arXiv subjects

Jacob T. Baillie

Publications and source records attributed to Jacob T. Baillie.

3 recordsLinked to original sources

arXiv2026

The Impact of Magnons, Defects, and Rapid Energy Migration on the Optical Properties of the 2D Magnet CrPS4

Strong coupling between optical and magnetic excitations could enable contactless, spatially resolved, or ultrafast interrogation and control of magnetism in two-dimensional (2D) materials and devices. The layered 2D A-type antiferromagnet CrPS4 stands out among van der Waals (vdW) magnets for its rich optical fine structure, but its spectroscopy is not yet understood and has so far been interpreted without consideration of magnetic exchange. Here, we show that this fine structure comes primarily from exchange-mediated coupling between on-site optical "spin-flip" transitions of Cr3+ and low-energy spin transitions involving the surrounding lattice. Well-resolved magnon sidebands to optical 4A2 <--> 2E transitions are observed in photoluminescence (PL) and PL excitation spectra, as well as a pronounced PL sideband due to short-range exchange splitting. Energy migration is probed using Yb3+ dopants as traps, revealing sub-picosecond inter-site excitation hopping. Formation of dispersive Frenkel excitons of coupled on-site d-d transitions due to inter-site exchange is discussed. In addition to impacting how optical fine structure is interpreted in this and potentially other vdW magnets, these findings may have ramifications for future applications of layered 2D magnets by revealing new opportunities to drive mode-specific spin-wave excitations using light.

cond-mat.mtrl-sci↗

arXiv2025

Hydrothermal Synthesis of Ultra-high Aspect Ratio $β$-NaYF Disks via Methyliminodiacetic Acid (MIDA)

The hexagonal $β$-phase of sodium yttrium fluoride (NaYF) is a leading host material for lanthanide upconversion and anti-Stokes fluorescence laser refrigeration based on its low phonon energies and high upconversion efficiency. Recently experiments have been proposed to use this material as an optically-levitated sensor of high-frequency gravitational waves. In order to maximize signal-to-noise in this experiment, the NaYF sensor must have both a two-dimensional, disk-like morphology and also a large mass. Here we report a novel hydrothermal process based on the chelation ligand methylimidodiacetic acid (MIDA) to realize hexagonal $β$-NaYF prisms with corner-to-corner diameters up to 44 $\mathrm{μm}$ while keeping the height around 1 $\mathrm{μm}$. The surface quality is comparable to particles synthesized with EDTA based on atomic force microscopy (AFM) measurements. Unlike particles synthesized with EDTA the $β$-NaYF particles show no lensing based on curvature of the hexagonal basal plane. Single crystal X-ray diffraction data were refined to the P-62c (#190) space group which to the best of our knowledge has not been reported in the literature. One of six 44 $\mathrm{μm}$ $β$-NaYF disks doped with 10% ytterbium showed laser refrigeration of ($-4.9 \pm 1.0$) K suggesting future applications in both levitated optomechanics and microoptics.

cond-mat.mtrl-sci↗

arXiv2025

Optical Spin Sensing and Metamagnetic Phase Control in the 2D Van der Waals Magnet Yb3+-Doped CrPS4

The emergence of two-dimensional magnets within the van der Waals toolkit has introduced unprecedented opportunities to develop ultrathin spintronic technologies. Strong coupling between spin and optical properties in such materials can further enable novel spin-photonic capabilities of both fundamental and technological interest. Here, we investigate the optical and spin properties of the air-stable, layered A-type antiferromagnet chromium thiophosphate (CrPS4) when doped with Yb3+. We show that the collective spin properties of CrPS4 are encoded in the sharp f-f luminescence of isolated Yb3+ dopants via strong magnetic superexchange coupling between the two, and that spontaneous magnetic ordering in CrPS4 induces large exchange splittings in the narrow Yb3+ f-f photoluminescence features below TN. Spin reorientation in CrPS4 via a "spin-flop" metamagnetic transition modulates the Yb3+ f-f luminescence energies and exchange splittings. This pronounced link between spin and optical properties enables the demonstration of optically driven spin-flop transitions in CrPS4.

cond-mat.mtrl-sci↗