arXiv subjects

J. W. Villanova

Publications and source records attributed to J. W. Villanova.

4 recordsLinked to original sources

arXiv2025

Observation of anisotropic dispersive dark exciton dynamics in CrSBr

Many-body excitons in CrSBr are attracting intense interest in view of their highly anisotropic magneto-optical coupling and their potential for novel optical interfaces within spintronic and magnonic devices. Characterizing the orbital character and propagation of these electronic excitations is crucial for understanding and controlling their behavior; however, this information is challenging to access. Ultra-high resolution resonant inelastic x-ray scattering is a momentum-resolved technique that can address these crucial questions. We present measurements collected at the Cr $L_3$-edge which show a rich spectrum of excitations with a variety of spin-orbital characters. While most of these excitations appear to be localized, the dispersion of the lowest energy dark exciton indicates that it is able to propagate along both the $a$ and $b$ directions within the planes of the crystal. This two-dimensional character is surprising as it contrasts with electrical conductivity and the behavior of the bright exciton, both of which are strongly one-dimensional. The discovery of this propagating dark exciton highlights an unusual coexistence of one- and two-dimensional electronic behaviors in CrSBr.

cond-mat.str-el↗

arXiv2025

Dispersive dark excitons in van der Waals ferromagnet CrI3

Spin-flip dark excitons are optical-dipole-forbidden quasiparticles with remarkable potential in optoelectronics, especially when they are realized within cleavable van der Waals materials. Despite this potential, dark excitons have not yet been definitively identified in ferromagnetic van der Waals materials. Here, we report two dark excitons in a model ferromagnetic material CrI3 using high-resolution resonant inelastic x-ray scattering (RIXS) and show that they feature narrower linewidths compared to the bright excitons previously reported in this material. These excitons are shown to have spin-flip character, to disperse as a function of momentum, and to change through the ferromagnetic transition temperature. Given the versatility of van der Waals materials, these excitons hold promise for new types of magneto-optical functionality.

cond-mat.str-el↗

arXiv2023

Non-linear magnons and exchange Hamiltonians of delafossite proximate quantum spin liquids

Quantum spin liquids (QSL) are theoretical states of matter with long-range entanglement and exotic quasiparticles. However, they generally elude quantitative theory, rendering their underlying phases mysterious and hampering efforts to identify experimental QSL states. Here we study triangular lattice resonating valence bond QSL candidate materials KYbSe$_2$ and NaYbSe$_2$. We measure the magnon modes in their 1/3 plateau phase, where quantitative theory is tractable, using inelastic neutron scattering and fit them using nonlinear spin wave theory. We also fit the KYbSe$_2$ heat capacity using high temperature series expansion. Both KYbSe$_2$ fits yield the same magnetic Hamiltonian to within uncertainty, confirming previous estimates and showing the Heisenberg $J_2/J_1$ to be an accurate model for these materials. Most importantly, comparing KYbSe$_2$ and NaYbSe$_2$ shows that smaller $A$-site Na$^+$ ion has a larger $J_2/J_1$ ratio. However, hydrostatic pressure applied to KYbSe$_2$ increases the ordering temperature (a result consistent with density functional theory calculations), indicating that pressure decreases $J_2/J_1$. These results show how periodic table and hydrostatic pressure can tune the $A$YbSe$_2$ materials in a controlled way.

cond-mat.str-el↗

arXiv2023

Spin wave Hamiltonian and anomalous scattering in NiPS$_3$

We report a comprehensive spin wave analysis of the semiconducting honeycomb van der Waal antiferromagnet NiPS$_3$. Using single crystal inelastic neutron scattering, we map out the full Brillouin zone and fit the observed modes to a spin wave model with rigorously defined uncertainty. We find that the third neighbor exchange $J_3$ dominates the Hamiltonian, a feature which we fully account for by ab-initio density functional theory calculations. We also quantify the degree to which the three-fold rotation symmetry is broken and account for the $Q=0$ excitations observed in other measurements, yielding a spin exchange model which is consistent across multiple experimental probes. We also identify a strongly reduced static ordered moment and reduced low-energy intensity relative to the linear spin wave calculations, signaling unexplained features in the magnetism which requires going beyond the linear spin wave approximation.

cond-mat.str-el↗