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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 $T_N∼25\mathrm{K}$ 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

Abstract:

We demonstrate a novel defect-mediated, thermally-activated emission mechanism in [(CH3)3NPh]2MnBr4 single crystals, driven by the coexistence of temperature-sensitive shallow traps and temperature-independent deep traps introduced by Br vacancies. Through comprehensive temperature-dependent photoluminescence (PL) and time-resolved PL measurements, combined with first-principles calculations, we reveal that the material exhibits exceptional thermal stability, retaining 67 % of its relative PL quantum yield at room temperature and achieving an absolute quantum yield of ∼38.9 % under optimal excitation conditions. The dual-component PL decay dynamics consist of a fast decay (∼hundreds of ps) governed by shallow traps and a long decay (∼350 μs) dominated by deep traps, creating an energy cascade that efficiently promotes radiative recombination while minimizing non-radiative losses. Our findings provide critical insights into defect-mediated, thermally-sensitive delayed emission mechanisms and establish [(CH3)3NPh]2MnBr4 as a lead-free, thermally stable material with high efficiency, making it an excellent candidate for next-generation optoelectronic applications, including solid-state lighting and temperature-sensitive devices.

Abstract:

High-resolution spectroscopy unveils the fundamental physics of quantum states, molecular dynamics, and energy transfers. Ideally, a higher spectral resolution over a broader bandwidth is the prerequisite, but traditional spectroscopic techniques can only partially fulfill this requirement even with a bulky system. Here we report that a multi-frequency acousto-optic phase modulation at a chip-scale of soft polydimethylsiloxane can readily 91̽»¨ a 200-times higher 0.5-MHz spectral resolution for the frequency-comb-based spectroscopy, while co-located plasmonic nanostructures mediate the strong light-matter interaction. These results suggest the potential of polydimethylsiloxane acousto-optic phase modulation for cost-effective, compact, multifunctional chip-scale tools in diverse applications such as quantum spectroscopy, high-finesse cavity analysis, and surface plasmonic spectroscopy.

Abstract:

Semiconductor photonic nanowires are critical components for nanoscale light manipulation in integrated photonic and electronic devices. Optimizing their optical performance requires enhanced photon conversion efficiency, for which a promising solution is to combine semiconductors with noble metals, using the surface plasmon resonance of noble metals to enhance the photon absorption efficiency. Here, we report plasmon-enhanced light emission in a hybrid nanowire device composed of perovskite semiconductor nanowires and silver nanoparticles formed using superfluid helium droplets. A cesium lead halide perovskite-based four-layer structure (CsPbBr3/PMMA/Ag/Si) effectively reduces the metal’s plasmonic losses while ensuring efficient surface plasmon–photon coupling at moderate power. Microphotoluminescence and time-resolved spectroscopy techniques are used to investigate the optical properties and emission dynamics of carriers and excitons within the hybrid device. Our results demonstrate an intensity enhancement factor of 29 compared with pure semiconductor structures at 4 K, along with enhanced carrier recombination dynamics due to plasmonic interactions between silver nanoparticles and perovskite nanowires. This work advances existing approaches for exciting photonic nanowires at low photon densities, with potential applications in optimizing single-photon excitations and emissions for quantum information processing.