Abstract
In recent year, nanoporous Si thin films have been widely studied for their potential applications in thermoelectrics, in which high thermoelectric performance can be obtained by combining both the dramatically reduced lattice thermal conductivity and bulk-like electrical properties. Along this line, a high thermoelectric figure of merit (ZT) is also anticipated for other nanoporous thin films, whose bulk counterparts possess superior electrical properties but also high lattice thermal conductivities. Numerous thermoelectric studies have been carried out on Si-based nanoporous thin films, whereas cost-effective nitrides and oxides are not systematically studied for similar thermoelectric benefits. In this work, the cross-plane thermal conductivities of nanoporous In0.1Ga0.9N thin films with varied porous patterns were measured with the time-domain thermoreflectance technique. These alloys are suggested to have better electrical properties than conventional Si x Ge1–x alloys; however, a high ZT is hindered by their intrinsically high lattice thermal conductivity, which can be addressed by introducing nanopores to scatter phonons. In contrast to previous studies using dry-etched nanopores with amorphous pore edges, the measured nanoporous thin films of this work are directly grown on a patterned sapphire substrate to minimize the structural damage by dry etching. This removes the uncertainty in the phonon transport analysis due to amorphous pore edges. Based on the measurement results, remarkable phonon size effects can be found for a thin film with periodic 300-nm-diameter pores of different patterns. This indicates that a significant amount of heat inside these alloys is still carried by phonons with ~300 nm or longer mean free paths. Our studies provide important guidance for ZT enhancement in alloys of nitrides and similar oxides.
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Johnson W, Piner E L. GaN HEMT Technology. Berlin: Springer Berlin Heidelberg, 2012
Wu Y R, Singh J. Transient study of self-heating effects in AlGaN/GaN HFETs: consequence of carrier velocities, temperature, and device performance. Journal of Applied Physics, 2007, 101(11): 113712
Rosker M, Bozada C, Dietrich H, Hung A, Via D, Binari S, Vivierios E, Cohen E, Hodiak J. The DARPA wide band gap semiconductors for RF applications (WBGS-RF) program: Phase II results. In: CS MANTECH Conference. Tampa, Florida, USA, 2009
Lee H, Agonafer D D, Won Y, Houshmand F, Gorle C, Asheghi M, Goodson K. Thermal modeling of extreme heat flux microchannel coolers for GaN-on-SiC semiconductor devices. Journal of Electronic Packaging, 2016, 138(1): 010907
Calame J P, Myers R E, Binari S C, Wood F N, Garven M. Experimental investigation of microchannel coolers for the high heat flux thermal management of GaN-on-SiC semiconductor devices. International Journal of Heat and Mass Transfer, 2007, 50(23–24): 4767–4779
Yan Z, Liu G, Khan J M, Balandin A A. Graphene quilts for thermal management of high-power GaN transistors. Nature Communications, 2012, 3(3): 199–202
Tsurumi N, Ueno H, Murata T, Ishida H, Uemoto Y, Ueda T, Inoue K, Tanaka T. AlN passivation over AlGaN/GaN HFETs for surface heat spreading. IEEE Transactions on Electron Devices, 2010, 57 (5): 980–985
Liu W, Balandin A A. Thermoelectric effects in wurtzite GaN and AlxGa1-xN alloys. Journal of Applied Physics, 2005, 97(12): 123705
Pantha B N, Dahal R, Li J, Lin J Y, Jiang H X, Pomrenke G. Thermoelectric properties of In0.3Ga0.7N alloys. Journal of Electronic Materials, 2009, 38(7): 1132–1135
Sztein A, Bowers J E, DenBaars S P, Nakamura S. Polarization field engineering of GaN/AlN/AlGaN superlattices for enhanced thermoelectric properties. Applied Physics Letters, 2014, 104(4): 042106
Sztein A, Haberstroh J, Bowers J E, Denbaars S P, Nakamura S. Calculated thermoelectric properties of InxGa1–xN, InxAl1–xN, and AlxGa1–xN. Journal of Applied Physics, 2013, 113(18): 183707
Hurwitz E N, Asghar M, Melton A, Kucukgok B, Su L, Orocz M, Jamil M, Lu N, Ferguson I T. Thermopower study of GaN-based materials for next-generation thermoelectric devices and applications. Journal of Electronic Materials, 2011, 40(5): 513–517
Goldsmid H J. Thermoelectric Refrigeration. New York: Plenum Press, 1964
Pantha B N, Dahal R, Li J, Lin J Y, Jiang H X, Pomrenke G. Thermoelectric properties of InxGa1–xN alloys. Applied Physics Letters, 2008, 92(4): 042112
Sztein A, Ohta H, Bowers J E, DenBaars S P, Nakamura S. High temperature thermoelectric properties of optimized InGaN. Journal of Applied Physics, 2011, 110(12): 123709
Cahill D G, Braun P V, Chen G, Clarke D R, Fan S, Goodson K E, Keblinski P, King W P, Mahan G D, Majumdar A, Maris H J, Phillpot S R, Pop E, Shi L. Nanoscale thermal transport. II. 2003–2012. Applied Physics Reviews, 2014, 1(1): 011305
Marconnet A M, Asheghi M, Goodson K E. From the casimir limit to phononic crystals: 20 years of phonon transport studies using silicon-on-insulator technology. Journal of Heat Transfer, 2013, 135 (6): 061601–1/10
Lim J, Wang H T, Tang J, Andrews S C, So H, Lee J, Lee D H, Russell T P, Yang P. Simultaneous thermoelectric property measurement and incoherent phonon transport in holey silicon. ACS Nano, 2016, 10(1): 124–132
Yu J K, Mitrovic S, Tham D, Varghese J, Heath J R. Reduction of thermal conductivity in phononic nanomesh structures. Nature Nanotechnology, 2010, 5(10): 718–721
Tang J, Wang H T, Lee D H, Fardy M, Huo Z, Russell T P, Yang P. Holey silicon as an efficient thermoelectric material. Nano Letters, 2010, 10(10): 4279–4283
Chen G. Nanoscale Energy Transport and Conversion: A Parallel Treatment of Electrons, Molecules, Phonons, and Photons. Oxford: Oxford University Press, 2005
Maldovan M. Narrow low-frequency spectrum and heat management by thermocrystals. Physical Review Letters, 2013, 110(2): 025902
Song D, Chen G. Thermal conductivity of periodic microporous silicon films. Applied Physics Letters, 2004, 84(5): 687–689
He Y, Donadio D, Lee J H, Grossman J C, Galli G. Thermal transport in nanoporous silicon: interplay between disorder at mesoscopic and atomic scales. ACS Nano, 2011, 5(3): 1839–1844
Ravichandran N K, Minnich A J. Coherent and incoherent thermal transport in nanomeshes. Physical Review B: Condensed Matter and Materials Physics, 2014, 89(20): 205432
Hopkins P E, Reinke C M, Su M F, Olsson R H III, Shaner E A, Leseman Z C, Serrano J R, Phinney L M, El-Kady I. Reduction in the thermal conductivity of single crystalline silicon by phononic crystal patterning. Nano Letters, 2011, 11(1): 107–112
Lee J, Lim J, Yang P. Ballistic phonon transport in holey silicon. Nano Letters, 2015, 15(5): 3273–3279
Tong T, Fu D, Levander A, Schaff W, Pantha B, Lu N, Liu B, Ferguson I, Zhang R, Lin J, Jiang H X, Wu J, Cahill D G. Suppression of thermal conductivity in InxGa1–xN alloys by nanometer-scale disorder. Applied Physics Letters, 2013, 102(12): 121906
Hsiao T K, Chang H K, Liou S C, Chu M W, Lee S C, Chang C W. Observation of room-temperature ballistic thermal conduction persisting over 8.3 mm in SiGe nanowires. Nature Nanotechnology, 2013, 8(7): 534–538
Hao Q, Xu D, Zhao H. Systematic studies of periodically nanoporous Si films for thermoelectric applications. MRS Proceedings, 2015, 1779, 27–32
Kim B, Nguyen J, Clews P J, Reinke CM, Goettler D, Leseman Z C, El-Kady I, Olsson R. Thermal conductivity manipulation in single crystal silicon via lithographycally defined phononic crystals micro electro mechanical systems (MEMS). In: 2012 IEEE 25th International Conference on Micro Electro Mechanical Systems (MEMS), 2012, 176–179
Marconnet A M, Kodama T, Asheghi M, Goodson K E. Phonon conduction in periodically porous silicon nanobridges. Nanoscale and Microscale Thermophysical Engineering, 2012, 16(4): 199–219
Nomura M, Nakagawa J, Sawano K, Maire J, Volz S. Thermal conduction in Si and SiGe phononic crystals explained by phonon mean free path spectrum. Applied Physics Letters, 2016, 109(17): 173104
Alaie S, Goettler D F, Su M, Leseman Z C, Reinke C M, El-Kady I. Thermal transport in phononic crystals and the observation of coherent phonon scattering at room temperature. Nature Communications, 2015, 6: 7228
Jain A, Yu Y J, McGaughey A J. Phonon transport in periodic silicon nanoporous films with feature sizes greater than 100 nm. Physical Review B: Condensed Matter and Materials Physics, 2013, 87(19): 195301
Choi K, Arita M, Arakawa Y. Selective-area growth of thin GaN nanowires by MOCVD. Journal of Crystal Growth, 2012, 357: 58–61
Cahill D G. Analysis of heat flow in layered structures for timedomain thermoreflectance. Review of Scientific Instruments, 2004, 75(12): 5119–5122
Krukowski S, Witek A, Adamczyk J, Jun J, Bockowski M, Grzegory I, Lucznik B, Nowak G, Wróblewski M, Presz A, Gierlotka S, Stelmach S, Palosz B, Porowski S, Zinn P. Thermal properties of indium nitride. Journal of Physics and Chemistry of Solids, 1998, 59(3): 289–295
Leitner J, Strejc A, Sedmidubský D, Růžička K. High temperature enthalpy and heat capacity of GaN. Thermochimica Acta, 2003, 401 (2): 169–173
Oh D W, Ravichandran J, Liang C W, Siemons W, Jalan B, Brooks C M, Huijben M, Schlom D G, Stemmer S, Martin L W, Majumdar A, Ramesh R, Cahill D G. Thermal conductivity as a metric for the crystalline quality of SrTiO3 epitaxial layers. Applied Physics Letters, 2011, 98(22): 221904
Zhu J, Zhu Y, Wu X, Song H, Zhang Y, Wang X. Structure-thermal property correlation of aligned silicon dioxide nanorod arrays. Applied Physics Letters, 2016, 108(23): 231903
Majumdar A. Microscale heat conduction in dielectric thin films. Journal of Heat Transfer, 1993, 115(1): 7–16
Jeong C, Datta S, Lundstrom M. Thermal conductivity of bulk and thin-film silicon: a Landauer approach. Journal of Applied Physics, 2012, 111(9): 093708
Hua Y C, Cao B Y. Cross-plane heat conduction in nanoporous silicon thin films by phonon Boltzmann transport equation and Monte Carlo simulations. Applied Thermal Engineering, 2017, 111: 1401–1408
Hao Q, Xiao Y, Zhao H. Characteristic length of phonon transport within periodic nanoporous thin films and two-dimensional materials. Journal of Applied Physics, 2016, 120(6): 065101
Liu W, Balandin A A. Thermal conduction in AlxGa1–xN alloys and thin films. Journal of Applied Physics, 2005, 97(7): 073710
Dames C, Chen G. Theoretical phonon thermal conductivity of Si/Ge superlattice nanowires. Journal of Applied Physics, 2004, 95(2): 682–693
Dames C, Chen G. Thermal conductivity of nanostructured thermoelectric materials. In: Rowe D M ed. Thermoelectrics Handbook: Macro to Nano. Boca Raton, USA: CRC Press 2005, 42:1–16
Toberer E S, Zevalkink A, Snyder G J. Phonon engineering through crystal chemistry. Journal of Materials Chemistry, 2011, 21(40): 15843–15852
Klemens P G. Theory of thermal conductivity in solids. In: Tye R P ed. Thermal Conductivity. London: Academic Press, 1969, 1–68
Roufosse M, Klemens P G. Thermal conductivity of complex dielectric crystals. Physical Review B: Condensed Matter and Materials Physics, 1973, 7(12): 5379–5386
Julian C L. Theory of heat conduction in rare-gas crystals. Physical Review, 1965, 137(1A): A128–A137
Slack G A, Galginaitis S. Thermal conductivity and phonon scattering by magnetic impurities in CdTe. Physical Review, 1964, 133(1A): A253–A268
Leibfried G, Schloemann E. Thermal conductivity of dielectric solids by a variational technique. Nachr Akad Wiss Goettingen, Math-Phys Kl, 2A. Math-Phys-Chem Abt, 1954, 23: 1366–1370
Freedman J P, Leach J H, Preble E A, Sitar Z, Davis R F, Malen J A. Universal phonon mean free path spectra in crystalline semiconductors at high temperature. Scientific Reports, 2013, 3(1): 2963
Yang F, Dames C. Mean free path spectra as a tool to understand thermal conductivity in bulk and nanostructures. Physical Review B: Condensed Matter and Materials Physics, 2013, 87(3): 035437
Lindsay L, Broido D, Reinecke T. Thermal conductivity and large isotope effect in GaN from first principles. Physical Review Letters, 2012, 109(9): 095901
Mion C, Muth J, Preble E, Hanser D. Accurate dependence of gallium nitride thermal conductivity on dislocation density. Applied Physics Letters, 2006, 89(9): 092123
Tamura S I. Isotope scattering of dispersive phonons in Ge. Physical Review B: Condensed Matter and Materials Physics, 1983, 27(2): 858–866
Ziman J M. Electrons and Phonons: the Theory of Transport Phenomena in Solids. Oxford: Oxford University Press, 2001
Klemens P G. The scattering of low-frequency lattice waves by static imperfections. Proceedings of the Physical Society. Section A, 1955, 68(12): 1113–1128
Wright A. Elastic properties of zinc-blende and wurtzite AlN, GaN, and InN. Journal of Applied Physics, 1997, 82(6): 2833–2839
Pantha B, Dahal R, Li J, Lin J, Jiang H, Pomrenke G. Thermoelectric properties of InxGa1–xN alloys. Applied Physics Letters, 2008, 92(4): 042112
Regner K T, Sellan D P, Su Z, Amon C H, McGaughey A J, Malen J A. Broadband phonon mean free path contributions to thermal conductivity measured using frequency domain thermoreflectance. Nature Communications, 2013, 4: 1640
Koh Y K, Cahill D G. Frequency dependence of the thermal conductivity of semiconductor alloys. Physical Review B: Condensed Matter and Materials Physics, 2007, 76(7): 075207
Kucukgok B, Wu X, Wang X, Liu Z, Ferguson I T, Lu N. The structural properties of InGaN alloys and the interdependence on the thermoelectric behavior. AIP Advances, 2016, 6(2): 025305
Mingo N, Hauser D, Kobayashi N, Plissonnier M, Shakouri A. “Nanoparticle-in-Alloy” approach to efficient thermoelectrics: silicides in SiGe. Nano Letters, 2009, 9(2): 711–715
Koh Y K, Singer S L, Kim W, Zide J M O, Lu H, Cahill D G, Majumdar A, Gossard A C. Comparison of the 3ω method and timedomain thermoreflectance for measurements of the cross-plane thermal conductivity of epitaxial semiconductors. Journal of Applied Physics, 2009, 105(5): 054303
Jeżowski A, Danilchenko B, Boćkowski M, Grzegory I, Krukowski S, Suski T, Paszkiewicz T. Thermal conductivity of GaN crystals in 4.2–300K range. Solid State Communications, 2003, 128(2–3): 69–73
Jung K, Cho M, Zhou M. Strain dependence of thermal conductivity of [0001]-oriented GaN nanowires. Applied Physics Letters, 2011, 98(4): 041909
Hao Q, Zhao H, Xiao Y. Multi-length scale thermal simulations of GaN-on-SiC high electron mobility transistors. In: Zhang Y, He Y-L ed. Multiscale Thermal Transport in Energy Systems. Hauppauge. New York: Nova Science Publishers, 2016
Han Y J. Intrinsic thermal-resistive process of crystals: umklapp processes at low and high temperatures. Physical Review B: Condensed Matter and Materials Physics, 1996, 54(13): 8977–8980
Dubey K, Misho R. Three-phonon scattering relaxation rate and phonon conductivity. Application to Mg2Ge. Physica Status Solidi. B, Basic Research, 1977, 84(1): 69–81
Joshi Y, Verma G. Analysis of phonon conductivity: application to Si. Physical Review B: Condensed Matter and Materials Physics, 1970, 1(2): 750–755
Ohta H, Kim S, Mune Y, Mizoguchi T, Nomura K, Ohta S, Nomura T, Nakanishi Y, Ikuhara Y, Hirano M, Hosono H, Koumoto K. Giant thermoelectric Seebeck coefficient of a two-dimensional electron gas in SrTiO3. Nature Materials, 2007, 6(2): 129–134
Acknowledgements
This material is based on research sponsored by Defense Advanced Research Agency (DARPA) under agreement number FA8650-15-1-7523 and US Air Force Office of Scientific Research under award number FA9550-16-1-0025. The US Government is authorized to reproduce and distribute reprints for Governmental purposes notwithstanding any copyright notation thereon. The views and conclusions contained herein are those of the authors and should not be interpreted as necessarily representing the official policies or endorsements, either expressed or implied, of Air Force Research Laboratory (AFRL) and the DARPA or the US Government. X.W.W., J.Z., and X.J.W. would like to thank the supports from the National Science Foundation (NSF) through the University of Minnesota MRSEC under Award Number DMR-1420013 and from the Legislative-Citizen Commission on Minnesota Resources (LCCMR).
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Xu, D., Wang, Q., Wu, X. et al. Largely reduced cross-plane thermal conductivity of nanoporous In0.1Ga0.9N thin films directly grown by metal organic chemical vapor deposition. Front. Energy 12, 127–136 (2018). https://doi.org/10.1007/s11708-018-0519-5
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DOI: https://doi.org/10.1007/s11708-018-0519-5