Supplementary information L ħ T kB q s cqs qs nqs qs Dqs L V0 s D,s M s d m s pq x Lattice thermal conductivity Planck constant divided by 2 Temperature Boltzmann constant Wavevector Phonon polarization Group velocity Phonon frequency Bose-Einstein equilibrium phonon distribution function Total relaxation time Phonon density of states Effective diameter of the bulk sample Impurity scattering parameter Volume per atom Grüneisen parameter Debye temperature Atomic mass average Inverse of Knudsen number Film thickness. Bulk mean free path Wavevector dependent specularity parameter Integration variable The thermal conductivity simulation of free-standing membranes was carried out, first, by deriving the lattice thermal conductivity in Si bulk system using the modified Callaway model1,2 under the single mode relaxation time approximation. Then, once the thermal conductivity for bulk Si is determined, we introduced the effect of finite size through the so-called Fuchs-Sondheimer boundary corrections3,4. bulk 2 3k BT 2 c qs2 qs nqs (nqs 1)Dqs dq 2 qs (1) s film 3 1 pq 1 e x 3 5 1 (x x ) dx bulk 2 s 1 1 pq e x s s (2) where pq = exp(42q2) is the fraction of phonons that are specularly reflected by the boundaries5 and s = dms is the inverse of Knudsen number. The dispersion relation, qs, was determinate applying the approach suggested by Hopkins et al.6 and obtained an analytical form from a fourth-order polynomial fit to the experimental data for direction. Aq Bq 2 Cq3 Dq 4 , (3) with A, B, C and D constants determined via numerical fitting of experimental values. The total bulk, qs, relaxation time for each polarization, s, is limited by various scattering mechanisms such as: boundary B,qs, mass defect I,qs and Umklapp phonon-phonon interactions U,qs. This can be obtained via the Matthiessen rule as q,1s B1,qs I,1qs U1,qs , where the relaxation times B,qs, I,qs and U,qs are given by7–9 (4) B1,qs I,1qs U1,qs cqs L V 0 3 qs4 4cqs s2 qs2 exp D ,s /(3T ) 2 Mcqs D ,s (5) (6) (7) The parameters main used in the calculations are shown in table 1. L L T (K) (K) (mm) 2.01 Silicon 5.0 Table 1 Silicon parameters used in the calculations. Material L T Figure 1 (a) Phonon dispersion relation of bulk silicon: experimental results (red dots) from Ref.10 and fourth-order polynomial fit (black solid line). (b) Temperaturedependence of the lattice thermal conductivity: black solid line calculated temperaturedependence of the lattice thermal conductivity of bulk silicon. Red dots: the experimental data of silicon obtained from Ref.11 With the thermal conductivity determined we introduce the effect of the finite size using the equation 2. The surface roughness surface parameter, , was fixed in 0.5 nm taken from the estimated value in ref12 for Si membranes. References (1) Callaway, J. Physical Review 1959, 113, 1046–1051. (2) Holland, M. Physical Review 1963, 132, 2461–2471. (3) Fuchs, K. Mathematical Proceedings of the Cambridge Philosophical Society 1938, 34, 100–108. (4) Sondheimer, E. H. Advances in Physics 1952, 1, 1–42. (5) Ziman, J. M. Electrons and Phonons: The Theory of Transport Phenomena in Solids; Oxford University Press, USA, 1960. (6) Hopkins, P. E.; Rakich, P. T.; Olsson, R. H.; El-kady, I. F.; Phinney, L. M. Applied Physics Letters 2009, 95, 161902. (7) Klemens, P. G. Proceedings of the Physical Society. Section A 1955, 68, 1113–1128. (8) Slack, G.; Galginaitis, S. Physical Review 1964, 133, A253–A268. (9) Casimir, H. B. G. Physica 1938, 5, 495–500. (10) Group IV Elements, IV-IV and III-V Compounds. Part a - Lattice Properties; Madelung, O.; Rössler, U.; Schulz, M., Eds.; Springer-Verlag: Berlin/Heidelberg, 2001; Vol. a. (11) C. J. Glassbrenner and Glen A. Slack Phys. Rev. 1964, 134, 1058–1069. (12) Cuffe, J.; Ristow, O.; Chávez, E.; Shchepetov, A.; Chapuis, P.-O.; Alzina, F.; Hettich, M.; Prunnila, M.; Ahopelto, J.; Dekorsy, T.; Sotomayor Torres, C. M. Physical Review Letters 2013, 110, 095503.