Search Results (11)

The film thickness, temperature, substrate and doping dependence of the phonon energy $\omega$ and damping $\gamma$, as well as the electrical conductivity, of pure and Sr-doped LaMnO₃ thin films near the phase transition temperature $T_N$ are investigated using a microscopic model and the Green’s function technique. Due to the strong spin–phonon interaction, there appears a kink at $T_N$ in the temperature dependence of $\omega \left(T\right)$ and $\gamma \left(T\right)$. The softening and hardening of the $\omega$ = 495 cm⁻¹ (A_1g) and $\omega$ = 614 cm⁻¹ (B_2g) modes is explained by the different sign of the anharmonic spin–phonon interaction constant R. The damping increases with T for both cases because it is proportional to $R^2$. $\omega$ decreases whereas $\gamma$ increases with an increasing Sr concentration. This is due to the strain caused by the difference between the ionic radii of the La and Sr ions. The film thickness dependence is also considered. $\omega$ and $\gamma$ increase strongly with the decreasing film thickness. The electrical conductivity is enhanced after the doping of the LMO thin films with Sr, which could be used for energy storage applications. The observed results are in good qualitative agreement with the experimental data. Full article

YSZ is a promising material for resistive memory devices due to its high concentration of oxygen vacancies, which provide the high anion migration rates crucial for the manifestation of resistance switching in metal oxides. Therefore, investigating the ionic conductivity of YSZ is an important issue. The ionic conductivity and thermal stability of 8 mol% YSZ were studied using the theories and methods of solid-state physics and physical chemistry. The impact of anomalous atomic vibrations on the material was also explored, and the variation in the ion vibration frequency, electrical conductivity, and thermal stability coefficient of electrical conductivity with temperature was obtained. The results show that the ion conductivity of an 8 mol% YSZ solid electrolyte increases nonlinearly with temperature, with a smaller increase at lower temperatures and a larger increase at higher temperatures. Considering the anharmonic effect of ion vibrations, the electrolyte conductivity is higher than the result of the harmonic approximation, and the anharmonic effect becomes more significant at higher temperatures. Our research fills the gap in the current literature regarding the theoretical non-harmonic exploration of the ion conductivity and thermal stability factor of YSZ solid electrolytes. These results provide valuable theoretical guidance for the development and application of high-performance YSZ resistive memory devices in high-temperature environments. Full article

By applying the WKB (Wentzel, Kramers, Brillouin) approximation, we search for bound state solutions to the time-independent Schrödinger equation for an attractive inverse-square potential and anharmonic oscillators that stem from the interaction of a point charge with radial electric fields. We focus on the bound states associated with the s-waves. Further, we obtain the revival time associated with each case studied. Full article

Contemporary design of new organic non-linear optical (NLO) materials relies to a large extent on the understanding of molecular and electronic structure–property relationships revealed during the years by available computational approaches. The progress in theory—hand-in-hand with experiment—has enabled us to identify and analyze various physical aspects affecting the NLO responses, such as the environmental effects, molecular vibrations, frequency dispersion, and system dynamics. Although it is nowadays possible to reliably address these effects separately, the studies analyzing their mutual interplay are still very limited. Here, we employ density functional theory (DFT) methods in combination with an implicit solvent model to examine the solvent effects on the electronic and harmonic as well as anharmonic vibrational contributions to the static first hyperpolarizability of a series of push–pull $\alpha$,$\omega$-diphenylpolyene oligomers, which were experimentally shown to exhibit notable second-order NLO responses. We demonstrate that the magnitudes of both vibrational and electronic contributions being comparable in the gas phase significantly increase in solvents, and the enhancement can be, in some cases, as large as three- or even four-fold. The electrical and mechanical anharmonic contributions are not negligible but cancel each other out to a large extent. The computed dynamic solute NLO properties of the studied systems are shown to be in a fair agreement with those derived from experimentally measured electric-field-induced second-harmonic generation (EFISHG) signals. Our results substantiate the necessity to consider concomitantly both solvation and vibrational effects in modeling static NLO properties of solvated systems. Full article

By combining density functional theory, quantum theory of atoms in molecules and transport properties calculations, we evaluated the thermoelectric properties of Sb-S system compounds and shed light on their relationships with electronic structures. The results show that, for Sb₂S₃, the large density of states (DOS) variation induces a large Seebeck coefficient. Taking into account the long-range weak bonds distribution, Sb₂S₃ should exhibit low lattice thermal conductivity. Therefore, Sb₂S₃ is promising for thermoelectric applications. The insertion of Be atoms into the Sb₂S₃ interstitial sites demonstrates the electrical properties and Seebeck coefficient anisotropy and sheds light on the understanding of the role of quasi-one-dimensional structure in the electron transport. The large interstitial sites existing in SbS₂ are at the origin of phonons anharmonicity which counteracts the thermal transport. The introduction of Zn and Ga atoms into these interstitial sites could result in an enhancement of all the thermoelectric properties. Full article

The standard D-G-2D pattern of Raman spectra of sp² amorphous carbons is considered from the viewpoint of graphene domains presenting their basic structure units (BSUs) in terms of molecular spectroscopy. The molecular approximation allows connecting the characteristic D-G doublet spectra image of one-phonon spectra with a considerable dispersion of the C=C bond lengths within graphene domains, governed by size, heteroatom necklace of BSUs as well as BSUs packing. The interpretation of 2D two-phonon spectra reveals a particular role of electrical anharmonicity in the spectra formation and attributes this effect to a high degree of the electron density delocalization in graphene domains. A size-stimulated transition from molecular to quasi-particle phonon consideration of Raman spectra was experimentally traced, which allowed evaluation of a free path of optical phonons in graphene crystal. Full article

We have investigated caesium hydrogen sulfate, CsHSO₄, in all three of its ambient pressure phases by total scattering neutron diffraction, inelastic neutron scattering (INS) and Raman spectroscopies and periodic density functional theory calculations. Above 140 °C, CsHSO₄ undergoes a phase transition to a superprotonic conductor that has potential application in intermediate temperature fuel cells. Total scattering neutron diffraction data clearly show that all the existing structures of this phase are unable to describe the local structure, because they have either partial occupancies of the atoms and/or non-physical O–H distances. Knowledge of the local structure is crucial because it is this that determines the conduction mechanism. Starting from one of the previous models, we have generated a new structure that has no partial occupancies and reasonable O–H distances. After geometry optimisation, the calculated radial distribution function is in reasonable agreement with the experimental data, as are the calculated and observed INS and Raman spectra. This work is particularly notable in that we have measured INS spectra in the O–H stretch region above room temperature, which is extremely rare. The INS spectra have the enormous advantage that the electrical anharmonicity that complicates the infrared spectra is absent and the stretch modes are plainly seen. Full article

Metal oxide gas sensors generally need to be operated at elevated temperatures, up to and above 400 °C. Following the need for miniaturization of gas sensors and implementation into smart devices such as smartphones or wireless sensor nodes, recently complementary metal-oxide-semiconductor (CMOS) process-based micro electromechanical system (MEMS) platforms (micro-hotplates, µhps) have been developed to provide Joule heating of metal oxide sensing structures on the microscale. Heating precision and possible spatial temperature distributions over the µhp are key issues potentially affecting the performance of the overall gas sensor device. In this work, we use Raman spectroscopy to directly (in-situ and in-operando) measure the temperature of CMOS-based µhps during the application of electric current for Joule heating. By monitoring the position of the Raman mode of silicon and applying the theoretical framework of anharmonic phonon softening, we demonstrate that state-of-the-art µhps are able to reach the set temperature with an error below 10%, albeit with significant spatial temperature variations on the hotplate. This work demonstrates the potential of Raman spectroscopy for in-situ and in-operando temperature measurements on Si-based devices, an aspect of high relevance for micro- and nano-electronic device producers, opening new possibilities in process and device control. Full article

Recently, Cu-containing p-type Bi_0.5Sb_1.5Te₃ materials have shown high thermoelectric performances and promising prospects for practical application in low-grade waste heat recovery. However, the position of Cu in Bi_0.5Sb_1.5Te₃ is controversial, and the roles of Cu in the enhancement of thermoelectric performance are still not clear. In this study, via defects analysis and stability test, the possibility of Cu intercalation in p-type Bi_0.5Sb_1.5Te₃ materials has been excluded, and the position of Cu is identified as doping at the Sb sites. Additionally, the effects of Cu dopants on the electrical and thermal transport properties have been systematically investigated. Besides introducing additional holes, Cu dopants can also significantly enhance the carrier mobility by decreasing the Debye screen length and weakening the interaction between carriers and phonons. Meanwhile, the Cu dopants interrupt the periodicity of lattice vibration and bring stronger anharmonicity, leading to extremely low lattice thermal conductivity. Combining the suppression on the intrinsic excitation, a high thermoelectric performance—with a maximum thermoelectric figure of merit of around 1.4 at 430 K—has been achieved in Cu_0.005Bi_0.5Sb_1.495Te₃, which is 70% higher than the Bi_0.5Sb_1.5Te₃ matrix. Full article

Outstanding electrical properties of solids are often due to the composition heterogeneity and/or the competition between two or more sublattices. This is true for superionic and superprotonic conductors and supraconductors, as well as for many ferroelectric materials. As in PLZT ferroelectric materials, the exceptional ferro- and piezoelectric properties of the PMN-PT ((1−x)PbMg_1/3Nb_2/3O₃−xPbTiO₃) solid solutions arise from the coexistence of different symmetries with long and short scales in the morphotropic phase boundary (MPB) region. This complex physical behavior requires the use of experimental techniques able to probe the local structure at the nanoregion scale. Since both Raman signature and thermal expansion behavior depend on the chemical bond anharmonicity, these techniques are very efficient to detect and then to analyze the subtitle structural modifications with an efficiency comparable to neutron scattering. Using the example of poled (field cooling or room temperature) and unpoled PMN-PT single crystal and textured ceramic, we show how the competition between the different sublattices with competing degrees of freedom, namely the Pb-Pb dominated by the Coulombian interactions and those built of covalent bonded entities (NbO₆ and TiO₆), determine the short range arrangement and the outstanding ferro- and piezoelectric properties. Full article

The oscillation frequencies of charged particles in a Penning trap can serve as sensors for spectroscopy when additional field components are introduced to the magnetic and electric fields used for confinement. The presence of so-called “magnetic bottles” and specific electric anharmonicities creates calculable energy-dependences of the oscillation frequencies in the radiofrequency domain which may be used to detect the absorption or emission of photons both in the microwave and optical frequency domains. The precise electronic measurement of these oscillation frequencies therefore represents an optical sensor for spectroscopy. We discuss possible applications for precision laser and microwave spectroscopy and their role in the determination of magnetic moments and excited state lifetimes. Also, the trap-assisted measurement of radiative nuclear de-excitations in the X-ray domain is discussed. This way, the different applications range over more than 12 orders of magnitude in the detectable photon energies, from below μeV in the microwave domain to beyond MeV in the X-ray domain. Full article