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After more than three decades of molecular and carbon-based electronics, the creation of air- and thermally stable n-type materials remains a challenge in the development of future p/n junction devices such as solar cells and thermoelectric modules. Here a series of ordinary salts are reported such as sodium chloride (NaCl), sodium hydroxide (NaOH), and potassium hydroxide (KOH) with crown ethers as new doping reagents for converting single-walled carbon nanotubes to stable n-type materials. Thermoelectric analyses reveal that these new n-type single-walled carbon nanotubes display remarkable air stability even at 100 °C for more than 1 month. Their thermoelectric properties with a dimensionless figure-of-merit (ZT) of 0.1 make these new n-type single-walled carbon nanotubes a most promising candidate for future n-type carbon-based thermoelectric materials., Grant-in-Aid for Young Scientists (B) of Japan Society for the Promotion of Science. Grant Number: 26790014

We have estimated the thermal conductivity of nanocrystalline bismuth telluride thin films using the differential 3ω method, taking into account the thermal contact resistance (TCR) between the substrate and thin-film layers. The thin films were prepared on alumina substrates by radio-frequency (RF) magnetron sputtering at temperature of 200°C. Film thickness varied between 0.8 μm and 3.1 μm. The structural properties of the films were analyzed using x-ray diffraction analysis. Their electrical conductivity, Seebeck coefficient, and power factor were evaluated. For measurement of thermal properties by the differential 3ω method, SiO2 thin films were deposited onto the samples, to act as insulating layers. Thin aluminum wire was then patterned onto the SiO2 layer. The observed variations in temperature amplitude as a function of film thickness indicated that the TCR contribution was very small and could therefore be neglected when estimating the thermal conductivity of the thin films. The thermal conductivity of the nanocrystalline bismuth telluride thin films with thickness of 0.8 μm and 2.1 μm were determined to be 0.55 W/(m K) and 0.48 W/(m K), respectively.

The effects of homogeneous irradiation of electron beam (EB) on the crystal growth and thermoelectric properties of nanocrystalline bismuth selenium telluride thin films were investigated. The thin films were prepared using a flash evaporation method, after which EB irradiation was performed under N 2 at room temperature at an accelerated voltage of 0.17 MeV. SEM revealed that the untreated thin film was composed of a large quantity of rice-like nanostructures. With increasing the EB irradiation dose, a number of nanodots with diameters of less than 10 nm became visible on the surface of the rice-like nanostructures. The crystallinity and the crystal orientation were enhanced with increasing EB irradiation dose while the average crystal grain size remained almost the same size as that of the untreated thin film. In terms of thermoelectric properties, the mobility of the thin films was enhanced as the EB irradiation dose was increased while the carrier concentration was not greatly changed. As a result, both the electrical conductivity and the Seebeck coefficient were improved with increasing EB irradiation dose. Consequently, even though there is still room for further improvement, the power factor was enhanced around sevenfold (from 0.14 to 0.96 μW/cm/K 2 ) by the EB irradiation treatment.

We investigated the effects of strain and grain size on the thermal transport of highly-oriented nanocrystalline bismuth antimony telluride thin films using both experimental studies and modeling. The fabricated thin films had preferred crystal orientation along the c-axis, average grain sizes of 30 < d < 100 nm, and strain of −0.8% < e < −1.4% in the c-axis direction, whereas the strain in the a–b-axis direction was constant at 1.7%. The thermal conductivities were measured to be 0.32 < κ < 0.52 W/m/K using a 3ω method at room temperature. To gain insight into the thermal transport in the strained nanocrystalline thin films, we estimated the lattice thermal conductivities from the measured thermal conductivities. We then calculated the lattice thermal conductivity using a simplified phonon transport model that accounts for the strain effect based on the Christoffel equation and uses Lennard–Jones potentials, and the grain size effect based on the full distribution of mean free paths. The theoretical calculations were in good agreement with our experimental results, and we conclude that the decrease of the lattice thermal conductivity of nanocrystalline thin films can be mainly attributed to the nano-size effect rather than the strain effect.

The microstructure of materials affects thermal and electrical transport as well as the physical properties. The effects of the microstructure on both thermal and electrical transport in silicon membranes with periodic microporous structures produced from silicon-on-insulator wafers using microfabrication processes were studied. The in-plane thermal and electrical conductivities of the Si membranes were measured simultaneously by using a self-heating method. The measured thermal conductivity was compared with the result from the periodically laser-heating method. The thermal and electrical conductivities were much lower in the porous membranes than in the non-porous membrane. The measured thermal conductivity was much lower than expected based on values determined using classical models. A significant phonon size effect was observed even in microsized structures, and the mean free path for phonons was very long. It was concluded that phonon transport is quasi-ballistic and electron transport is diffuse in microporous Si structures. It was suggested that the microstructure had a different effect on thermal and electrical transport.

In this study, we investigated the effect of the structure of microporous p-type (Bi0.4Te3Sb1.6) and n-type (Bi2.0Te2.7Se0.3) BiTe-based thin films on their thermoelectric performance. High-aspect-ratio porous thin films with pore depth greater than 1 μm and pore diameter ranging from 300 nm to 500 nm were prepared by oxygen plasma etching of polyimide (PI) layers capped with a heat-resistant block copolymer, which acted as the template. The cross-plane thermal conductivities of the porous p- and n-type thin films were 0.4 W m−1 K−1 and 0.42 W m−1 K−1, respectively, and the dimensionless figures of merit, ZT, of the p- and n-type BiTe films were estimated as 1.0 and 1.0, respectively, at room temperature. A prototype thermoelectric module consisting of 20 pairs of p- and n-type strips over an area of 3 cm × 5 cm was fabricated on the porous PI substrate. This module produced an output power of 0.1 mW and an output voltage of 0.6 V for a temperature difference of 130°C. The output power of the submicrostructured module was 1.5 times greater than that of a module based on smooth BiTe-based thin films. Thus, the thermoelectric performance of the thin films was improved owing to their submicroscale structure.

We prepared both n- and p-type bismuth telluride thin films by using a coaxial-type vacuum arc evaporation method. The atomic compositions of the as-grown thin films and several annealed thin films were comparable to that of bulk bismuth telluride. Their thermoelectric properties were measured and found to be comparable to those of bulk materials. The Seebeck coefficient and electrical conductivity of the as-grown thin films were improved by the annealing process. The measured figures of merit (ZT) of the films were 0.86 for the n-type and 0.41 for the p-type at 300 K for annealing temperatures of 573 K and 523 K, respectively.

We prepared a mixture of thermoelectric bismuth telluride particles, a conductive polymer [poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)], poly(acrylic acid) (PAA), and several organic additives to fabricate thermoelectric films using printing or coating techniques. In the mixture, the organic components (PEDOT:PSS, PAA, and an additive) act as a binder to connect bismuth telluride particles mechanically and electrically. Among the organic additives used, glycerol significantly enhanced the electrical conductivity and bismuth telluride particle dispersibility in the mixture. Bi0.4Te3.0Sb1.6 films fabricated by spin-coating the mixture showed a thermoelectric figure of merit (ZT) of 0.2 at 300 K when the Bi0.4Te3Sb1.6 particle diameter was 2.8 μm and its concentration in the elastic films was 95 wt.%.

To investigate the effect of strain on bismuth telluride films, we applied different compressive and tensile strains to thin films by changing the bending radius of a flexible substrate so the strain ranged from −0.3% (compressive) to +0.3% (tensile). The structural properties of the strained thin films, composed of nanosized grains, were analyzed by x-ray diffraction and scanning electron microscopy. For all samples the main peak was the (015) diffraction peak; crystal orientation along the (015) growth direction was slightly enhanced by application of compressive strain. The thermoelectric properties of strained bismuth telluride thin films were evaluated by measurement of electrical conductivity, Seebeck coefficient, and power factor. The magnitude and direction of the applied strain did not significantly affect the power factor, because when the strain changed from compressive to tensile the electrical conductivity increased and the absolute Seebeck coefficient decreased.

A two-step method that combines homogeneous electron beam (EB) irradiation and thermal annealing has been developed to enhance the thermoelectric properties of nanocrystalline bismuth selenium telluride thin films. The thin films, prepared using a flash evaporation method, were treated with EB irradiation in a N2 atmosphere at room temperature and an acceleration voltage of 0.17 MeV. Thermal annealing was performed under Ar/H2 (5%) at 300 °C for 60 min. X-ray diffraction was used to determine that compositional phase separation between bismuth telluride and bismuth selenium telluride developed in the thin films exposed to higher EB doses and thermal annealing. We propose that the phase separation was induced by fluctuations in the distribution of selenium atoms after EB irradiation, followed by the migration of selenium atoms to more stable sites during thermal annealing. As a result, thin film crystallinity improved and mobility was significantly enhanced. This indicates that the phase separation resulti...

Here, we investigate the combined effect of the nanoscale crystal grains and porosity on the lattice thermal conductivity of bismuth-telluride-based bulk alloys using both experimental studies and modeling. The fabricated bulk alloys exhibit average grain sizes of 30

The in-plane effective thermal conductivity of free-standing Si thin films with periodic micropores was measured at -100 to 0 °C. The Si thin films with micropores were prepared from silicon-on-insulator (SOI) wafers by standard microfabrication processes. The dimensions of the free-standing Si thin films were 200μm×150μm×2 μm, with staggered 4 μm pores having an average pitch of 4 mm. The Si thin film serves both as a heater and thermometer. The average temperature rise of the thin film is a function of its in-plane thermal conductivity. The effective thermal conductivity was calculated using a simple one-dimensional heat conduction model. The measured thermal conductivity was much lower than that expected based on classical model evaluations. A significant phonon size effect was observed even in the microsized structures, and the mean free path for phonons is very long even at the room temperature.