Room Temperature Electron Mobility Research Articles

Intrinsic electron transport in monolayer MoSi2N4 and WSi2N4

We systematically studied the intrinsic electron transport of the recently fabricated two-dimensional (2D) monolayer MoSi2N4 and WSi2N4 (belong to the MA2Z4 family, where M is a transition metal; A is Si or Ge; and Z is N, P, or As) by using the Boltzmann transport theory with the scattering rates calculated from first-principles calculations. It is found that both materials have moderate room temperature electron mobility of 87 cm2/V s for MoSi2N4 and 119 cm2/V s for WSi2N4. Our detailed analysis shows that their electron mobility difference is attributed to the different average effective mass. Moreover, by comparing studies with monolayer MoS2 and WS2, we reveal that the polar optical phonon pattern of MoSi2N4 and WSi2N4 is governed by the antiparallel silicon–nitrogen bond oscillation, different from MoS2 and WS2, in which is governed by the antiparallel transition metal–sulfur bond oscillation. This feature is arising from the large electronegativity difference between N and Si. Nitrogen has the fourth largest electronegativity, so it always tends to attract plenty of electrons from Si and thus Si has a large Born effective charge, thereby resulting in strong Fröhlich interaction. We further found that all the 2D semiconducting MA2Z4 have large Born effective charges, thereby indicating a generally strong electron–phonon coupling strength.

Steady-state and transient electronic transport properties of β-(Al x Ga1–x )2O3/Ga2O3 heterostructures: An ensemble Monte Carlo simulation

The steady-state and transient electron transport properties of β-(Al x Ga1−x )2O3/Ga2O3 heterostructures were investigated by Monte Carlo simulation with the classic three-valley model. In particular, the electronic band structures were acquired by first-principles calculations, which could provide precise parameters for calculating the transport properties of the two-dimensional electron gas (2DEG), and the quantization effect was considered in the Γ valley with the five lowest subbands. Wave functions and energy eigenvalues were obtained by iteration of the Schrödinger–Poisson equations to calculate the 2DEG scattering rates with five main scattering mechanisms considered. The simulated low-field electron mobilities agree well with the experimental results, thus confirming the effectiveness of our models. The results show that the room temperature electron mobility of the β-(Al0.188Ga0.812)2O3/Ga2O3 heterostructure at 10 kV⋅cm−1 is approximately 153.669 cm2⋅V−1⋅s−1, and polar optical phonon scattering would have a significant impact on the mobility properties at this time. The region of negative differential mobility, overshoot of the transient electron velocity and negative diffusion coefficients are also observed when the electric field increases to the corresponding threshold value or even exceeds it. This work offers significant parameters for the β-(Al x Ga1−x )2O3/Ga2O3 heterostructure that may benefit the design of high-performance β-(Al x Ga1−x )2O3/Ga2O3 heterostructure-based devices.

Valence Disproportionation of GeS in the PbS Matrix Forms Pb5Ge5S12 Inclusions with Conduction Band Alignment Leading to High n-Type Thermoelectric Performance.

Converting waste heat into useful electricity using solid-state thermoelectrics has a potential for enormous global energy savings. Lead chalcogenides are among the most prominent thermoelectric materials, whose performance decreases with an increase in chalcogen amounts (e.g., PbTe > PbSe > PbS). Herein, we demonstrate the simultaneous optimization of the electrical and thermal transport properties of PbS-based compounds by alloying with GeS. The addition of GeS triggers a complex cascade of beneficial events as follows: Ge2+ substitution in Pb2+ and discordant off-center behavior; formation of Pb5Ge5S12 as stable second-phase inclusions through valence disproportionation of Ge2+ to Ge0 and Ge4+. PbS and Pb5Ge5S12 exhibit good conduction band energy alignment that preserves the high electron mobility; the formation of Pb5Ge5S12 increases the electron carrier concentration by introducing S vacancies. Sb doping as the electron donor produces a large power factor and low lattice thermal conductivity (κlat) of ∼0.61 W m-1 K-1. The highest performance was obtained for the 14% GeS-alloyed samples, which exhibited an increased room-temperature electron mobility of ∼121 cm2 V-1 s-1 for 3 × 1019 cm-3 carrier density and a ZT of 1.32 at 923 K. This is ∼55% greater than the corresponding Sb-doped PbS sample and is one of the highest reported for the n-type PbS system. Moreover, the average ZT (ZTavg) of ∼0.76 from 400 to 923 K is the highest for PbS-based systems.

Revealing the Defect-Dominated Electron Scattering in Mg3Sb2-Based Thermoelectric Materials.

The thermoelectric parameters are essentially governed by electron and phonon transport. Since the carrier scattering mechanism plays a decisive role in electron transport, it is of great significance for the electrical properties of thermoelectric materials. As a typical example, the defect-dominated carrier scattering mechanism can significantly impact the room-temperature electron mobility of n-type Mg3Sb2-based materials. However, the origin of such a defect scattering mechanism is still controversial. Herein, the existence of the Mg vacancies and Mg interstitials has been identified by synchrotron powder X-ray diffraction. The relationship among the point defects, chemical compositions, and synthesis conditions in Mg3Sb2-based materials has been revealed. By further introducing the point defects without affecting the grain size via neutron irradiation, the thermally activated electrical conductivity can be reproduced. Our results demonstrate that the point defects scattering of electrons is important in the n-type Mg3Sb2-based materials.

Precise composition control and cation nonstoichiometry in La-doped BaSnO3 thin films grown by MOCVD

La:BaSnO3 has recently emerged as an outstanding perovskite oxide material due to its high electron mobility. To-date, lower electron mobility in thin films compared to the single-crystal are discussed in terms of the presence of dislocations, nearly neglecting the role of cation nonstoichiometry. However, by controlling Sn/Ba compositional ratio, we demonstrate the significance of stoichiometry and resulting point defects on microstructure, morphology, electrical properties, and Raman defect modes in epitaxial La:BaSnO3 films. A narrow compositional window is demonstrated to yield high mobility and smooth morphology in La:BaSnO3 thin films using the metalorganic chemical vapor deposition. The room temperature electron mobility of 121 cm2V−1s−1 and 85 cm2V−1s−1 was achieved on SrTiO3 and MgO substrates, respectively. Correlation between the lowering of the A1 g soft mode near 140 cm−1 frequency and increase in the carrier mobility is demonstrated by Raman spectroscopy analysis. It was suggested that the position of this soft mode might be employed as a marker band for probing the electrical properties of La-doped BaSnO3 perovskites.

First-principles study of electron transport in ScN

We investigate the conduction-band structure and electron mobility in rocksalt ScN based on density functional theory. The first-principles band structure allows us to obtain band velocities and effective masses as a function of energy. Electron-phonon scattering is assessed by explicitly computing the $q$-dependent electron-phonon matrix elements, with the inclusion of the long-range electrostatic interaction. The influence of free-carrier screening on the electron transport is assessed using the random-phase approximation. We find a notable enhancement of electron mobility when the carrier concentration exceeds ${10}^{20}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$. We calculate the room-temperature electron mobility in ScN to be 587 ${\mathrm{cm}}^{2}/\mathrm{Vs}$ at low carrier concentrations. When the carrier concentration is increased, the electron mobility starts to decrease significantly around $n={10}^{19}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$ and drops to 240 ${\mathrm{cm}}^{2}/\mathrm{Vs}$ at $n={10}^{21}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$. We also explore the influence of strain in (111)- and (100)-oriented ScN films. For (111) films, we find that a 1.0% compressive epitaxial strain increases the in-plane mobility by 72 ${\mathrm{cm}}^{2}/\mathrm{Vs}$ and the out-of-plane mobility by 50 ${\mathrm{cm}}^{2}/\mathrm{Vs}$. For (100) films, a 1.0% compressive epitaxial strain increases the out-of-plane mobility by as much as 172 ${\mathrm{cm}}^{2}/\mathrm{Vs}$, but has a weak impact on the in-plane mobility. Our study sheds light on electron transport in ScN at different electron concentrations and shows how strain engineering could increase the electron mobility.

One-step epitaxy of high-mobility La-doped BaSnO3 films by high-pressure magnetron sputtering

As unique perovskite transparent oxide semiconductors, high-mobility La-doped BaSnO3 films have been successfully synthesized by molecular beam epitaxy and pulsed laser deposition. However, it remains a big challenge for magnetron sputtering, a widely applied technique suitable for large-scale fabrication, to grow high-mobility La-doped BaSnO3 films. In this work, we developed a method to synthesize high-mobility epitaxial La-doped BaSnO3 films (with mobility up to 121 cm2 V−1 s−1 at the carrier density of ∼4.0 × 1020 cm−3 at room temperature) directly on SrTiO3 single crystal substrates using high-pressure magnetron sputtering. The structural and electrical properties of La-doped BaSnO3 films were characterized by combined high-resolution x-ray diffraction, x-ray photoemission spectroscopy, and temperature-dependent electrical transport measurements. The room-temperature electron mobility of La-doped BaSnO3 films achieved in this work is two to four times higher than the reported values of the films grown by magnetron sputtering. Moreover, in the high carrier density range (n > 3 × 1020 cm−3), the electron mobility value of 121 cm2 V−1 s−1 achieved in our work is among the highest values for all reported doped BaSnO3 films. It is revealed that high argon pressure during sputtering plays a vital role in stabilizing the fully relaxed films and inducing oxygen vacancies, which facilitates high mobility at room temperature. Our work provides an easy and economical way to massively synthesize high-mobility transparent conducting films for transparent electronics.

High-mobility n−-GaN drift layer grown on Si substrates

We have investigated the interaction between carbon impurities and threading dislocations and their impact on the transport properties of GaN grown on Si substrates. The incorporation of carbon impurity was found to be associated with dislocation density, with a linear dependence. It indicates that the carbon may accumulate around the dislocations. The temperature-dependent Hall-effect measurement further confirmed that those carbon-decorated dislocations can act as acceptor-like traps, existing at every c-lattice spacing along a threading dislocation. The acceptor-like traps are important scattering centers and, thus, cannot be neglected. By reducing the density of the carbon-decorated dislocation via introducing a thick dislocation filtering layer to reduce the dislocation-related acceptor-like trap scattering, a record room-temperature electron mobility of 1090 cm2/V s with a carrier concentration of ∼2 × 1016 cm−3 for n--GaN on Si was achieved. Our results provide an effective approach to obtain high-quality n−-GaN on Si for vertical GaN based devices.

Why Two-Dimensional Semiconductors Generally Have Low Electron Mobility

Atomically thin (two-dimensional, 2D) semiconductors have shown great potential as the fundamental building blocks for next-generation electronics. However, all the 2D semiconductors that have been experimentally made so far have room-temperature electron mobility lower than that of bulk silicon, which is not understood. Here, by using first-principles calculations and reformulating the transport equations to isolate and quantify contributions of different mobility-determining factors, we show that the universally low mobility of 2D semiconductors originates from the high “density of scatterings,” which is intrinsic to the 2D material with a parabolic electron band. The density of scatterings characterizes the density of phonons that can interact with the electrons and can be fully determined from the electron and phonon band structures without knowledge of electron-phonon coupling strength. Our work reveals the underlying physics limiting the electron mobility of 2D semiconductors and offers a descriptor to quickly assess the mobility [1,2,3].[1] L. Cheng, C. Zhang, Y. Liu, Phys. Rev. Lett., 2020, DOI: 10.1103/PhysRevLett.125.177701[2] L. Cheng, C. Zhang, Y. Liu, J. Am. Chem. Soc., 2019, DOI: 10.1021/jacs.9b05923[3] L. Cheng, Y. Liu, J. Am. Chem. Soc., 2018, 140, 17895-17900

Phonon-Limited Mobility and Electron-Phonon Coupling in Lead-Free Halide Double Perovskites.

Lead-free halide double perovskites have attracted considerable attention as complements to lead-based halide perovskites in a range of optoelectronic applications. Experiments on Cs2AgBiBr6 indicate carrier mobilities in the range of 0.3-11 cm2/(V s) at room temperature, considerably lower than in lead-based perovskites. The origin of low mobilities is currently unclear, calling for an atomic-scale investigation. We report state-of-the-art ab initio calculations of the phonon-limited mobility of charge carriers in lead-free halide double perovskites Cs2AgBiX6 (X = Br, Cl). For Cs2AgBiBr6, we obtain room-temperature electron and hole mobilities of 17 and 14 cm2/(V s), respectively, in line with experiments. We demonstrate that the cause for the lower mobility of this compound, compared to CH3NH3PbI3, resides in the heavier carrier effective masses. A mode-resolved analysis of scattering rates reveals the predominance of Fröhlich electron-phonon scattering, similar to lead-based perovskites. Our results indicate that, to increase the mobility of lead-free perovskites, it is necessary to reduce the effective masses, for example by cation engineering.

MOCVD growth of high purity Ga2O3 epitaxial films using trimethylgallium precursor

We report on the growth of β-Ga2O3 thin films using trimethylgallium (TMGa) as a source for gallium and pure O2 for oxidation. The growth rate of the films was found to linearly increase with the increase in the molar flow rate of TMGa and reach as high as ∼6 μm/h at a flow rate of 580 μmol/min. High purity, lightly Si-doped homoepitaxial β-Ga2O3 films with a good surface morphology, a record low temperature electron mobility exceeding 23 000 cm2/V s at 32 K, and an acceptor concentration of 2 × 1013 cm−3 were realized, showing an excellent purity film. Films with room temperature (RT) electron mobilities ranging from 71 cm2/V s to 138 cm2/V s with the corresponding free carrier densities between ∼1.1 × 1019 cm−3 and ∼1.5 × 1016 were demonstrated. For layers with the doping concentration in the range of high-1017 and low-1018 cm−3, the RT electron mobility values were consistently more than 100 cm2/V s, suggesting that TMGa is suitable to grow channel layers for lateral devices, such as field effect transistors. The results demonstrate excellent purity of the films produced and confirm the suitability of the TMGa precursor for the growth of device quality β-Ga2O3 films at a fast growth rate, meeting the demands for commercializing Ga2O3-based high voltage power devices by metalorganic chemical vapor deposition.

Plasma-assisted molecular beam epitaxy of SnO(001) films: Metastability, hole transport properties, Seebeck coefficient, and effective hole mass

Transparent conducting or semiconducting oxides are important materials for (transparent) optoelectronics and power electronics applications. While most of these oxides can be doped n-type only with room-temperature electron mobilities on the order of 100cm^2/Vs p-type oxides are needed for the realization of pn-junction devices but typically suffer from exessively low (<<1cm^2/Vs) hole mobilities. Tin monoxide (SnO) is one of the few p-type oxides with a higher hole mobility, lacking a well-established understanding of its hole transport properties. Moreover, growth of SnO is complicated by its metastability with respect to SnO2 and Sn, requiring epitaxy for the realization of single crystalline material typically required for high-end applications. Here, we give a comprehensive account on the epitaxial growth of SnO, its (meta)stability, and its thermoelectric transport properties in the context of the present literature. Textured and single-crystalline, unintentionally-doped p-type SnO(001) films are grown by plasma-assisted molecular beam epitaxy. The metastability of this semiconducting oxide is addressed theoretically through an equilibrium phase diagram. Experimentally, the related SnO growth window is rapidly determined by an in-situ growth kinetics study as function of Sn-to-O-plasma flux ratio and growth temperature. The presence of secondary Sn and SnOx (1 < x <= 2) phases is comprehensively studied by different methods, indicating the presence of Sn3O4 or Sn as major secondary phases, as well as a fully oxidized SnO2 film surface. The hole transport properties, Seebeck coefficient, and density-of-states effective mass are determined and critically discussed in the context of the present literature on SnO, considering its anisotropic hole-effective mass.

High thermoelectric figure of merit in monolayer Tl2O from first principles

The thermoelectric properties of monolayer Tl2O are studied using first-principles calculations with all involved electrical and thermal transport properties calculated in the parameter-free frameworks. It is found that monolayer Tl2O possesses remarkably high thermoelectric figure of merit, zT, due to its ultralow lattice thermal conductivity and fairly good power factor. The room temperature zT can be as high as 1.4 and 1.2 for n- and p-type systems, respectively, whereas the maximum zT values can reach up to 5.3 and 4.2 as the temperature increases to 800 K. In addition, it is clarified that the mobilities of monolayer Tl2O are orders of magnitude smaller than previous estimation from simplified semiempirical models. The room temperature electron and hole mobilities are only about 56 and 11cm2V−1s−1, respectively, due to the heavy effective mass along with strong polar optical phonons coupling scattering. Nonetheless, the intrinsically ultrahigh zT from entire first-principles calculations stimulate that the further experimental verification and exploration for practical application are worthwhile.

Optical and electronic properties in amorphous BaSnO3 thin films

Wide-bandgap perovskite stannates are of interest for the emergent all-oxide transparent electronic devices due to their unparalleled room temperature electron mobility. Considering the advantage of amorphous material in integrating with non-semiconductor platforms, we herein reported the optical and electronic properties in the prototypical stannate, amorphous barium stannate (BaSnO3) thin films, which were deposited at room temperature and annealed at various temperatures. Despite remaining amorphous status, with increasing the annealing temperature, the defect level within amorphous BaSnO3 thin films could be suppressed. Accordingly, the optical band gap, the leakage current, and the breakdown electric field could be improved from 2.81 eV, 3.94 × 10−6 A cm−2 at 400 kV/cm, 1.43 MV/cm for the as-prepared BaSnO3 thin films to 2.90 eV, 6.17 × 10−8 A cm−2 at 400 kV/cm, 1.93 MV/cm for the 400 °C-annealed BaSnO3 thin films.

Why Two-Dimensional Semiconductors Generally Have Low Electron Mobility.

Atomically thin (two-dimensional, 2D) semiconductors have shown great potential as the fundamental building blocks for next-generation electronics. However, all the 2D semiconductors that have been experimentally made so far have room-temperature electron mobility lower than that of bulk silicon, which is not understood. Here, by using first-principles calculations and reformulating the transport equations to isolate and quantify contributions of different mobility-determining factors, we show that the universally low mobility of 2D semiconductors originates from the high "density of scatterings," which is intrinsic to the 2D material with a parabolic electron band. The density of scatterings characterizes the density of phonons that can interact with the electrons and can be fully determined from the electron and phonon band structures without knowledge of electron-phonon coupling strength. Our work reveals the underlying physics limiting the electron mobility of 2D semiconductors and offers a descriptor to quickly assess the mobility.

Manoeuvring Morphological, Optical and Electrical Properties of CVD-Grown Ba-Doped SnO2 Nanostructures via Mn Co-Doping

Barium and manganese (Ba and Mn) co-doped nanostructures of tin oxide (SnO2) are synthesized in situ using a thermal chemical vapour deposition method. The structural property correlation is established using X-ray diffraction, field emission scanning electron microscopy, high-resolution transmission electron microscopy, ultraviolet–visible light (UV–Vis), X-ray photoelectron spectroscopy and Hall measurements. The role of substrate type (n-type silicon and quartz) and catalyst layer thickness is also studied for detailed examination of the correlation with SnO2 properties at nanoscale. In this study, the significant role of Mn as co-dopant in Ba-doped SnO2 one-dimensional and two-dimensional nanostructures (nanowires and nanoflakes) is studied. Optical and room-temperature (RT) electrical measurements confirm the band gap tailoring from 3.2 eV to 3.6 eV relating to the Ba increase with Mn as co-dopant. Subsequently, the RT electron mobility changes from 46 cm2 s−1 V−1 to 88 cm2 s−1 V−1 as SnO2 changes from Ba-doped to Ba/Mn co-doped. The effective role of the co-dopant in band gap tailoring and the effects on morphology, optical and electrical properties are studied for SnO2 nanostructures. This study helps to gain a better understanding of the dopant population and the electrical and optical properties for transparent conducting oxides (TCOs), sensors, photocatalysis, solar cell materials and other applications.

Ledge-directed epitaxy of continuously self-aligned single-crystalline nanoribbons of transition metal dichalcogenides.

Two-dimensional transition metal dichalcogenide nanoribbons are touted as the future extreme device downscaling for advanced logic and memory devices but remain a formidable synthetic challenge. Here, we demonstrate a ledge-directed epitaxy (LDE) of dense arrays of continuous, self-aligned, monolayer and single-crystalline MoS2 nanoribbons on β-gallium (III) oxide (β-Ga2O3) (100) substrates. LDE MoS2 nanoribbons have spatial uniformity over a long range and transport characteristics on par with those seen in exfoliated benchmarks. Prototype MoS2-nanoribbon-based field-effect transistors exhibit high on/off ratios of 108 and an averaged room temperature electron mobility of 65 cm2 V-1 s-1. The MoS2 nanoribbons can be readily transferred to arbitrary substrates while the underlying β-Ga2O3 can be reused after mechanical exfoliation. We further demonstrate LDE as a versatile epitaxy platform for the growth of p-type WSe2 nanoribbons and lateral heterostructures made of p-WSe2 and n-MoS2 nanoribbons for futuristic electronics applications.

Efficient light harvesting using simple porphyrin-oxide perovskite system

Here, we report the systematic studies on photoanodes of phase pure polycrystalline microrods of Barium Stannate (BaSnO3) microrods for application in porphyrin dye-sensitized solar cell (DSSC). We were able to establish the effect of vacuum annealing on BaSnO3 thin films on its electrical, optical and adsorption properties using XPS, UV–Vis, photoluminescence and adsorption isotherm studies. Increase in oxygen vacancy with annealing is found to increase the room temperature (RT) electron mobility from 49.1 to 82.4 cm2/V sec whereas macroporous nature of samples were found suitable for faster dye adsorption (~ 30 min). Post TiCl4 treatment studies, the maximum efficiency (η) of 4.7% is achieved in BSO films with current density Jsc ~ value as 10.4 mA/cm2; whereas DSSC fabricated using annealed BSO films gave maximum efficiency of 6.1% with Jsc value as 12.2 mA/cm2, during which the value of FF increased from 73.4 to 81%. The IPCE and proposed electron transfer mechanism suggested the potential application of macroporous BSO with unconventional dyes such as metallised-porphyrin. Our results strengthen the idea of using phase-pure, visible transparent porous BSO nanostructures with induced oxygen vacancies due to annealing process post-synthesis which eventually increased DSSC performance from by 84%.

Electron mobility modulation in graphene oxide by controlling carbon melt lifetime

The lack of bandgap is a fundamental issue in graphene devices, which can be solved by fabricating reduced graphene oxide (rGO). However, its device integration is impeded by the elevated reduction temperature (>2000 K) requirements. Recently, we demonstrated a new approach for laser writing heavily-reduced GO by employing the nonequilibrium approach of nanosecond laser annealing (Gupta and Narayan, 2019) [1]. Here, we report on the electron mobility modulation in the liquid phase grown graphene oxide. The process involves melting and subsequent quenching of molten carbon, which triggers the first-order phase transformation of amorphous carbon (a-C) into rGO. Laser annealing at energy density above the 0.3 J/cm2 melting threshold results in liquid-phase rGO growth on Si/SiO2. The rGO films exhibit 26 cm2/V-s room-temperature electron mobility and −4.7 × 1021/cc charge carrier concentration on annealing near melt threshold. The heavily-reduced GO films are formed on -O- creeping in the loosely-packed low undercooled carbon melt during ultrafast quenching. We establish that -O- injection is an implicit function of melt lifetime, and a rise in melt lifetime triggers GO film regrowth with increased mobility >210 cm2/V-s and 2.2 × 1019/cc carrier concentration on annealing at 0.6 J/cm2. Laser annealing resolves the fundamental issues of impurities and topological defects in rGO fabrication by equilibrium-based methods, facilitating increased electron mobility in laser patterned graphene-based materials.

Prospects for high carrier mobility in the cubic germanates

High-mobility wide-band-gap oxides are essential materials for device applications in high-frequency and power electronics. We use first-principles calculations to evaluate the potential of two cubic perovskite germanates, SrGeO3 and BaGeO3, for these applications. We find their effective masses to be small, both for electrons and holes. The prospect of p-type conductivity renders the germanates attractive for complementary metal-oxide-semiconductor technology. We calculate the electron drift mobility in SrGeO3 to lie between 400 and 500 cm2V−1s−1 for a range of accessible carrier concentrations; this mobility is as much as 50% larger than in BaSnO3, which has the highest room-temperature electron mobility among perovskite oxides. Our results suggest that the germanates hold promise for high-mobility electronic applications.