Seong Gi Jeon

Twin-driven thermoelectric figure-of-merit enhancement of Bi2Te3 nanowires

Thermoelectric figure-of-merits (ZT) are enhanced or degraded by crystal defects such as twins and excess atoms that are correlated with thermal conductivity (k) and carrier concentration (n). For Bi2Te3, it is unclear whether the crystal defects can enhance ZT without a degradation in the thermopower factor. In the present study, n-type Bi2Te3 nanowires (NWs) are electrochemically synthesized to have twin-free (TF) or twin-containing (TC) microstructures with a ZT of 0.10 and 0.08, respectively, at 300 K. The ZTs of TF and TC NWs remarkably increase up to 0.21 and 0.31, when heat-treatments cause n-reduction and twins induce phonon scattering, as follows: first, the enhancement of the Seebeck coefficient from -70 to -98 μV K(-1) for TF NWs and from -57 to -143 μV K(-1) for TC NWs, by virtue of n-reduction; secondly, twin-driven k-reduction from 1.9 to 1.4 W m(-1) K(-1) of TC NWs, while the k of TF NWs increases from 2.3 to 2.6 W m(-1) K(-1) due to the enhanced carrier mobility. The lattice thermal conductivities of TC NW are lowered from 1.1 to 0.8 W m(-1) K(-1) by phonon scattering at twins. Density functional theory calculations indicate that twins do not significantly influence the Seebeck coefficient of Bi2Te3. It is strongly recommended that twins be incorporated with an optimum carrier concentration to enhance the ZT of Bi2Te3.

Monolithic Bi1.5Sb0.5Te3 ternary alloys with a periodic 3D nanostructure for enhancing thermoelectric performance

The selective reduction of thermal conductivity while preserving the Seebeck coefficient and electrical conductivity is regarded as a key strategy for achieving the high dimensionless figure-of-merit (ZT) of thermoelectric materials. Here, we newly propose a periodic three-dimensional (3D) nanostructure that has an ability to significantly reduce thermal conductivity, resulting in an improved ZT value of thermoelectric materials near room temperature. A 3D nanostructured thermoelectric monolith is developed by electrochemical deposition of a Bi–Sb–Te ternary alloy into a highly ordered, interstitial porous network in an epoxy template predefined by advanced lithography. The resultant inch-scale, bicontinuous nanocomposite monolith released from a substrate can be easily transferred to a customized reliable platform for evaluating thermoelectric properties. The measured thermal conductivity is only ∼0.89 W mK−1 at 350 K due to greatly increased phonon boundary scattering without any degradation in the Seebeck coefficient and electrical conductivity, leading to an enhanced ZT value (∼0.56) which is ∼50% higher than that of an ordinary film with the same elemental composition. The 3D nanostructure developed here will provide new design opportunities for nanostructured thermoelectric materials, potentially usable in flexible thermoelectric coolers and wearable energy harvesting systems.

Effect of the Thermal Conductivity on Resistive Switching in GeTe and Ge2Sb2Te5 Nanowires.

The thermal conduction characteristics of GeTe and Ge2Sb2Te5(GST) nanowires were investigated using an optical method to determine the local temperature by Raman spectroscopy. Since the localization of surface charge in a single-crystalline nanostructure can enhance charge-phonon scattering, the thermal conductivity value (κ) of single crystalline GeTe and GST nanowires was decreased significantly to 1.44 Wm(-1) K(-1) for GeTe and 1.13 Wm(-1) K(-1) for GST, compared to reported values for polycrystalline structures. The SET-to-RESET state in single-crystalline GeTe and GST nanowires are characteristic of a memory device. Unlike previous reports using GeTe and GST nanowires, the SET-to-RESET characteristics showed a bipolar switching shape and no unipolar switching. In addition, after multiple cycles of operation, a significant change in morphology and composition was observed without any structural phase transition, indicating that atoms migrate toward the cathode or anode, depending on their electronegativities. This change caused by a field effect indicates that the structural phase transition does not occur in the case of GeTe and GST nanowires with a significantly lowered thermal conductivity and stable crystalline structure. Finally, the formation of voids and hillocks as the result of the electromigration critically degrades device reliability.

Structural and electrical properties of catalyst-free Si-doped InAs nanowires formed on Si(111)

We report structural and electrical properties of catalyst-free Si-doped InAs nanowires (NWs) formed on Si(111) substrates. The average diameter of Si-doped InAs NWs was almost similar to that of undoped NWs with a slight increase in height. In the previous works, the shape and size of InAs NWs formed on metallic catalysts or patterned structures were significantly changed by introducing dopants. Even though the external shape and size of the Si-doped NWs in this work were not changed, crystal structures inside the NWs were significantly changed. For the undoped InAs NWs, both zincblende (ZB) and wurzite (WZ) structures were observed in transmission-electron microscope images, where the portion of WZ structure was estimated to be more than 30%. However, only ZB was observed with an increase in stacking fault (SF) for the Si-doped NWs. The undoped and Si-doped InAs NWs were used as channels of four-point electrical measurements with Al/Ni electrodes to investigate electrical properties. The resistivity calculated from the current-voltage curve of a Si-doped InAs NW showed 1.32 × 10−3 Ωcm, which was dramatically decreased from 10.14 × 10−3 Ωcm for the undoped InAs NW. A relatively low resistivity of catalyst-free Si-doped InAs NWs was achieved without significant change in structural dimensions.

Effects of doping and planar defects on the thermoelectric properties of InAs nanowires

Undoped InAs and Si-doped InAs nanowires with stacking faults and twins were synthesized by catalyst-free molecular beam epitaxy and their thermoelectric enhancements due to planar defects were experimentally and theoretically demonstrated. The Seebeck coefficients, electrical resistivities, and thermal conductivities of the Si-doped and undoped InAs nanowires were measured using a micro-fabricated thermoelectric measurement platform over the temperature range of 50 to 300 K. The Si-doping increased electrical conductivity from 1.0 × 10−4 to 7.8 × 10−4 S m−1, due to the increase in carrier concentration from 2 × 1017 to 8 × 1017 cm−3, and then decreased the thermopower from −216 to −81 μV K−1 at 300 K, in agreement with the two-band model based on the Boltzman transport theory. Phonon scattering, caused by planar defects such as surfaces, twins, and stacking-fault boundaries, suppressed the lattice thermal conductivity below 3 W m−1 K−1 following the Callaway model. The planar defect-induced phonon scattering as well as the optimization of carrier concentration is very effective at enhancing the thermoelectric properties of InAs nanowires and is expected to be utilized for improving the thermoelectric properties of other thermoelectric materials.