The broken symmetry in the atomic-scale ordering of glassy versus crystalline solids leads to a daunting challenge to provide suitable metrics for describing the order within disorder, especially on length scales beyond the nearest neighbor that are characterized by rich structural complexity. Here, we address this challenge for silica, a canonical network-forming glass, by using hot versus cold compression to (i) systematically increase the structural ordering after densification and (ii) prepare two glasses with the same high-density but contrasting structures. The structure was measured by high-energy X-ray and neutron diffraction, and atomistic models were generated that reproduce the experimental results. The vibrational and thermodynamic properties of the glasses were probed by using inelastic neutron scattering and calorimetry, respectively. Traditional measures of amorphous structures show relatively subtle changes upon compacting the glass. The method of persistent homology identifies, however, distinct features in the network topology that change as the initially open structure of the glass is collapsed. The results for the same high-density glasses show that the nature of structural disorder does impact the heat capacity and boson peak in the low-frequency dynamical spectra. Densification is discussed in terms of the loss of locally favored tetrahedral structures comprising oxygen-decorated SiSi4 tetrahedra.
We performed terahertz time-domain spectroscopy, low-frequency Raman scattering, and Brillouin light scattering on vitreous glucose to investigate the boson peak (BP) dynamics. In the spectra of is the absorption coefficient], the BP is clearly observed around 1.1 THz. Correspondingly, the complex dielectric constant spectra show a universal resonancelike behavior only below the BP frequency. As an analytical scheme, we propose the relative light-vibration coupling coefficient (RCC), which is obtainable from the combination of the far-infrared and Raman spectra. The RCC reveals that the infrared light-vibration coupling coefficient of the vitreous glucose behaves linearly on frequency which deviates from Taraskin's model of [S. N. Taraskin et al., Phys. Rev. Lett. 97, 055504 (2006)]. The linearity of might require modification of the second term of the model. The measured transverse sound velocity shows an apparent discontinuity with the flattened mode observed in the inelastic neutron scattering study [N. Violini et al., Phys. Rev. B 85, 134204 (2012)] and suggests a coupling between the transverse acoustic and flattened modes.
Ultrafast control of magnets using femtosecond light pulses attracts interest regarding applications and fundamental physics of magnetism. Antiferromagnets are promising materials with magnon frequencies extending into the terahertz range. Visible or near-infrared light interacts mainly with the electronic orbital angular momentum. In many magnets, however, in particular with iron-group ions, the orbital momentum is almost quenched by the crystal field. Thus, the interaction of magnons with light is hampered, because it is only mediated by weak unquenching of the orbital momentum by spin–orbit interactions. Here we report all-optical excitation of magnons with frequencies up to 9 THz in antiferromagnetic CoO with an unquenched orbital momentum. In CoO, magnon modes are coupled oscillations of spin and orbital momenta with comparable amplitudes. We demonstrate excitations of magnon modes by directly coupling light with electronic orbital angular momentum, providing possibilities to develop magneto-optical devices operating at several terahertz with high output-to-input ratio.
The development of dielectric materials with colossal permittivity is important for the miniaturization of electronic devices and fabrication of high-density energy-storage devices. The electron-pinned defect-dipoles has been recently proposed to boost the permittivity of (Nb + In) co-doped TiO2 to 105. However, the follow-up studies suggest an extrinsic contribution to the colossal permittivity from thermally excited carriers. Herein, we demonstrate a marked enhancement in the permittivity of (Nb + In) co-doped TiO2 single crystals at sufficiently low temperatures such that the thermally excited carriers are frozen out and exert no influence on the dielectric response. The results indicate that the permittivity attains quadruple of that for pure TiO2. This finding suggests that the electron-pinned defect-dipoles add an extra dielectric response to that of the TiO2 host matrix. The results offer a novel approach for the development of functional dielectric materials with large permittivity by engineering complex defects into bulk materials.
We report anomalous circularly polarized Raman spectra of phonons in right- and left-handed quartzes. The phonon branches splitting from the -mode at a finite wave number were found to be chiral with mutually opposite angular momenta. Our analysis reveals the Raman selection rules for chiral phonons. We also find that the conservation of angular momentum should be satisfied between two photons and one chiral phonon in the Raman process. Furthermore, we experimentally proved that the helicity of phonons with a certain frequency and wave vector should be opposite in the other enantiomer.