Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userEffective $n$-type Doping of Mg$_3$Sb$_2$ with Group-3 Elements
158
0
0.0
(
0
)
Ask ChatGPT about the research
No Arabic abstract
The recent discovery of high thermoelectric performance in Mg$_3$Sb$_2$ has been critically enabled by the success in $n$-type doping of this material, which is achieved under Mg-rich growth conditions, typically with chalcogens (Se, Te) as extrinsic dopants. Using first-principles defect calculations, we previously predicted that higher electron concentrations ($sim10^{20}$ cm$^{-3}$) can be achieved in Mg$_3$Sb$_2$ by doping with La instead of Se or Te. Subsequent experiments showed that free electron concentration in La-doped Mg$_3$Sb$_{2-x}$Bi$_x$ indeed exceeds those in the Te-doped material. Herein, we further investigate $n$-type doping of Mg$_3$Sb$_2$ and predict that, in addition to La, other group-3 elements (Sc, Y) are also effective as $n$-type dopants; Y is as good as La while Sc slightly less. Overall, we find that doping with any group-3 elements should lead to higher free electron concentrations than doping with chalcogens.
rate research
Read More
The recent discovery of n-type Mg$_3$Sb$_2$ thermoelectric has ignited intensive research activities on searching for potential n-type dopants for this material. Using first-principles defect calculations, here we conduct a systematic computational screening of potential efficient n-type lanthanide dopants for Mg$_3$Sb$_2$. In addition to La, Ce, Pr, and Tm, we find that high electron concentration ($geq$ 10$^{20}$ cm$^{-3}$ at the growth temperature of 900 K) can be achieved by doping on the Mg sites with Nd, Gd, Ho, and Lu, which are generally more efficient than other lanthanide dopants and the anion-site dopant Te. Experimentally, we confirm Nd and Tm as effective n-type dopants for Mg$_3$Sb$_2$ since doping with Nd and Tm shows superior thermoelectric figure of merit zT $geq$ 1.3 with higher electron concentration than doping with Te. Through codoping with Nd (Tm) and Te, simultaneous power factor improvement and thermal conductivity reduction are achieved. As a result, we obtain high zT values of about 1.65 and 1.75 at 775 K in n-type Mg$_{3.5}$Nd$_{0.04}$Sb$_{1.97}$Te$_{0.03}$ and Mg$_{3.5}$Tm$_{0.03}$Sb$_{1.97}$Te$_{0.03}$, respectively, which are among the highest values for n-type Mg$_3$Sb$_2$ without alloying with Mg$_3$Bi$_2$. This work sheds light on exploring promising n-type dopants for the design of Mg$_3$Sb$_2$ thermoelectrics.
The lattice thermal conductivity of the candidate thermoelectric material Mg$_3$Sb$_2$ is studied from first principles, with the inclusion of anharmonic, isotope, and boundary scattering processes, and via an accurate solution of the Boltzmann equation. We find that the anomalously low observed conductivity is due to grain-boundary scattering of phonons, whereas the purely anharmonic conductivity is an order of magnitude larger. Mass disorder due to alloying and off-stoichiometry is also found to contribute significantly to its decrease. Combining ab initio values vs sample size with measured grain-size distributions, we obtain an estimate of $kappa$ vs T in nano-polycrystalline material in good agreement with typical experiments, and compute the ZT figure of merit in the various cases.
Nodal-line semimetals (NLSs) represent a new type of topological semimetallic beyond Weyl and Dirac semimetals in the sense that they host closed loops or open curves of band degeneracies in the Brillouin zone. Parallel to the classification of type-I and type-II Weyl semimetals, there are two types of NLSs. The conventional NLS phase, in which the two bands forming the nodal line have opposite signs for their slopes along any direction perpendicular to the nodal line, has been proposed and realized in many compounds, whereas the exotic type-II NLS is very rare. Our first-principles calculations show that Mg$_3$Bi$_2$ is a material candidate that hosts a single type-II nodal loop around $Gamma$. The band crossing is close to the Fermi level and the two crossing bands have the same sign in their slopes along the radial direction of the loop, indicating the type-II nature of the nodal line. Spin-orbit coupling generates only a small energy gap ($sim$35 meV) at the nodal points and does not negate the band dispersion of Mg$_3$Bi$_2$ that yields the type-II nodal line. Based on this prediction we have synthesized Mg$_3$Bi$_2$ single crystals and confirmed the presence of the type-II nodal lines in the material. Our angle-resolved photoemission spectroscopy (ARPES) measurements agree well with our first-principles results and thus establish Mg$_3$Bi$_2$ as an ideal materials platform for studying the exotic properties of type-II nodal line semimetals.
Bi2Te3-xSex family has been the n-type start-of-the-art thermoelectric materials near room temperatures (RT) for more than half-century, which dominates the active cooling and novel waves harvesting application near RT. However, the drawbacks of brittle nature and Te-containing restrict the further applications exploring. Here, we show that a Mg3+{delta}SbxBi2-x family ((ZT)avg =1.05) could be a promising substitute for the Bi2Te3-xSex family ((ZT)avg =0.9-1.0) in the temperature range of 50-250 {deg}C based on the comparable thermoelectric performance through a synergistic effect from the tunable band gap using the alloy effect and the suppressible Mg-vacancy formation using interstitial Mn dopant. The former is to shift the optimal thermoelectric performance to near RT, and latter is helpful to partially decouple the electrical transport and thermal transport in order to get an optimal RT power factor. A positive temperature-dependence of band gap suggested this family is also a superior medium-temperature thermoelectric material for the significantly suppressed bipolar effect. Furthermore, a two times higher mechanical toughness, compared with Bi2Te3-xSex family, consolidates the promising substitute for the start-of-art n-type thermoelectric materials near RT.
Nitrides feature many interesting properties, such as a wide range of bandgaps suitable for optoelectronic devices including light-emitting diodes (LEDs), and piezoelectric response used in microelectromechanical systems (MEMS). Nitrides are also significantly underexplored compared to oxides and other chemistries, with many being thermochemically metastable, sparking interest from a basic science point of view. This paper reports on experimental and computational exploration of the Mg-Sb-N material system, featuring both metastable materials and interesting semiconducting properties. Using sputter deposition, we discovered a new Mg2SbN3 nitride with a wurtzite-derived crystal structure and synthesized the antimonide-nitride Mg3SbN with an antiperovskite crystal structure for the first time in thin film form. Theoretical calculations indicate that Mg2SbN3 is metastable and has properties relevant to LEDs and MEMS, whereas Mg3SbN has a large dielectric constant (28epsilon_0) and low hole effective masses (0.9m_0), of interest for photovoltaic solar cell absorbers. The experimental solar-matched 1.3 eV optical absorption onset of the Mg3SbN antiperovskite agrees with the theoretical prediction (1.3 eV direct, 1.1 eV indirect), and with the measurements of room-temperature near-bandgap photoluminescence. These results make an important contribution towards understanding semiconductor properties and chemical trends in the Mg-Sb-N materials system, paving the way to future practical applications of these novel materials.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
