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A twisted grain boundary is introduced in the tellurium crystal to effectively block phonon propagation while maintaining high electron mobility for superior thermoelectric properties.

Atomic layer deposition (ALD) of Sb

Tin selenide (SnSe) is considered a robust candidate for thermoelectric applications due to its very high thermoelectric figure of merit, ZT, with values of 2.6 in p-type and 2.8 in n-type single crystals. Sn has been replaced with various lower group dopants to achieve successful p-type doping in SnSe with high ZT values. A known, facile, and powerful alternative way to introduce a hole carrier is to use a natural single Sn vacancy, VSn. Through transport and scanning tunneling microscopy studies, we discovered that VSn are dominant in high-quality (slow cooling rate) SnSe single crystals, while multiple vacancies, Vmulti, are dominant in low-quality (high cooling rate) single crystals. Surprisingly, both VSn and Vmulti help to increase the power factors of SnSe, whereas samples with dominant VSn have superior thermoelectric properties in SnSe single crystals. Additionally, the observation that Vmulti are good p-type sources observed in relatively low-quality single crystals is useful in thermoelectric applications because polycrystalline SnSe can be used due to its mechanical strength; this substance is usually fabricated at very high cooling speeds.

Tin selenide (SnSe) has attracted much attention due to its record ZT value in both pristine and doped crystals. This issue has renewed interest in the single-crystal form of tin-based chalcogenide compounds which possess the same layered structure as SnSe such as tin sulfide (SnS). Due to their natural abundances and low toxicities, SnSe and SnS can be alloyed at reduced the processing cost while maintaining the favorable electrical properties of SnSe. In this research, using the temperature gradient method, we successfully fabricated single crystals of SnS1-xSex with 0 ≤ x ≤ 1. High-quality crystals were obtained, and the electrical properties of those crystals were investigated. The results showed that the p-type crystals have layered structures with lattice constants changing gradually according to Vegard’s law. The value of the band gap monotonically decreased with increasing Se amount (x). The substitution of Se into S sites results in not only a large increase in the electrical conductivity but also a decrease in the Seebeck coefficient; i.e., the electrical conductivity at room temperature increased from 5 × 10–4 (x = 0) to 5.24 S⋅cm−1 (x = 0.8). The Seebeck coefficient decreased from 1069 in SnS to 525 μVK−1 in SnS0.2Se0.8 and to 481 μVK−1 in SnSe at room temperature. This work provides positive information for the growth of large-size SnS–SnSe single crystals.

In this work, pure, large Br-doped SnSe2 single crystals were successfully synthesized using the temperature gradient technique. Br acts as a donor, resulting in electron concentrations up to ∼6.83...

We report on the growth, thermoelectric, magnetic properties, and re-entrant spin-glass state in MnP-type orthorhombic FeAs thin film, grown on LaAlO3 (100) substrate by using a molecular beam epitaxy. The film is polycrystalline with a grain size about 200 nm. Electrical resistivity as a function of temperature revealed a metallic behavior. A sign change of Seebeck coefficient was observed at 370 K, due to the contribution of multiple bands to charge transport. We found a re-entrant spin-glass state in the film, attributed to strain in the sample. As a result, a very sharp spin-glass magnetic transition at 50 K was observed in the temperature dependence of Seebeck coefficient, electrical resistivity, and magnetization curves. The bifurcation point between zero field cooled and field cooled magnetization occurred at 350 K. A ferromagnetic-type behavior was observed over a temperature range from 10 to 300 K, confirming the re-entrant spin-glass state. Where the determined magnetization and coercive field are small, around 7 emu cm−3 and 300 Oe at 10 K, respectively. Our work provided a study on thermoelectric and magnetic properties of re-entrant spin-glass FeAs in thin film form

Author(s): Pham, AT; Vu, TH; Cheng, C; Trinh, TL; Lee, JE; Ryu, H; Hwang, C; Mo, SK; Kim, J; Zhao, LD; Duong, AT; Cho, S | Abstract: High-quality SnSe2 single crystals were successfully synthesized using a temperature gradient method. N-type characteristics and strong anisotropic transport properties of SnSe2 single crystals were exhibited between the ab plane and the c-axis. At 673 K, the power factor (PF) value along the ab plane is 3.43 μW cm-1 K-2, while it is 0.92 μW cm-1 K-2 along the c-axis. The ratio between thermal conductivities along the ab plane (κab) and c-axis (κc) is on the order of 7.6 at 300 K, while this value is about 5.6 at 673 K. The thermoelectric figure of merit (ZT) in the c-axis (0.15) is higher than that (0.1) along the ab plane, according to the ultralow out-of-plane thermal conductivity. The electronic band structure results, which were examined by angle-resolved photoemission spectroscopy (ARPES) predicted the potential of improving the thermoelectric performance of SnSe2 single crystals by electron doping.

The evolution of the optical phonons in layered semiconductor alloys SnSe1-xSx is studied as a function of the composition by using polarized Raman spectroscopy with six different excitation wavelengths (784.8, 632.8, 532, 514.5, 488, and 441.6 nm). The polarization dependences of the phonon modes are compared with transmission electron diffraction measurements to determine the crystallographic orientation of the samples. Some of the Raman modes show significant variation in their polarization behavior depending on the excitation wavelengths. It is established that the maximum intensity direction of the Ag2 mode of SnSe1-xSx (0, X

We investigated the spectral-dependent dielectric function and temperature-dependent bandgap energy of layered chalcogenide FeIn2Se4 crystals. The critical-point energy and Lorentzian broadening were analyzed by fitting second-derivative spectra using the standard critical point model. The temperature effect of the bandgap energy was analyzed based on an analytical model considering both thermal lattice expansion and electron–phonon interactions. We also extensively analyzed the temperature dependence of absorption tails and identified their possible origins. The dielectric functions and absorption coefficient in the photon-energy range of 0.75–4.75 eV were obtained. The results also showed that optical phonon modes associated with the electron–phonon interactions could be closely related to the average phonon energy.

Stroboscopic visualization of nuclear or electron dynamics in atoms, molecules or solids requires ultrafast pump and probe pulses and a close to perfect synchronization between the two. We have developed a 3 MeV ultrafast electron diffraction (UED) probe technology that nominally reduces the electron bunch duration and the arrival time jitter to the subfemtosecond level. This simple configuration uses a radiofrequency photogun and a 90° achromatic bend and is designed to provide effectively jitter-free conditions. Terahertz streaking measurements reveal an electron bunch duration of 25 fs, even for a charge as high as 0.6 pC, and an arrival time jitter of 7.8 fs, the latter limited by only the measurement accuracy. From pump–probe measurements of photoexcited bismuth films, the instrument response function was determined to be 31 fs. This pioneering jitter-free technique paves the way towards UED of attosecond phenomena in atomic, molecular and solid-state dynamics. An ultrafast electron diffraction facility with an overall temporal resolution of 31 fs root mean square is developed. Even for a charge as high as 0.6 pC, the electron bunch duration and timing jitter are 25 fs and less than 10 fs, respectively.

Two-dimensional (2D) indium selenide (InSe) has been widely studied for application in transistors and photodetectors, which benefit from its excellent optoelectronic properties. Among the three specific polytypes (γ-, ϵ- and β-phase) of InSe, only the crystal lattice of InSe in β-phase (β-InSe) belongs to a non-symmetry point group of $D_{6h}^4$, which indicates stronger anisotropic transport behavior and potential in the polarized photodetection of β-InSe-based optoelectronic devices. Therefore, we prepare the stable p-type 2D-layered β-InSe via temperature gradient method. The anisotropic Raman, transport and photoresponse properties of β-InSe have been experimentally and theoretically proven, showing that the β-InSe-based device has a ratio of 3.76 for the maximum to minimum dark current at two orthogonal orientations and a high photocurrent anisotropic ratio of 0.70 at 1 V bias voltage, respectively. The appealing anisotropic properties demonstrated in this work clearly identify β-InSe as a competitive candidate for filter-free polarization-sensitive photodetectors.

We report the dielectric tensors on the cleavage plane of biaxial SnSxSe1-x alloys in the spectral energy region from 0.74 to 6.42 eV obtained by spectroscopic ellipsometry. Single-crystal SnSxSe1-x alloys were grown by the temperature-gradient method. Strongly anisotropic optical responses are observed along the different principal axes. An approximate solution yields the anisotropic dielectric functions along the zigzag (a-axis) and armchair (b-axis) directions. The critical point (CP) energies of SnSxSe1-x alloys are obtained by analyzing numerically calculated second derivatives, and their physical origins are identified by energy band structure. Blue shifts of the CPs are observed with increasing S composition. The fundamental bandgap for Se = 0.8 and 1 in the armchair axis arises from band-to-band transitions at the M0 minimum point instead of the M1 saddle point as in SnS. These optical data will be useful for designing optoelectronic devices based on SnSxSe1-x alloys.

We explore strain-modulated helimagnetism in highly crystalline MnP nanorod films grown on Si(100) substrates using molecular beam epitaxy. The strained MnP film exhibits a paramagnetic to ferromagnetic (PM-FM) phase transition at TC ~ 279 K, and the FM to helical phase transition at TN ~ 110 K. The value of TN is greater than TN ~ 47 K for the MnP single crystal, indicating strong strain-modulated helimagnetic states in the MnP nanorod film. The presence of significant thermal hysteresis in the helical phase indicates coexistence of competing magnetic interactions, leading to the first-order metamagnetic transition. Similar to its single crystal counterpart, an anisotropic magnetic effect is observed in the MnP film, which is independently confirmed by magnetic hysteresis loop and radio-frequency transverse susceptibility (TS) measurements. The evolution of screw (SCR) to CONE and FAN phase is precisely tracked from magnetization versus magnetic field/temperature measurements. The temperature dependence of the anisotropy fields, extracted from the TS spectra, yields further insight into the competing nature of the magnetic phases. Unfolding of the different helical phases at T < 120 K (~TN) is analyzed by the temperature- and field-dependent magnetic entropy change. Based on these findings, the comprehensive magnetic phase diagrams of the MnP nanorod film are constructed for the first time for both the in-plane and out-of-plane magnetic field directions, revealing emergent strain/dimensionality-driven helical magnetic features that are absent in the magnetic phase diagram of the MnP single crystal., 9 figures

We report the temperature dependence of the dielectric function ε = ε1 + iε2 and critical point (CP) energies of biaxial α-SnS in the spectral energy region from 0.74 to 6.42 eV and temperatures from 27 to 350 K using spectroscopic ellipsometry. Bulk SnS was grown by temperature gradient method. Dielectric response functions were obtained using multilayer calculations to remove artifacts due to surface roughness. We observe sharpening and blue-shifting of CPs with decreasing temperature. A strong exciton effect is detected only in the armchair direction at low temperature. New CPs are observed at low temperature that cannot be detected at room temperature. The temperature dependences of the CP energies were determined by fitting the data to the phenomenological expression that contains the Bose–Einstein statistical factor and the temperature coefficient for describing the electron–phonon interaction.

Recent advances in two-dimensional (2D) crystals make it possible to realize an ideal interface structure that is required for device applications. Specifically, a p-n junction made of 2D crystals is predicted to exhibit an atomically well-defined interface that will lead to high device performance. Using angle-resolved photoemission spectroscopy, a simple surface treatment was shown to allow the possible formation of such an interface. Ta adsorption on the surface of a p-doped SnSe shifts the valence band maximum towards higher binding energy due to the charge transfer from Ta to SnSe that is highly localized at the surface due to the layered structure of SnSe. As a result, the charge carriers of the surface are changed from holes of its bulk characteristics to electrons, while the bulk remains as a p-type semiconductor. This observation suggests that the well-defined interface of a p-n junction with an atomically thin {\it n}-region is formed between Ta-adsorbed surface and bulk., 4 figures

The evolution of the optical phonons in layered semiconductor alloys SnSe(1–x)Sx is studied as a function of the composition by using polarized Raman spectroscopy with six different excitation wavelengths (784.8, 632.8, 532, 514.5, 488, and 441.6 nm). The polarization dependences of the phonon modes are compared with transmission electron diffraction measurements to determine the crystallographic orientation of the samples. Some of the Raman modes show significant variation in their polarization behavior depending on the excitation wavelengths. It is established that the maximum intensity direction of the Ag2 mode of SnSe(1−x)Sx (0 ≤ x ≤ 1) does not depend on the excitation wavelength and corresponds to the armchair direction. It is additionally found that the lower-frequency Raman modes of Ag1, Ag2 and B3g1 in the alloys show the typical one-mode behavior of optical phonons, whereas the higher-frequency modes of B3g2, Ag3 and Ag4 show two-mode behavior.

Gallium selenide (GaSe) is one of layered group-III metal monochalcogenides, which has an indirect bandgap in monolayer and direct bandgap in bulk unlike other conventional transition metal dichalcogenides (TMDs) such as MoX2 and WX2 (X=S and Se). Four polytypes of bulk GaSe, designated as beta-, epsilon-, gamma-, and delta-GaSe, have been reported. Since different polytypes result in different optical and electrical properties even for the same thickness, identifying the polytype is essential in utilizing this material for various optoelectronic applications. We performed polarized Raman measurement on GaSe and found different ultra-low-frequency Raman spectra of inter-layer vibrational modes even for the same thickness due to different stacking sequences of the polytypes. By comparing the ultra-low-frequency Raman spectra with theoretical calculations and high-resolution electron microscopy measurements, we established the correlation between the ultra-low-frequency Raman spectra and the stacking sequences for trilayer GaSe. We further found that the AB-type stacking is more stable than the AA'-type stacking in GaSe.

Non-magnetic (NM) metals with strong spin-orbit coupling have been recently explored as a probe of interface magnetism on ferromagnetic insulators (FMI) by means of the spin Hall magnetoresistance (SMR) effect. In NM/FMI heterostructures, increasing the spin mixing conductance (SMC) at the interface comes as an important step towards devices with maximized SMR. Here we report on the study of SMR in Pt/Fe3O4 bilayers at cryogenic temperature, and identify a strong dependence of the determined real part of the complex SMC on the interface roughness. We tune the roughness of the Pt/Fe3O4 interface by controlling the growth conditions of the Fe3O4 films, namely by varying the thickness, growth technique, and post-annealing processes. Field-dependent and angular-dependent magnetoresistance measurements sustain the clear observation of SMR. The determined real part of the complex SMC of the Pt/Fe3O4 bilayers ranges from 4.96 × 1014 Ω−1 m−2 to 7.16 × 1014 Ω−1 m−2 and increases with the roughness of the Fe3O4 underlayer. We demonstrate experimentally that the interface morphology, acting as an effective interlayer potential, leads to an enhancement of the spin mixing conductance.

We demonstrate a high-performance photodetector with multilayer tin diselenide (SnSe2) exfoliated from a high-quality crystal which was synthesized by the temperature gradient growth method. This SnSe2 photodetector exhibits high photoresponsivity of 5.11 × 105 A W-1 and high specific detectivity of 2.79 × 1013 Jones under laser irradiation (λ = 450 nm). We also observed a reproducible and stable time-resolved photoresponse to the incident laser beam from this SnSe2 photodetector, which can be used as a promising material for future optoelectronic applications.

In this paper, thermoelectric performance of the ZnO thin films were investigated via doping (Gallium - Ga and Indium - In) and post-thermal treatment. Various kinds of defects, such as zinc (Zn) vacancies, Ga substitute for Zn, zinc interstitials, oxygen vacancies, oxygen interstitials, oxygen antisite, were induced in the ZnO thin films by doping with Ga, In and post-thermal treatment. Annealed thin films have better thermoelectric performance than unannealed thin films. The figure of merit ZT values at 300 °C were 0.114 and 0.186 for the single Ga-doped ZnO (GZO@500) and dually In, Ga doped ZnO (IGZO@500) thin films annealed at 500 °C, respectively. Higher concentration of zinc interstitial led the GZO@500 thin film to have larger power factor and larger total thermal conductivity, resulting in lower ZT than the IGZO@500 thin film. To the best of our knowledge, the ZT value of 0.186 at 300 °C obtained from our IGZO@500 thin films is the highest ever reported for n-type ZnO based thin films.

SnSe is a 2D semiconductor with an indirect energy gap of 0.86 - 1 eV; it is widely used in solar cell, optoelectronics, and electronic device applications. Recently, SnSe has been considered as a robust candidate for energy conversion applications due to its high thermoelectric performance (ZT = 2.6 in p-type and 2.2 in n-type), which is assigned mainly to its anhamornic bonding leading to an ultralow thermal conductivity. In this review, we first discuss the crystalline and electronic structures of SnSe and the source of its p-type characteristic. Then, some typical single crystal and polycrystal growth techniques, as well as an epitaxial thin film growth technique, are outlined. The reported thermoelectric properties of SnSe grown by using each technique are also reviewed. Finally, we will describe some remaining issues concerning the use of SnSe for thermoelectric applications.

In this work, we report on the structural and thermoelectric properties of Sb2Te3 films deposited on GaSb(111) substrates by using molecular beam epitaxy. The effects of the growth temperature on the microstructure and thermoelectric properties of the films were investigated. The results show that Sb2Te3 films grow on GaSb(111) along (00l) axis normal to the substrate and have a hexagonal structure with a layer-by-layer growth mode in growth temperature range from 200 to 250 °C while at 175 and 300 °C, the films show an island growth mode. Te and Sb2Te3 phases coexist at a growth temperature of 175 °C. The films exhibit a metallic behavior for growth temperatures below 250 °C and a semiconductor behavior at 300 °C. By changing growth temperature, we were able to vary the carrier density from 9.96×1018 to 4.55×1019 cm −3. At room temperature, the Seebeck coefficients are 110, 146, and 138 μV/K for growth temperatures of 175, 200 and 250 °C, respectively, and a large value of the power factor 61.67 μW/cm-K2 is achieved for the film grown at 250 °C.

Fe 2 SiO 4 thin films have been grown on n-type, p-type and semi-insulating Si(100) substrates by molecular beam epitaxy. When Fe-O thin films were deposited on Si(100) substrate at 300 °C, the film reacted with Si, resulting in a Fe 2 SiO 4 film because of the high reactivity between Fe and Si. The electrical resistance and Seebeck coefficient of Fe 2 SiO 4 thin films grown were different in different doping states. On n-type and p-type Si(100), the electrical resistance decreased suddenly and increased again at 350 and 250 K, respectively, while on semi-insulating Si(100), it exhibited typical semiconducting resistance behavior. We observed similar crossovers at 350 and 250 K in temperature dependent Seebeck coefficients on n-type and p-type Si(100), respectively. These results suggest that the measured electrical and thermoelectric properties originate from Si substrate.

We report on the structural and magneto-transport properties of the as-grown and oxidized Mn:Ge magnetic semiconductors. Based on X-ray diffraction and X-ray photoelectron spectroscopy results, the samples annealed at 650 and 700 °C became fully oxidized and the chemical binding energies of Mn was found to be Mn3O4. Thus, the system became Mn3O4 clusters embedded in Ge1−yOy. The as-grown sample showed positive linear Hall effect and negligible negative magnetoresistance (MR), which trend remained for the sample annealed up to 550 °C. Interestingly, for the samples annealed at above 650 °C, we observed the anomalous Hall effect around 45 K and the giant positive MR, which are respectively 59.2% and 78.5% at 7 kOe annealed at 650 °C and 700 °C.

A perspective magneto-thermo-electric cooling device (MTECD) comprising a central magnetocaloric (MC) material (e.g., Gd) sandwiched by two thermoelectric (TE) materials (e.g., MnP) is proposed. The presence of the TE materials in the MTECD guides the heat flow direction and enhances heat pulsation. In this case, the usage of a ferromagnetic TE material that combines large TE with small MC properties within a similar temperature region can enhance the magnetic flux density and heat exchange efficiency. Here, we show that MnP nanorod-structured films with desired magnetic, MC and TE properties are very promising for use in MTECDs. The films were grown on Si substrates at 300, 400 and 500{\deg}C using molecular beam epitaxy. The 400 oC sample shows a desired TE and MC combination. A large power factor of 24.06 {\mu}W m-1 K-2 is achieved at room temperature. In this temperature region, the film exhibits a small MC effect (-deltaSM ~0.64 J/kg K and deltaTad ~0.3 K at m0H = 2 T) but ferromagnetism that gives rise to the enhanced MC effect of the central MC material. These properties could enable the MTECD to operate at high frequency., Comment: Accepted in Physics Status Solidi A