neutron and Raman spectroscopy to study the dynamics of this transition in ${\text{CoTi}}_2{\mathrm{O}}_5$ . We find anomalous acoustics associated with a symmetry breaking strain that characterizes the spin Jahn-Teller transition. Crucially, the energy of this phonon coincides with the energy scale of the magnetic excitations, and has the same symmetry of an optic mode, observed with Raman spectroscopy, which atypically softens in energy with decreasing temperature. Taken together, we propose that the energetics of the spin Jahn-Teller effect in ${\text{CoTi}}_2{\mathrm{O}}_5$ are related to cooperative magnetoelastic fluctuations as opposed to conventional soft critical dynamics which typically drive large measurable static displacements. Published by the American Physical Society 2025