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Register a new userMg$_{3+delta}$Sb$_x$Bi$_{2-x}$ family: A promising substitute for the start-of-art n-type thermoelectric materials near room temperature
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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.
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A topological p-n junction (TPNJ) is an important concept to control spin and charge transport on a surface of three dimensional topological insulators (3D-TIs). Here we report successful fabrication of such TPNJ on a surface of 3D-TI Bi$_{2-x}$Sb$_x$Te$_{3-y}$Se$_y$ thin films and experimental observation of the electrical transport. By tuning the chemical potential of n-type topological Dirac surface of BSTS on its top half by employing tetrafluoro-7,7,8,8-tetracyanoquinodimethane as an organic acceptor molecule, a half surface can be converted to p-type with leaving the other half side as the opposite n-type, and consequently TPNJ can be created. By sweeping the back-gate voltage in the field effect transistor structure, the TPNJ was controlled both on the bottom and the top surfaces. A dramatic change in electrical transport observed at the TPNJ on 3D-TI thin films promises novel spin and charge transport of 3D-TIs for future spintronics.
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.
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.
Magnetism breaks the time reversal symmetry expected to open a Dirac gap in 3D topological insulators that consequently leads to quantum anomalous Hall effect. The most common approach of inducing ferromagnetic state is by doping magnetic 3$d$ elements into bulk of 3D topological insulators. In Cr$_{0.15}$(Bi$_{0.1}$Sb$_{0.9}$)$_{1.85}$Te$_3$, the material where the quantum anomalous Hall effect was initially discovered at temperatures much lower than the ferromagnetic transition, $T_C$, the scanning tunneling microscopy studies have reported a large Dirac gap $sim20-100$ meV. The discrepancy between the low temperature of quantum anomalous Hall effect ($ll T_C$) and large spectroscopic Dirac gaps ($gg T_C$) found in magnetic topological insulators remains puzzling. Here, we used angle-resolved photoemission spectroscopy to study the surface electronic structure of pristine and potassium doped surface of Cr$_{0.15}$(Bi$_{0.1}$Sb$_{0.9}$)$_{1.85}$Te$_3$. Upon potassium deposition, the $p$-type surface state of pristine sample was turned into an $n$-type, allowing spectroscopic observation of Dirac point. We find a gapless surface state, with no evidence of a large Dirac gap reported in tunneling studies.
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.
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