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Copyright © 2011 American Scientific Publishers All rights reserved Printed in the United States of America Journal of Nanoscience and Nanotechnology Vol. 11, 9984–9988, 2011 Hot Electrons and Electron-Phonon Coupling in a Cylindrical Nanoshell Shi-Xian Qu1 ∗ , Ya-Ni Zhao1 , Lin Zhang1 , and Michael R. Geller2 1 Institute of Theoretical and Computational Physics, School of Physics and Information Technology, Shaanxi Normal University, Xi’an 710062, China 2 Department of Physics and Astronomy, University of Georgia, Athens, Georgia 30602-2451, USA We use a standard model for the low-temperature electron-phonon interaction in metals to calculate the rate of thermal energy transfer between electrons and acoustic phonons in suspended metallic nanoshells. The electrons are treated as three-dimensional and noninteracting, whereas the vibrational modes are that of an thin cylindrical elastic shell of radius R with a free surface and Delivered by Ingenta to: thickness h. Disorder is neglected. The temperature dependence of the thermal power is obtained Michael Geller analytically for this model, and a crossover from the T 3 dependence expected for one-dimensional 3 2 4 ∗ IP : 72.194.211.160 2 3/2 phonons to a T /1 − + 9T /T 1 − dependence is obtained. Sun, 06 Jan 2013 22:09:24 Keywords: Hot Electrons, Nanoshell. RESEARCH ARTICLE 1. INTRODUCTION The development of modern nanofabrication techniques and low-temperature measurement technology enable us to explore the mechanical properties of condensed matter at the nanoscale.1 In particular, the phonon thermal conductance at low temperature has been of considerable interest.1–5 In addition to its significance for investigating fundamental phonon physics and macroscopic quantum phenomena, it may find applications in nanoscale bolometers and calorimeters with unprecedented sensitivity,3, 6, 7 and even in quantum information processing.8–10 It is known that the conduction electrons in a metal at low temperature are only weakly coupled to the lattice phonons.11, 12 Therefore, the electron–electron scattering will cause electrons to equilibrate on a timescale that is typically much shorter than the electron-phonon relaxation time, resulting in an electron distribution that is thermal, but at a temperature higher than that of the lattice. Understanding this hot-electron effect is crucial in studies of transport in semiconductors and metals at low temperatures.13 The electron-phonon scattering rate in conductors has been studied both theoretically14–16 and experimentally,16, 17 with good agreement between theory and experiment. The theoretical work has focused on the rate of energy transfer between electrons and acoustic phonons in an infinite bulk metal. The weak coupling between electrons and phonons ∗ Author to whom correspondence should be addressed. 9984 J. Nanosci. Nanotechnol. 2011, Vol. 11, No. 11 allows separate temperatures Tel and Tph to be defined for the electron and phonon subsystems, and at low temperatures significant differences in these temperatures are easily achieved. Assuming a deformation-potential coupling, theory predicts that the rate of energy exchange P from the electrons to the phonons is given by16 (1) P = V Teln − Tphn where n = 5 for bulk electrons and phonons, V is the volume of the system, and is a material parameter given by 8 5 kB5 F2 Nel F (2) = 3 4 vF vl4 Here n is the Riemann zeta function, F is the Fermi energy, Nel is the electronic density of states (DOS) per unit volume, is the mass density, vl is the bulk longitudinal sound speed, and vF is the Fermi velocity. Most of the experiments to date, however, have been performed on thin metal films deposited on semiconducting substrates, whereas the theory has assumed bulk metals. The metal films typically have a thickness d of the order of ten to several hundred nanometers, with lateral dimensions of a few microns. Although the electrons in the films are three dimensional (i.e., the Fermi wavelength being much smaller than any of the physical dimensions), the phonons at low temperatures will have wavelengths larger than d. Therefore, one expects similar temperature dependence of the thermal power described by Eq. (1), but with different pre-factors and 1533-4880/2011/11/9984/005 doi:10.1166/jnn.2011.5301 Qu et al. Hot Electrons and Electron-Phonon Coupling in a Cylindrical Nanoshell field equations, exponents n ranging from n = 3 to 6.11, 12, 18, 19 In addi normalized over the phonon volume Vph tion, there is a growing interest in the low-temperature according to V d 3 r fn∗ · fn = nn . It will be convenient to properties of electrons and phonons in mechanically susrewrite the electron-phonon interaction as pended nanostructures,2, 4, 6, 7, 21–25 where the phonon spec † ∗ † H = gnq ck+q ck an + gnq ck−q ck a†n (7) trum is strongly modified from that in a bulk metal. kqn Experiments have found that the reduction of phonon dimensionality leads to a weak temperature dependence with coupling constant (smaller exponent) of the heat flux between electrons 2 and phonons.11, 18, 22, 23 In many cases the power exhibgnq ≡ F 2n −1/2 V −1 d 3 r · fn e−iq·r (8) D+2 ited a P ∼T temperature dependence, where D is 3 V the phonon dimensionality. The T 3 dependence of the The quantity we calculate is the thermal energy per unit heat flux obtained for suspended one-dimensional metallic time transferred from the electrons to the phonons, nanowires in Ref. [26] also supports the above conjecture. It stimulates us to investigate the hot-electron effect in a P ≡ 2 n nem k → k − q − nab k → k + q geometry of cylindrical nanoshell. kqn In the current work, we will propose a general expres(9) sion for calculating the thermal power transferring from 3-dimensional electron to any D-dimensional phonon subwhere system firstly, and then apply it to a prototype with geomeDelivered to: try of cylindrical nanoshell which approximates a metallic by Ingenta nem k → k − q = 2 gnq 2 nB n + 1nF k Michael Geller system with no band gap. IP : 72.194.211.160 × 1 − nF k−q k−q − k + n Sun, 06 Jan 2013 22:09:24 2. GENERAL EXPRESSION FOR THE THERMAL POWER k n where ck† and ck are electron creation and annihilation operators, with k the momentum, and a†n and an are bosonic phonon creation and annihilation operators. The vibrational modes, labeled by an index n, are eigenfunctions of the continuum elasticity equation vt2 × × u − vl2 · u = 2 u (4) for linear isotropic media, along with accompanying boundary conditions. vt and vl are the bulk transverse and longitudinal sound velocities. The electron-phonon interaction H is described by the deformation potential 2 H ≡ F d 3 r † · u (5) 3 V with ur = 2n −1/2 fn ran + fn∗ ra†n (6) n the quantized displacement field. The vibrational eigenfunctions fn r are defined to be solutions of the elasticity J. Nanosci. Nanotechnol. 11, 9984–9988, 2011 is the golden-rule rate for an electron of momentum k scattering to k − q while emitting a phonon n, and nab k → k + q = 2gnq 2 nB n nF k × 1 − nF k+q k+q − k − n (11) is the corresponding phonon absorption rate. nB is the Bose distribution function with temperature Tph and nF is the Fermi distribution with temperature Tel . The factor of 2 in Eq. (9) accounts for spin degeneracy. Before integrating Eq. (9) to obtain the exact expression for P , we have to make a statement on the phonon wave vector q and the dimensionality (denoted by D) felt by phonons according to different thermal wavelength thermal = hvl /kB Tph at phonon temperature Tph and model velocity vl . The wave vector q is a 3-dimensional vector and thus D = 3 when thermal is much less than the dimension in any one of the three directions. It becomes a 2-dimensional vector and D = 2 if thermal is larger than the dimension in any one direction, but an 1-dimensional vector and D = 1 if thermal is larger than the dimensions in any two directions. The integrations of Eq. (9) by considering three cases gives a general expression of P for a metallic system consisting of a three-dimensional electron gas and a any Ddimensional phonon subsystem. The result (suppressing factors of and kB ) is m2 V ph P = d−n /T − /Tph e el −1 e −1 n 0 9985 RESEARCH ARTICLE In Ref. [27], two of the authors have advanced a general method for calculating the rate of thermal energy (thermal power) transfer based upon a kind of weighted DOS. There, we consider the hot electron effect in a system consisting of a three-dimensional electron gas and a threedimensional solid. The volume of the system is V and the Hamiltonian reads H = k ck† ck + n a†n an + H (3) (10) Qu et al. Hot Electrons and Electron-Phonon Coupling in a Cylindrical Nanoshell RESEARCH ARTICLE d D k g 2 nk × +Tel ln 2D k 1+expm2 /2k2 +k2 /8m−/2−/Tel × 1+expm2 /2k2 +k2 /8m+/2−/Tel 3. HOT-ELECTRONS IN A CYLINDRICAL NANOSHELL In this section we consider a cylindrical metallic nanoshell in which the external pressure on the inner surfaces is equal to that on the outer surfaces, and the trans(12) verse dimensions are far smaller than the length in the z-direction, and the inner radius is R and the thickness where, ph is the volume felt by phonons, which is not is h. Disorder is neglected. For convenience, we may, in necessarily equals to the system volume V . The logasome extend, assume that there is no band gap in the rithmic term in P can be shown to be negligible in the system. At the low temperature range we are interested, temperature regime of interest and will be dropped. the thermal wave length of electrons is far smaller than The DOS weighted form of P (suppressing factors of the length and the thickness of the cylinder, and thus and kB ) reads electrons move 3-dimensionally. While the thermal wave length of phonons is very smaller than the length but larger 2 2 D 2m F ph than the thickness. Therefore, one may reasonably assume dF /T − P= 9 e el − 1 e/Tph − 1 0 thin cylinder for the phonon counterpart. There has been (13) extensively study on the property of acoustic phonons in where D is the Debye frequency, and F is a strainthin cylindrical shells.29–32 The thin cylindrical elastic shell weighted vibrational DOS, defined by might beto: used as a model for the in-plane vibrations in Delivered by Ingenta 33 In our calculations, we employ the result of nanotubes. Michael F ≡ Un − n (14) Geller Ref. [29], in which the eigenfunction reads, IP : 72.194.211.160 n ⎞ ⎛ Sun, 06 Jan 2013 22:09:24 −iCr with (19) fr = ⎝ C ⎠ exp im + iqz z C z 1 d 3 rd 3 r · fn r · fn∗ r Un ≡ where is the azimuth angular, qz ≡ q/R is the wavevecV V tor in the z-direction. Cr C and Cz are respectively the dD k −1 −ik·r−r × k e (15) normalization constants in three orthogonal directions. The 2D eigenmodes are given by Here Un can be interpreted as an energy associated with mass-density fluctuations interacting via an potential determined by the last integration in Eq. (15). To this end we have reduced the calculation of P to the calculation of F . Allen28 has derived a related weighted-DOS formalism. For the conventional hot-electron effect in bulk materials,16 one deals with 3-dimensional phonon subsystem and ph = V . Carrying out the last integration in Eq. (15) gives Un = 1 3 3 · fn r · fn∗ r d rd r 2 2 V V r − r 2 (16) where the longitudinal acoustic phonon eigenfunction with momentum k is eiq · r (17) fk = √ ek V Substituting this eigenfunction into Eq. (16) and carrying out the integration, we obtain the weighted DOS F = 1 3 2 2 vl4 (18) The conventional expression for the net rate of energy relaxation in Eq. (1) and the corresponding coefficient in Eq. (2) can be easily reduced by this DOS. 9986 (20) Im q c q 2 + m2 + 1 IIm q c − q 2 + m2 (21) √ q 1 − 2 III (22) m=0 q c 1+q √ q2 1 − 2 III m q c √ (23) m m2 + 1 + q 2 Here c ≡ vl /R is the cutoff frequency for the mode with frequency I0 , q is the dimensionless wavevector, m is the branch index, − = 1 − /2, is the Poisson ratio, and vl = E/1 − 2 is the longitudinal sound velocity (E is Young’s modulus). In the axisymmetric case with m = 0 the I, II and III modes correspond to pure radial, torsional, and longitudinal modes respectively. They correspond to pure longitudinal modes, torsional, and radial respectively in the large q limitation. Simply calculation via Eq. (8) reveals that only the axisymmetric modes with I0 and III 0 contribute to the electron-phonon interaction. The corresponding dispersion relations are (24) I0 q = c q 2 + 1 √ q 1 − 2 (25) III 0 q = c q +1 J. Nanosci. Nanotechnol. 11, 9984–9988, 2011 Qu et al. Hot Electrons and Electron-Phonon Coupling in a Cylindrical Nanoshell Here one may find that the minimum of I0 is always bigger than the maximum of III 0 . The normalization constants for the first mode are respectively Cr = iA1 , C = 0 and Cz = qA1 with A1 ≡ V 2 + q 2 −1/2 . Those for the second mode are Cr = −iqA2 , C = 0 and Cz = A2 1 + 2q + 2 q 2 /1 + q2 with A2 ≡ 1 + q2 V 2 q 2 1 + q4 + 1 + 2q + 2 q 2 2 −1/2 . Obviously, phonons in this subsystem move quasi-one dimensionally and thus we have ph = L with L the length of the cylindrical nanoshell. Employing identity −1 −ikz−z dk k e = isignz − z, Eq. (15) gives − Uqmz ≡ i 3 3 d rd r · fn r · fn∗ r signz − z 2V V The strain-weighted DOS has distinct high- and lowfrequency character crossing over at = c because F1 has a cut off at this frequency. Clearly, c defines a nature crossover temperature T ≡ c kB (32) distinguishing the high and low temperature behaviors. At high temperature where T > T , F1 dominates the contribution, and the large frequency asymptotic behavior of strain-weighted DOS reads F = F1 2vl2 (26) leading to the high-temperature expression of thermal power where the superscript m = 1 or 2 distinguishes two vibra tional modes associated with the two dispersion rela(33) P = 1D L 3 D /Tel Tel3 − 3 D /Tph Tph3 tions defined in Eqs. (24) and (25), respectively. The Delivered by Ingenta to: strain-weighted vibration DOS is here 1D is the material parameter defined by F = F1 + F2 with Fm defined by Fm ≡ Uqmz − 1 qz Michael Geller (27) IP : 72.194.211.160 Sun, 06 Jan 2013 22:09:24 qz = V (28) Here, F1 is valid in the range confined by ≥ c . Carrying out the integrations over r, r , and q, we obatin 1 − 2 /2c (29) F1 = 2vl2 1 − 2 − 2 /2c and F2 = 2vl2 √ 1 − 2 √ 1 − 2 − /c 2 1 − 2 /2c × √ 2 2 /2c + 1 − 2 /2c 2 1 − 2 − /c 2 (30) Then the thermal power can be calculated by the following formula, 2m2 F2 L D dF1 /T − P = 9 e el − 1 e/Tph − 1 c D + − /Tph dF2 /T e el − 1 e −1 0 (31) J. Nanosci. Nanotechnol. 11, 9984–9988, 2011 The T 3 law for the thermal power for cylindrical nanoshells revealed by this relation is the same to that in one dimensional phonon systems where electron cooling devices are manipulated.23, 26 The crossover from the T 5 law in three-dimensional phonon systems to the T 3 law in their one-dimensional counterparts shows that the electron-phonon interaction changes very significantly when dimensionality of the phonon subsystem reduces, which agrees with the effect of phonon dimensionality on the electron-phonon coupling observed by other researches.11, 19, 23, 26 At low-temperature when T < T , the dominant contributions to the thermal power are due to the small frequency asymptotical behavior of F , which are ≥ c 2vl2 1 3 + F2 2vl2 1 − 2 c 1 − 2 3/2 F1 Combining these two expressions with Eq. (31), we get the low-temperature expression of the thermal power P = 1D L Tel Tel3 − Tph Tph3 + 1D L Tel Tel4 − Tph Tph4 (36) 9987 RESEARCH ARTICLE iL dq − m q 4RV − × d 3 rd 3 r · fn r · fn∗ r signz − z 3kB3 kF4 (34) 18 2 vl2 y and m y ≡ m − 1!m−1 0 dx xm−1 /ex − 1. It can be shown that the 3 factors are equal to unity at temperatures above T but sufficiently smaller than the Debye temperature. Thus, expression (33) reduces to (35) P = 1D L Tel3 − Tph3 1D = Qu et al. Hot Electrons and Electron-Phonon Coupling in a Cylindrical Nanoshell where 23 D /T − 3 c /T 1 − 2 9 T ≡ /T T 1 − 2 3/2 4 D 108118) and by the U. S. National Science Foundation under grant CMS-0404031. T ≡ References and Notes 1. A. N. Cleland, Foundamentals of Nanomechanicss, Spinger-Verlag, Berlin (2002). 2. K. Schwab, E. A. Henriksen, J. M. Worlock, and M. L. Roukes, Nature (London) 404, 974 (2000). At extremely low temperature, i.e., T T , D /T 1, 3. M. L. Roukes, Physica B 263, 1 (1999). and thus 3 and 4 factors tend to unity. Therefore, we 4. A. N. Cleland, D. R. Schmidt, and C. S. Yung, Phys. Rev. B have T = 1/1 − 2 and T = 9/T 1 − 2 3/2 , 64, 172301 (2001). 5. M. Blencowe, Phys. Rep. 395, 159 (2004); Science 304, 56 (2004). and hence expression (36) reduces to 6. C. S. Yung, D. R. Schmidt, and A. N. Cleland, Appl. Phys. Lett. 81, 31 (2002). Tel3 − Tph3 9 Tel4 − Tph4 (37) + P = 1D L 7. D. R. Schmidt, C. S. Yung, and A. N. Cleland, Phys. Rev. B 2 2 3/2 1− T 1 − 69, 140301(R) (2004). 8. A. D. Armour, M. P. Blencowe, and K. C. Schwab, Phys. Rev. Lett. which reveals a crossover of the T 3 law for the temperature 88, 148301 (2002). 9. A. N. Cleland and M. R. Geller, Phys. Rev. Lett. 93, 070501 (2004). dependence of the thermal power at low temperature. 10. X. Zou and W. Mathis, Phys. Lett. A 324, 484 (2004). In order to get some sense on the order of the 11. J. T. Karvonen Delivered to: and I. J. Maasilta, Phys. Rev. Lett. 99, 145503 (2007). characteristic quantities, we take the corresponding mate-by Ingenta 12. J. T. Karvonen and I. J. Maasilta, J. Phys.: Conference Series rial parameters from those of a thin-walled hollowMichael cylin- Geller 92, 012043 (2007). IP : 72.194.211.160 ratio der of metallic carbon.31, 34, 35 They are the Poisson 13. P. Y. Yu and M. Cardona, Fundamentals of Semiconductors: Physics Sun,the 06mass Jan 2013 22:09:24 and Materials Properties, Springer-Verlag, Berlin (1999). = 0186, the Young’s modulus E = 1050 Gpa, 14. W. A. Little, Can. J. Phys. 37, 334 (1959). density = 226 g/cm3 , and the Fermi energy F = 10 eV. 15. V. F. Gantmakher, Rep. Prog. Phys. 37, 317 (1974). The calculated longitudinal sound velocity is vl = 219 × 16. F. C. Wellstood, C. Urbina, and John Clarke, Phys. Rev. B 49, 5942 4 −10 −1 −3 Wm K , 10 m/s, the parameter 1D = 108 × 10 (1994). and the crossover temperature T = 246 K which is in the 17. M. L. Roukes, M. R. Freeman, R. S. Germain, R. C. Richardson, and M. B. Ketchen, Phys. Rev. Lett. 55, 422 (1985). temperature zone that the current technology can achieve. 18. J. F. DiTusa, K. Lin, M. Park, M. S. Isaacson, and J. M. Parpia, Hence we expect the experimental observation of this Phys. Rev. Lett. 68, 1156 (1992). crossover phenomenon. 19. A. Vinante, P. Falferi, R. Mezzena, and M. Mück, Phys. Rev. B 75, 104303 (2007). 20. P. M. Echternach, M. R. Thoman, C. M. Gould, and H. M. Bozler, 4. CONCLUSION Phys. Rev. B 46, 10339 (1992). 21. M. C. Cross and R. Lifshitz, Phys. Rev. B 64, 085324 (2001). We have advanced a general expression for calculating 22. L. J. Taskinen and I. J. Maasilta, Appl. Phys. Lett. 89, 143511 (2006). the thermal power transferring from 3-dimensional elec23. J. T. Muhonen, A. O. Niskanen, M. Meschke, Yu. A. Pashkin, J. S. tron to any D-dimensional acoustic phonon subsystem. Tsai, L. Sainiemi, S. Franssila, and J. P. Pekola, Appl. Phys. Lett. 94, 073101 (2009). It transfers the calculation of thermal power to the com24. B. Huard, H. Pothier, D. Esteve, and K. E. Nagaev, Phys. Rev. B putation of the strain-weighted DOS for phonon sub76, 165426 (2007). systems of any dimensionality. Employing this method, 25. A. Gusso and L. G. C. Rego, Phys. Rev. B 75, 045320 (2007). we have investigated the hot-electron effect in free sus26. F. W. J. Hekking, A. O. Niskanen, and J. P. Pekola, Phys. Rev. B pended cylindrical nanoshells, in which electrons behave 77, 033401 (2008). 27. S.-X. Qu, A. N. Cleland, and M. R. Geller, Phys. Rev. B 72, 224301 three-dimensionally but phonons are confined to quasi-one (2005). dimension. The temperature dependence of the thermal 28. P. B. Allen, Phys. Rev. Lett. 59, 1460 (1987). power is obtained analytically, and the low-temperature 29. M. A. Stroscio and M. Dutta, Phonons in Nanostructures, Cambridge crossover from the T 3 to T 3 /1 − 2 + 9T 4 /T ∗ 1 − University Press, Cambridge (2001). 2 3/2 dependence is also deduced. The result shows that 30. Y. M. Sirenko, M. A. Stroscio, and K. W. Kim, Phys. Rev. E 53, 1003 (1996). reduction of phonon dimensionality leads to weak tem31. G. D. Mahan, Phys. Rev. B 65, 235402 (2002). perature dependence (smaller exponent) of the heat flux 32. Y. M. Sirenko, M. A. Stroscio, and K. W. Kim, Phys. Rev. E 54, 1816 between electrons and acoustic phonons. (1996). 33. H. Suzuura and T. Ando, Phys. Rev. B 65, 235412 (2002). Acknowledgments: This work was supported by the 34. M. F. Lin and K. W.-K. Shung, Phys. Rev. B 47, 6617 (1993). 35. F. Liu, P. B. Ming, and J. Li, Phys. Rev. B 76, 064120 (2007). Key Project of Chinese Ministry of Education. (No. RESEARCH ARTICLE ≡ 4/3 Received: 18 December 2010. Accepted: 19 May 2011. 9988 J. Nanosci. Nanotechnol. 11, 9984–9988, 2011