Temperature-dependent UV-Vis dielectric functions of BaTiO3 across ferroelectric-paraelectric phase transition.

Ferroelectric BaTiO3 with an electric-field-switchable spontaneous polarization has attracted wide attention in photovoltaic applications due to its efficient charge separation for photoexcitation. The evolution of its optical properties with rising temperature especially across the ferroelectric-paraelectric phase transition is critical to peer into the fundamental photoexcitation process. Herein, by combining spectroscopic ellipsometry measurements with first-principles calculations, we obtain the UV-Vis dielectric functions of perovskite BaTiO3 at temperatures varying from 300 to 873 K and provide the atomistic insights into the temperature-driven ferroelectric-paraelectric (tetragonal-cubic) structural evolution. The main adsorption peak in dielectric function of BaTiO3 is reduced by 20.6% in magnitude and redshifted as temperature increases. The Urbach tail shows an unconventional temperature-dependent behavior due to the microcrystalline disorder across the ferroelectric-paraelectric phase transition and the decreased surface roughness at around 405 K. From ab initio molecular dynamics simulations, the redshifted dielectric function of ferroelectric BaTiO3 coincidences with the reduction of the spontaneous polarization at elevated temperature. Moreover, a positive (negative) external electric field is applied which can modulate the dielectric function of ferroelectric BaTiO3 blueshift (redshift) with a larger (smaller) spontaneous polarization since it drives the ferroelectric further away from (closer to) the paraelectric structure. This work sheds light on the temperature-dependent optical properties of BaTiO3 and provides data support for advancing its ferroelectric photovoltaic applications.

Ellipsometric and first-principles study on temperature-dependent UV-Vis dielectric functions of GaN.

The third-generation wide bandgap semiconductor GaN currently occupies a hot spot in the fields of high-power electronics and optoelectronics. Fully exploring its optical and optoelectronic characteristics is of great significance. Here, we provide a systematic study on the temperature-dependent dielectric functions of GaN grown by metal-organic chemical vapor deposition in the spectral range of 0.73-5.90 eV via spectroscopic ellipsometry experiments and first-principles calculations. Ellipsometric measurements identify two typical absorption peaks that originate from the excitonic and phonon-assisted indirect absorption process, respectively. To explore the underlying physics, we perform first-principles calculations using the independent-particle approximation, model Bethe-Salpeter equation (mBSE), and phonon-assisted indirect absorption process (Inabs). In comparison with ellipsometric measurements, the mBSE calculation determines the absorption peak contributed by the many-body excitonic effect, while the Inabs calculation successfully predicts the second absorption peak. When heating the crystal, it observes the redshift and weakening of absorption peaks, intrinsically due to the nontrivial electron-phonon interaction as lattice vibration strengthens. While doping GaN with Fe or Si elements, the introduced free carriers modify the electronic interband transition. As the temperature increases, more free carriers are excited, and the temperature influence on the absorption peak is more significant than that of the undoped one. This work fully explores the physical origins of the temperature and doping effect on UV-Vis dielectric functions of GaN, aiming to promote its application in the fields of high-power electronic devices.

Temperature-induced surface phonon polaritons dissipation in perovskite SrTiO3.

Perovskite SrTiO3 has emerged as a relevant technological material for nano-photonics that confines light to subdiffraction geometry with remarkably wide spectral tunability. Yet, the influence of lattice vibrations on its surface phonon polaritons (SPhPs) and localized surface phonon resonances (LSPhRs) receives little attention, and the underlying physics still remains elusive. Here, we apply spectroscopic ellipsometry (SE) experiments and multiscale simulations spanning from first-principles to finite-difference time-domain (FDTD), and investigate the temperature influence on infrared dielectric functions, SPhPs and LSPhRs of SrTiO3. SE measurements find that the width of the Reststrahlen band lying between transverse and longitudinal oxygen-related optical phonons changes slightly, but infrared dielectric functions vary significantly as temperature increases. First-principles calculations confirm the coupling of the motion of oxygen atoms to incident photons, forming quasiparticles of SPhPs. FDTD simulations show that strong LSPhRs exist at 250 K in the SrTiO3 nanodisks but dissipate as lattice vibration strengthens, mainly due to the reduced phonon relaxation lifetime. This work reveals the underlying physics of temperature influence on SPhPs and LSPhRs of SrTiO3 and helps explore its potential applications as photonic resonators at high temperatures.

SO2 Absorption by Multiple Biomass Ash Types.

As the severity of environmental pollution continues to increase and ultralow emission standards are proposed, biomass power plants must implement additional processes to control SO2 emission. Biomass ash can be utilized as a sorbent for flue gas desulfurization because of its strong alkalinity. In this study, the characteristics of SO2 absorption in simulated flue gas using four types of typical biomass ashes were studied in fixed bed experiments. The results showed that the addition of water, the increase in water vapor, and the lower temperature were beneficial for SO2 absorption. The main components of wheat straw ash are KCl and SiO2, cotton stalk ash is rich in K2O and calcium compounds, poplar bark ash has a considerable content of calcium compounds, and corncob ash contains large amounts of KCl and K2O. Alkali substances, such as oxides or carbonates of potassium and calcium, play a crucial role in SO2 absorption. The SO2 removal effect of corncob ash was the best owing to the abundance of potassium oxides. Meanwhile, wheat straw ash performed worst in SO2 removal due to the small amount of K2O and Ca. The desulfurization products were mainly potassium and calcium sulfate.