Polar Optical Phonons Research Articles

Tl2XY (X, Y = S, Se) monolayers with low lattice thermal conductivity and high thermoelectric performance by full-band approach with four scattering mechanisms

Abstract The low lattice thermal conductivity and high thermoelectric performance of the Janus Tl2SSe monolayer in the temperature region of 300~700 K are identified based on the thermoelectric properties of the Tl2S2, Tl2SSe, and Tl2Se2 monolayers. The transport coefficients for carrier concentrations and temperatures are obtained by solving the linearized Boltzmann transport equation in a full-band electronic structure. Four scattering mechanisms of acoustic deformation potential, optical deformation potential, polar optical phonon, and ionized impurity scatterings are considered. The ionized impurity scattering is recognized as the most important. The lattice thermal conductivity of the Janus Tl2SSe monolayer is substantially smaller than those of the Tl2SSe, Tl2Se2 monolayers with higher symmetry. Moreover, we find that the Janus structures of the Tl2SSe monolayer increase the dielectronic constants and enhance the polar optical phonon scattering, then reduce the power factor to some extent. Therefore, the lattice thermal conductivity actually couples with the transport coefficient and cannot be individually regulated as is usually assumed. However, the ZT value of the Tl2SSe monolayer can still reach 1.77 at 700 K even if the intrinsic concentration and the bipolar effect are included. Therefore, the Tl2SSe monolayer is expected to be a promising candidate for thermoelectric materials.

Dynamical Manipulation of Polar Topologies from Acoustic Phonon Excitations.

Since the recent discovery of polar topologies, a recurrent question has been how to remotely tune them. Many efforts have focused on the pumping of polar optical phonons from optical methods, but with limited success, as only switching between specific phases has been achieved so far. Additionally, the correlation between optical pulse characteristics and the resulting phase is poorly understood. Here, we propose an alternative approach and demonstrate the deterministic and dynamical tailoring of polar topologies using acoustic phonon excitations. Our second-principles simulations reveal that by pumping specific longitudinal and transverse acoustic phonons, various topological textures can be induced in materials like BaTiO3 or PbTiO3. This method leverages the strong coupling between polarization and strain in these materials, enabling predictable and dynamic control of polar patterns. Our findings open up an alternative possibility for the manipulation of polar textures, suggesting a promising research direction.

Carrier scattering and temperature characteristics of mobility and resistivity of Fe-doped GaN

Abstract The electron mobility and dark resistivity of Fe-doped semi-insulating GaN (GaN:Fe) are calculated over the temperature range from 10 K to 500 K by considering the impurities compensation mechanism and majority carrier scattering. The temperature characteristic curve of the mobility exhibits unimodality and the curve of resistivity decreases monotonically with rising temperature. The carrier scatterings induced by ionized impurities, acoustic deformation potential, piezoelectric, and polar optical phonons are analyzed. It is found that the mobility is determined by ionized impurity scattering, piezoelectric scattering, and polar optical phonon scattering in different temperature ranges, and the contribution of acoustic deformation potential scattering is negligible over the entire temperature range. Furthermore, the effects of concentrations of shallow donors and deep acceptors on the temperature characteristic curves of mobility and resistivity, the peak mobility and its corresponding temperature (peak temperature), and the mobility and resistivity at room temperature are discussed. Our simulation shows the calculation results agree very well with the reported experimental and theoretical results when the Fe-related level is selected as 0.58 eV below the conduction band edge. Understanding of thermal properties of dark resistivity and mobility can be useful for optimizing GaN:Fe-based electronic and photonic devices performance in different temperature regimes.

Probing carrier transport of sphalerite Cadmium Chalcogenide (CdX, X=S, Se) from first-principles

Cadmium chalcogenide (CdX, X=S, Se) traps photons in the visible and near-infrared regions, and it has been widely used in optoelectronic devices such as solar cells and light-emitting diodes. The carrier concentration and intrinsic mobility are prerequisites for the optimized design of optoelectronic devices, while the underlying physics that determines the carrier mobility of sphalerite CdX remains elusive. Herein, we explore the temperature-dependent carrier transport properties and scattering mechanisms of sphalerite CdX from first-principles. The calculation results indicate that the isotropic electron mobility for CdS and CdSe are 180.2 cm2/Vs and 656.8 cm2/Vs at room temperature, respectively. An in-depth analysis reveals that polar optical phonon (POP) scattering is the main scattering mechanism limiting the mobility of sphalerite CdX, and electrons are mainly affected by long-range longitudinal optical phonon scattering. The lower electron mobility of CdS compared to CdSe is attributed to the larger Fröhlich coupling constant, -larger Pauling ionicity, and stronger electron-phonon interactions. As the temperature rises, the electron mobility of CdX consistently decreases due to the enhancement of POP scattering and lattice vibrations. The electron mobility of CdX at high doping concentrations decreases dramatically, attributing to the enhancement of ionized impurity scattering i.e. collisional scattering of electrons and ionized impurity ions. This work provides a systematic study of the electron transport properties of sphalerite cadmium chalcogenide from first-principles, which provides a theoretical guideline for the functional regulation and improvement of optoelectronic devices.

Insight into the origins of mobility deterioration in indium phosphide-based epitaxial layer

Ultra-high mobility speciality is a critical figure of merit for ultrapure materials and high-speed optoelectronic devices. However, unintentional doping-inducing various scattering frequently deteriorates mobility capacity. Therefore, how to elucidate the origin of mobility deterioration is still an open and technically challenging issue. Here we report that unintentional-doping silicon ion would be propagated into the indium phosphide (InP)’s epitaxial layer via analysis of time-of-flight and dynamic secondary ion mass spectrometry. The unintentional silicon ion in the InP wafer surface is responsible for the subsequent InGaAs epitaxial layer's mobility attenuation. The first-principles calculations and Boltzmann transport theory prove that polar optical phonon scattering (Fröhlich scattering) in non-doping InGaAs is the dominant scattering mechanism at high temperatures over 100 K. In contrast, the low-temperature scattering process is dominated by ionized impurities scattering. The unintentional silicon ion improves the Fröhlich scattering-dominated critical temperature. Our findings provide insight into the mobility degeneration originating from unintentional pollution and underlying scattering mechanisms, which lay a solid foundation for developing high-grade, super-speed, and low-power photoelectronic devices.

Fröhlich Scattering Effects on Electron Mobility in β‐Ga2O3 Power Devices under High Temperature

The impact of Fröhlich scattering on β‐Ga2O3 Schottky barrier diodes (SBDs) electron mobility, particularly at high temperatures, is investigated. This scattering is crucial due to electron–polar optical phonon interactions. Temperature‐dependent I–V characteristics of a β‐Ga2O3 SBD from 300 to 473 K showed significant current reduction due to electron–polar optical phonon scattering, supported by correlation with mobility profiles. Additionally, in situ temperature‐dependent XPS analysis revealed a notable positive shift in core‐level binding energy, attributed to heightened electron–phonon interactions. This study provides crucial insights into carrier transport mechanisms, essential for power device design and operation.

Influence of the Bias Voltage on Effective Electron Velocity in AlGaN/GaN High Electron Mobility Transistors.

The small-signal S parameters of the fabricated double-finger gate AlGaN/GaN high electron mobility transistors (HEMTs) were measured at various direct current quiescent operating points (DCQOPs). Under active bias conditions, small-signal equivalent circuit (SSEC) parameters such as Rs and Rd, and intrinsic parameters were extracted. Utilizing fT and the SSEC parameters, the effective electron velocity (νe-eff) and intrinsic electron velocity (νe-int) corresponding to each gate bias (VGS) were obtained. Under active bias conditions, the influence mechanism of VGS on νe-eff was systematically studied, and an expression was established that correlates νe-eff, νe-int, and bias-dependent parasitic resistances. Through the analysis of the main scattering mechanisms in AlGaN/GaN HEMTs, it has been discovered that the impact of VGS on νe-eff should be comprehensively analyzed from the aspects of νe-int and parasitic resistances. On the one hand, changes in VGS influence the intensity of polar optical phonon (POP) scattering and polarization Coulomb field (PCF) scattering, which lead to changes in νe-int dependent on VGS. The trend of νe-int with changes in VGS plays a dominant role in determining the trend of νe-eff with changes in VGS. On the other hand, both POP scattering and PCF scattering affect νe-eff through their impact on parasitic resistance. Since there is a difference in the additional scattering potential corresponding to the additional polarization charges (APC) between the gate-source/drain regions and the region under the gate, the mutual effects of PCF scattering on the under-gate electron system and the gate-source/drain electron system should be considered when adjusting the PCF scattering intensity through device structure optimization to improve linearity. This study contributes to a new understanding of the electron transport mechanisms in AlGaN/GaN HEMTs and provides a novel theoretical basis for improving device performance.

The scattering lifetime and thermoelectric properties for an inorganic flexible material of α-Ag2S

To clarified the influence of the scattering mechanism on thermoelectric properties α-Ag2S, the relationship between the scattering lifetime and transport properties of the inorganic flexible material α-Ag2S are investigated for the first time using first-principles calculation, Boltzmann transport theory, and the momentum relaxation time approximation (MRTA). Calculations reveal that the static dielectric constant, high frequency dielectric constant, and elastic constant are anisotropic. The acoustic deformation potential scattering (ADP), the ionized impurity scattering (IMP), the piezoelectric scattering (PIE), and the polar optical phonon scattering (POP) of α-Ag2S are first calculated, and the IMP and POP are found to be the major contributions for scattering mechanism. Furthermore, it is also found that the transverse wave of α-Ag2S effects on electrons along the XZ shear strain direction are non-negligible. These insights provide a new direction for the regulation of thermoelectric properties in α-Ag2S by offering a deeper understanding of the scattering mechanisms.

Cooperative dynamic polaronic picture of diamond color centers

Polarons can control carrier mobility and can also be used in the design of quantum devices. Although much effort has been directed into investigating the nature of polarons, observation of defect-related polarons is challenging due to electron-defect scattering. Here we explore the polaronic behavior of nitrogen-vacancy (NV) centers in a diamond crystal using an ultrafast pump-probe technique. A 10-fs optical pulse acts as a source of high electric field exceeding the dielectric breakdown threshold, in turn exerting a force on the NV charge distribution and polar optical phonons. The electronic and phononic responses are enhanced by an order of magnitude for a low density of NV centers, which we attribute to a combination of cooperative polaronic effects and scattering by defects. First-principles calculations support the presence of dipolar Fröhlich interaction via non-zero Born effective charges. Our findings provide insights into the physics of color centers in diamonds.

Few-layer Bi2O2Se: a promising candidate for high-performance near-room-temperature thermoelectric applications

Advancements in high-temperature thermoelectric (TE) materials have been substantial, yet identifying promising near-room-temperature candidates for efficient power generation from low-grade waste heat or TE cooling applications has become critical but proven exceedingly challenging. Bismuth oxyselenide (Bi2O2Se) emerges as an ideal candidate for near-room-temperature energy harvesting due to its low thermal conductivity, high carrier mobility and remarkable air-stability. In this study, the TE properties of few-layer Bi2O2Se over a wide temperature range (20-380 K) are investigated, where a charge transport mechanism transitioning from polar optical phonon to piezoelectric scattering at 140 K is observed. Moreover, the Seebeck coefficient (S) increases with temperature up to 280 K then stabilizes at∼-200μV K-1through 380 K. Bi2O2Se demonstrates high mobility (450 cm2V-1s-1) within the optimum power factor (PF) window, despite itsT-1.25dependence. The high mobility compensates the minor reduction in carrier densityn2Dhence contributes to maintain a robust electrical conductivity∼3 × 104S m-1. This results in a remarkable PF of 860μW m-1K-2at 280 K without the necessity for gating (Vg= 0 V), reflecting the innate performance of the as-grown material. These results underscore the considerable promise of Bi2O2Se for room temperature TE applications.

First-principles study of phase-dependent carrier transport mechanism for MASnI3 Sn-based halide perovskite

Organic-inorganic hybrid perovskites have attracted tremendous attentions owing to their excellent properties as next-generation photovoltaic devices. With soft covalent framework, organic-inorganic hybrid perovskites exhibit different phases at different temperatures. The band-edge features of perovskites are mainly contributed by inorganic framework, which means the structural differences between these phases would lead to complex carrier transport. We investigated the carrier transport of Sn-based organic-inorganic hybrid perovskite CH3NH3SnI3 (MASnI3), considering acoustic deformation potential scattering, ionized impurity scattering, and polar optical phonon scattering. It is found that the electron mobility of each phase of MASnI3 is strongly correlated with the Sn–I–Sn bond angle and there is in-plane/out-of-plane anisotropy. The projected crystal orbital Hamilton population analysis suggested that the tilt and rotation of the [SnI6]4− octahedron influence the Sn(p)–I(p) orbital electron coupling and the electron transport, leading to different band-edge features in multiple phases. The carrier mobility with respect to temperature was further calculated for each phase of MASnI3 in respective temperature intervals, showing lower carrier mobility in high temperature. Comparing the contribution of different scattering mechanisms, it was found that the dominant scattering mechanism is polar optical phonon scattering, while multiple scattering mechanisms compete in individual cases.

Correlating the electronic structures of β-Ga2O3 to its crystal tilts induced defects at nanoscale

Crosslinking structural transformation mechanism at nanoscale to the corresponding anisotropically electronic properties is essential to both the atomic-level controlled synthesis and extreme-conditional applications of the ultrawide bandgap semiconductors. Here, we report the first direct observation of bandgap variation at certain microstructural flaws in monoclinic crystal β-Ga2O3 via scanning transmission electron microscopy-electron energy loss spectrum (STEM-EELS) technology with both high energy and spatial resolution. Atomic-scale tilt of the Mosaic blocks relative to [010] zone axis is demonstrated to cause specific point defects accumulation at block boundaries, resulting in the formation of vacancy lines (or clusters) and then the crystal deformation induced flaws. These as-formed tiny Mosaic tilts observed from both in-plane and out-of-plane geometry are correlated to the corresponding electronic structure obtained by density functional calculations, indicating the carrier mobility limits transferred from intrinsic polar optical phonon scattering to the ionized oxygen atoms scattering in the defective monoclinic crystal. These findings provide a new insight on these anisotropic defect formation induced electronic structural variation, paving the way for precise synthesis and development of high-performance ultra-wide bandgap materials.

Phonon screening and dissociation of excitons at finite temperatures from first principles

The properties of excitons, or correlated electron-hole pairs, are of paramount importance to optoelectronic applications of materials. A central component of exciton physics is the electron-hole interaction, which is commonly treated as screened solely by electrons within a material. However, nuclear motion can screen this Coulomb interaction as well, with several recent studies developing model approaches for approximating the phonon screening of excitonic properties. While these model approaches tend to improve agreement with experiment, they rely on several approximations that restrict their applicability to a wide range of materials, and thus far they have neglected the effect of finite temperatures. Here, we develop a fully first-principles, parameter-free approach to compute the temperature-dependent effects of phonon screening within the ab initio [Formula: see text]-Bethe-Salpeter equation framework. We recover previously proposed models of phonon screening as well-defined limits of our general framework, and discuss their validity by comparing them against our first-principles results. We develop an efficient computational workflow and apply it to a diverse set of semiconductors, specifically AlN, CdS, GaN, MgO, and [Formula: see text]. We demonstrate under different physical scenarios how excitons may be screened by multiple polar optical or acoustic phonons, how their binding energies can exhibit strong temperature dependence, and the ultrafast timescales on which they dissociate into free electron-hole pairs.

Unraveling intrinsic mobility limits in two-dimensional (AlxGa1−x)2O3 alloys

β-(AlxGa1−x)2O3 presents a diverse material characterization exhibiting exceptional electrical and optical properties. Considering the miniaturization of gallium oxide devices, two-dimensional (AlxGa1−x)2O3 alloys, as a critical component in the formation of two-dimensional electron gases, demand an in-depth examination of their carrier transport properties. Herein, we investigate the temperature-dependent carrier mobility and scattering mechanisms of quasi-two-dimensional (2D) (AlxGa1−x)2O3 (x ≤ 5) by solving the Boltzmann transport equation from first-principles. Anisotropic electron mobility of 2D (AlxGa1−x)2O3 is limited to 30−80 cm2/Vs at room temperature, and it finds that the relatively large ion-clamped dielectric tensors (Δɛ) suggest a major scattering role for polar optical phonons. The mobility of 2D (AlxGa1−x)2 is less than that of bulk β-(AlxGa1−x)2O3 and shows no quantum effects attributed to the dangling bonds on the surface. We further demonstrate that the bandgap of 2D (AlxGa1−x)2O3 decreases with the number of layers, and the electron localization function also shows an anisotropy. This work comprehensively interprets the scattering mechanism and unintentional doping intrinsic electron mobility of (AlxGa1−x)2O3 alloys, providing physical elaboration and alternative horizons for experimental synthesis, crystallographic investigations, and power device fabrication of 2D (AlxGa1−x)2O3 atomically thin layered systems.

Low field mobility in bulk GaN and its ternary AlGaN/GaN compounds (quantum kinetic approach)

Analytical expressions for the low-field mobility of charge carrier gases with three-(3D), two-(2D) and one-(1D) dimensionalities are obtained. Multi-ion ionized impurities scattering, acoustic and polar optic phonons are considered as scattering mechanisms. The calculated values of mobility are compared to known experimental data for bulk (3D) n-and p-type wurtzite, n-type zinc-blende GaN crystals and low dimensional (2D and 1D) ternary GaAlN compounds. The resulting analytical expressions give the dependences of mobility on dimensionality of charge carrier gas, its density, effective mass, temperature and confining dimensions. A comparison of the experimental and calculated temperature dependences of the mobility in bulk GaN crystals (3D) and in AlGaN/GaN nanowires (1D) shows that the mobility at 100\\,{\ ext{K}}$?> T>100K is determined by the scattering of charge carriers by polar optical phonons with an energy of 91.2 meV. The temperature dependences of mobility in Al0.25Ga0.75N/GaN heterostructures (2D) at 100\\,{\ ext{K}}$?> T>100K are in consistent with experiment for electron scattering by polar optical phonons with a noticeably higher energy of 160 meV. We associate this fact with the heterointerface, which according to well-known theoretical studies can change both the strength of electron polar optical phonons scattering and the energy of the phonons.

Внезонное поглощение электромагнитного излучения электронами с оптическим фононным участием в сверхрешетках квантовых точек

Physics Institute of Azerbaijan National Academy of Sciences In this paper, we investigate the absorption of electromagnetic radiation by a free electron gas interacting with lattice vibrations in a quantum dot superlattice. It is assumed that the electron gas in the quantum dot superlattice is limited by the anisotropic parabolic potential. The absorption of light by free carriers with the participation of phonons is calculated in the second order of the perturbation theory. When calculating the absorption coefficient, the matrix elements of the electron-photon and electron-phonon interactions (with polar and nonpolar optical phonons) are used. We can expect three possible transitions in the absorption coefficient for electron-polar phonon scattering: (1) a transition due to the size subband levels for only the x direction, (2) a transition due to the size subband levels for only the y direction and (3) a transition due to the size subband levels for both the x direction and the y direction. For electron-nonpolar phonon scattering we can expect оnly one possible transitions in the, the absorption coefficient: a transition due to the size subband levels for both the x direction and the y direction.

Electron mobility of SnO2 from first principles

The transparent conducting oxide SnO2 is a wide bandgap semiconductor that is easily n-type doped and widely used in various electronic and optoelectronic applications. Experimental reports of the electron mobility of this material vary widely depending on the growth conditions and doping concentrations. In this work, we calculate the electron mobility of SnO2 from first principles to examine the temperature and doping concentration dependence and to elucidate the scattering mechanisms that limit transport. We include both electron–phonon scattering and electron-ionized impurity scattering to accurately model scattering in a doped semiconductor. We find a strongly anisotropic mobility that favors transport in the direction parallel to the c-axis. At room temperature and intrinsic carrier concentrations, the low-energy polar-optical phonon modes dominate scattering, while ionized-impurity scattering dominates above 1018 cm−3.

Tuning Spin-Polarized Lifetime at High Carrier Density through Deformation Potential in Dion-Jacobson-Phase Perovskites.

The control of spin relaxation mechanisms is of great importance for spintronics applications as well as for fundamental studies. Layered metal-halide perovskites represent an emerging class of semiconductors with rich optical spin physics, showing potential for spintronic applications. However, a major hurdle arises in layered metal-halide perovskites with strong spin-orbit coupling, where the spin lifetime becomes extremely short due to D'yakonov-Perel' scattering and Bir-Aronov-Pikus at high carrier density. Using the circularly polarized pump-probe transient reflection technique, we experimentally reveal the important scattering for spin relaxation beyond the electron-hole exchange strength in the Dion-Jacobson (DJ)-type 2D perovskites (3AMP)(MA)n-1PbnI3n+1 [3AMP = 3-(aminomethyl)piperidinium, n = 1-4]. Despite a more than 10-fold increase in carrier concentration, the spin lifetimes for n = 3 and 4 are effectively maintained. We reveal neutral impurity and polar optical phonon scatterings as significant contributors to the momentum relaxation rate. Furthermore, we show that more octahedral distortions induce a larger deformation potential which is reflected on the acoustic phonon properties. Coherent acoustic phonon analysis indicates that the polaronic effect is crucial in achieving control over the scattering mechanism and ensuring spin lifetime protection, highlighting the potential of DJ-phase perovskites for spintronic applications.

Exploring the impact of AlGaN barrier thickness and temperature on normally-on GaN HEMT performance

We study varying barrier thicknesses in GaN/AlGaN HEMTs as well as the effect of temperature fluctuation on device functionality theoretically. Structures A, B, C, D, and E are designed each with barrier thickness 16 nm, 19 nm, 22 nm, 25 nm, and 28 nm respectively. The impact of barrier thickness on the surface barrier height, strain relaxation and 2DEG concentration is explained including GaN HEMT’s drain and transfer properties. At elevated temperatures, the polar-optical phonon dispersion is the predominant process. Yet, at lower temperatures, the interface-roughness (IFR) and alloy disorder dispersion both satisfactorily account for the calculated mobilities.

Theoretical Studies of 2D Electron Gas Distributions and Scattering Characteristics in Double‐Channel n‐Al0.3Ga0.7N/GaN/i‐AlxGa1−xN/GaN High‐Electron‐Mobility Transistors

A detailed analysis of self‐consistent potentials, electric fields, electron distributions, and transport properties of dual‐channel (DC) n‐Al0.3Ga0.7N/GaN/i‐AlxGa1−xN/GaN high‐electron‐mobility transistors (HEMTs) is performed in this article. The 2D electron gas (2DEG) densities and mobility states limited by different scattering mechanisms in channel 1 and channel 2 are obtained, with varying values of doping concentrations, ambient temperatures, Al components, and thicknesses of the back barrier layer. The reduced and increased 2DEG densities are respectively observed in channel 1 and channel 2 with growing Al fractions and thicknesses of the AlxGa1−xN layer. Alloy disorder scattering exhibits a superior effect on carriers in channel 2 due to the lower barrier height and higher permeable electrons, which together with the interface roughness scattering severely depends on the thicknesses and Al fractions of the back barrier layer. Polar optical phonon scattering becomes important at higher temperatures. The trend of individual mobility in channel 1 is exactly opposite to that in channel 2. The parameter variation of the back barrier layer can effectively change the scattering characteristics of the main channel. Low‐temperature mobilities of n‐Al0.3Ga0.7N/GaN/i‐AlxGa1−xN/GaN HEMTs under varied doping concentrations are also obtained. Finally, the results are verified by comparison with the technology computer‐aided design simulations for DC HEMTs.