Enhanced thermoelectric performance of rough silicon nanowires

Approximately 90 per cent of the world’s power is generated by heat engines that use fossil fuel combustion as a heat source and typically operate at 30–40 per cent efficiency, such that roughly 15 terawatts of heat is lost to the environment. Thermoelectric modules could potentially convert part of this low-grade waste heat to electricity. Their efficiency depends on the thermoelectric figure of merit ZT of their material components, which is a function of the Seebeck coefficient, electrical resistivity, thermal conductivity and absolute temperature. Over the past five decades it has been challenging to increase ZT > 1, since the parameters of ZT are generally interdependent. While nanostructured thermoelectric materials can increase ZT > 1 (refs 2–4), the materials (Bi, Te, Pb, Sb, and Ag) and processes used are not often easy to scale to practically useful dimensions. Here we report the electrochemical synthesis of large-area, wafer-scale arrays of rough Si nanowires that are 20–300 nm in diameter. These nanowires have Seebeck coefficient and electrical resistivity values that are the same as doped bulk Si, but those with diameters of about 50 nm exhibit 100-fold reduction in thermal conductivity, yielding ZT = 0.6 at room temperature. For such nanowires, the lattice contribution to thermal conductivity approaches the amorphous limit for Si, which cannot be explained by current theories. Although bulk Si is a poor thermoelectric material, by greatly reducing thermal conductivity without much affecting the Seebeck coefficient and electrical resistivity, Si nanowire arrays show promise as high-performance, scalable thermoelectric materials.

[1]  T. Geballe,et al.  Seebeck Effect in Silicon , 1955 .

[2]  S. M. Sze,et al.  Physics of semiconductor devices , 1969 .

[3]  Paul G. Klemens,et al.  Thermophysical properties of matter - the TPRC data series. Volume 1. Thermal conductivity - metallic elements and alloys. (Reannouncement). Data book , 1970 .

[4]  M. Brinson,et al.  Thermal conductivity and thermoelectric power of heavily doped n-type silicon , 1970 .

[5]  Y. S. Touloukian Thermal conductivity: metallic elements and alloys , 1971 .

[6]  Pohl,et al.  Thermal conductivity of amorphous solids above the plateau. , 1987, Physical review. B, Condensed matter.

[7]  L. Weber,et al.  Transport properties of silicon , 1991 .

[8]  Watson,et al.  Lower limit to the thermal conductivity of disordered crystals. , 1992, Physical review. B, Condensed matter.

[9]  D. Rowe CRC Handbook of Thermoelectrics , 1995 .

[10]  Kenneth E. Goodson,et al.  PHONON-BOUNDARY SCATTERING IN THIN SILICON LAYERS , 1997 .

[11]  S. Wong,et al.  Temperature-Dependent Thermal Conductivity of Single-Crystal Silicon Layers in SOI Substrates , 1996, Microelectromechanical Systems (MEMS).

[12]  Kenneth E. Goodson,et al.  Phonon scattering in silicon films with thickness of order 100 nm , 1999 .

[13]  R. W. Henn,et al.  Thermal conductivity of isotopically enriched silicon , 2000 .

[14]  George S. Nolas,et al.  Thermoelectrics: Basic Principles and New Materials Developments , 2001 .

[15]  Alexander A. Balandin,et al.  Phonon heat conduction in a semiconductor nanowire , 2001 .

[16]  R. Venkatasubramanian,et al.  Thin-film thermoelectric devices with high room-temperature figures of merit , 2001, Nature.

[17]  Yunjie Yan,et al.  Synthesis of Large‐Area Silicon Nanowire Arrays via Self‐Assembling Nanoelectrochemistry , 2002 .

[18]  M. P. Walsh,et al.  Quantum Dot Superlattice Thermoelectric Materials and Devices , 2002, Science.

[19]  A. Majumdar,et al.  Predicting the thermal conductivity of Si and Ge nanowires , 2003 .

[20]  Li Shi,et al.  Measuring Thermal and Thermoelectric Properties of One-Dimensional Nanostructures Using a Microfabricated Device , 2003 .

[21]  Yiying Wu,et al.  Thermal conductivity of individual silicon nanowires , 2003 .

[22]  Yunjie Yan,et al.  Dendrite‐Assisted Growth of Silicon Nanowires in Electroless Metal Deposition , 2003 .

[23]  A. Majumdar Thermoelectricity in Semiconductor Nanostructures , 2004, Science.

[24]  M. Kanatzidis,et al.  Cubic AgPbmSbTe2+m: Bulk Thermoelectric Materials with High Figure of Merit , 2004, Science.

[25]  Wei Chen,et al.  Cubic : Bulk Thermoelectric Materials with High Figure of Merit , 2004 .

[26]  Peidong Yang,et al.  Controlled growth of Si nanowire arrays for device integration. , 2005, Nano letters.

[27]  Yin Wu,et al.  Uniform, axial-orientation alignment of one-dimensional single-crystal silicon nanostructure arrays. , 2005, Angewandte Chemie.

[28]  Dmitri O. Klenov,et al.  Thermal conductivity reduction and thermoelectric figure of merit increase by embedding nanoparticles in crystalline semiconductors. , 2006, Physical review letters.

[29]  Monte Carlo simulation of phonon backscattering in a nanowire , 2006 .