Understanding Phonon Dynamics via 1D Atomic Chains

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1 Understanding Phonon Dynamics via 1D Atomic Chains Timothy S. Fisher Purdue University School of Mechanical Engineering, and Birck Nanotechnology Center Nanotechnology 501 Lecture Series 11 August 2006

2 Phonon Heat Conduction Phonons are quantized lattice vibrations Govern thermal properties in electrical insulators and semiconductors Can be modeled to first order with spring-mass dynamics spring constant g a atom, mass m Wave solutions ω wave vector K=2π/λ phonon energy=ħω dispersion relations gives ω = fn(k) optical branch acoustic branch sound speed (group velocity) K

3 Heat Conduction Through Thin Films Experimental results for 3-micron silicon films 3 micron Non-equilibrium scattering models work fairly well Crystalline structure has generally larger impact than film thickness Asheghi et al., 1999

4 Heat Conduction Through Multiple Thin Films Fine-pitch 5 nm superlattices 5nm Cross-thickness conductivity measurement Measured values are remarkably close to bulk alloy values (nearly within measurement error) Expected large reduction in conductivity not observed Cahill et al., 2003

5 Lattice Vibrations Consider two neighboring atoms that share a chemical bond The bond is not rigid, but rather like a spring with an energy relationship such as u r 0 r 0 r

6 Lattice Vibrations, cont d Near the minimum, the energy is well approximated by a parabola x = r r 0 u = and g = spring constant Now consider a one-dimensional chain of molecules spring constant g 1 2 gx atom, mass m 2 a

7 Lattice Energy and Motion Harmonic potential energy is the sum of potential energies over the lattice 1 harm U = g xna [ ] x[( n+ 1) a] 2 { } 2 Equation of motion of atom at location x(na) Simplified notation 2 d xn m = g 2 dt 2x x x n 2 harm d x( na) U F = m = = g x na x n a x n+ a 2 dt x( na) { 2 ( ) [( 1) ] [( 1) ]} { } n n 1 n+ 1

8 Lattice Motion, cont d Seek solutions of the form Boundary conditions Born-von Karman: assume that the ends of the chain are connected x N+1 = x 1 x 0 = x N ( ) n ()~exp { ω } x t i Kna t N 1 2

9 Lattice Motion, cont d Then the boundary conditions become 1 ( ) { } xn + 1 ~exp i K N + 1 a ωt [ ω ] [ ] { } x ~exp i Ka t 1= exp ikna KNa = 2 πn, where n is an integer Let λ be the vibration wavelength, λ = an/n 2πn 2π K = = an λ Minimum wavelength, λ min = 2a = 2(lattice spacing)

10 Solution to the Equations of Motion Substitute exponential solution into equation of motion 2 ω ika ika mω e = g 2 e e e = 2g( 1 coska) e Solve for ω ( ) ( ω ) ikna t ikna t ( ωt) ikna 2 g(1 cos Ka) g 1 ω ( K) = = 2 sin( 2 Ka) m m This is the dispersion relation for acoustic phonons relates phonon frequency (energy) to wave vector (wavelength)

11 Dispersion Curve Changing K by 2π/a leaves x unaffected Only N values of K are unique We take them to lie in -π/a < K < π/a ω(k) 2(g/m) 1/2 - π/a π/a K

12 Phase velocity: Wave Velocities c = ω/k Group velocity: v g = ω/ K = a(g/m) 1/2 cos(ka/2) For small K: g lim ω= a K m K 0 g ω lim vg = a = = c m K K 0 Thus, for small K (large λ), group velocity equals phase velocity (and speed of sound) We call these acoustic vibration modes

13 Notes on Lattice Vibrations For K = ±π/a, the group velocity is zero why? xn + 1 exp { ika} exp { i } cos i x = = π = π+ sin π= 1 n neighbors are 180 deg out of phase The region -π/a < K < π/a is the first Brillouin zone of the 1D lattice We must extrapolate these results to three dimensions for bulk crystals

14 Density of Phonon States (Kittel, Ch5) Consider a 1D chain of total length L carrying M+1 particles (atoms) at a separation a Fix the position of atoms 0 and M Each normal vibrational mode of polarization p takes the form of a standing wave x ~sin( nka)exp( ω i t) n Only certain wavelengths (wavevectors) are allowed λ max =2L (K min =π/l), λ min =2a (K max =π/a=mπ/l) In general, the allowed values of K are π 2π 3 π ( M 1) π K =,,,..., L L L L L Kp Note: K=Mπ/L is not included because it implies no atomic motion, i.e., sin(nmπa/l)=sin(nπ)= M-1 M a

15 Density of States, cont d Thus, we have M-1 allowed, independent values of K This is the same number of particles allowed to move In K-space, we thus have M-1 allowable wavevectors Each wavevector describes a single mode, and one mode exists in each distance π/l of K-space Thus, dk/dn = π/l, where N is the number of modes Discrete K-space representation π/a π/(m-1)a π/l π/a

16 Density of States, cont d The phonon density of states gives the number of modes per unit frequency per unit volume of real space 1 dn 1dN dk 1 1 D( ω ) = = = 1 dω L dk dω π dω/ dk L α= The last denominator is simply the group velocity, derived from the dispersion relation 1 1 g 1 D( ω ) = = πa cos K( ω) a πvg ( ω) m 2 Note singularity for K =π/ a

17 Periodic Boundary Conditions For more generality, apply periodic boundary conditions to the chain and find K 2π 4π 0,,,..., M π = ± ± L L L Still gives same number of modes (one per particle that is allowed to move) as previous case, but now the allowed wavevectors are separated by ΔK = 2π/L Useful in the study of higher-dimension systems (2D and 3D)

18 2D Density of States Each allowable wavevector (mode) occupies a region of area (2π/L) 2 Thus, within the circle of radius K, approximately N=πK 2 / (2π/L) 2 allowed wavevectors exist Density of states 2 L α= K-space K π/a 2π/L 1 dn 1 dn dk K( ω) 1 D( ω ) = = = dω V dk dω 2 π v ( ω) g

19 3D Density of States Using periodic boundary conditions in 3D, there is one allowed value of K per (2π/L) 3 volume of K- space The total number of modes with wavevectors of magnitude less than a given K is thus 3 3 L 4 3 VK N = π K = 2π 3 2 6π The 3D density of states becomes 1 dn 1 dn dk K( ω) 1 D( ω ) = 3 2 L α= = = dω V dk dω 2π vg ( ω ) 2

20 Overview of Phonon Simulation Tools Boltzmann Transport Equation (BTE) Requires boundary scattering models Requires detailed understanding of phonon scattering and dispersion for rigorous inclusion of phonon physics Molecular Dynamics (MD) Computationally expensive Not strictly applicable at low temperatures Handling of boundaries requires great care for links to larger scales and simulation of functional transport processes Atomistic Green s Function (AGF) Efficient handling of boundary and interface scattering Straightforward links to larger scales Inclusion of anharmonic effects is difficult

21 Atomistic Green s Function (AGF) Modeling of Phonon Transport Based on Zhang et al. The Atomistic Green s Function Method: An Efficient Simulation Approach for Nanoscale Phonon Transport, Num Heat Trans-B, in review.

22 Some Background Non-equilibrium Green s function method initially developed to simulate electron ballistic transport (see Datta, 1995) Very efficient in the ballistic regime but requires significant effort to implement scattering Recently applied to phonon transport (see Mingo, 2003; Zhang et al., in press)

Includes effects of bulk contacts through self-energy matrices Suitable for ballistic transport Nanoscale devices at room temperature, or Low-temperature conditions,

23 Includes effects of bulk contacts through self-energy matrices Suitable for ballistic transport Nanoscale devices at room temperature, or Low-temperature conditions, or Scattering dominated by boundaries and interfaces Required inputs Atomistic Green s Function Equilibrium atomic positions Inter-atomic potentials Contact temperatures

24 Recall Lattice Dynamics Equation of motion for a 1D atomic chain 2 d xn m = g{ 2x } 2 n xn 1 xn+ 1 dt Plane wave assumption x t i Kna t ()~exp { ( )} n ω Combine 2 g ω x { } n = 2xn xn 1 xn+ 1 m Re-arrange and write in matrix form 2 ω I H x= 0 I is the identity matrix

25 Harmonic Matrix Define the k matrix as k ij 2 U = x x k = 2g nn nn, + 1 nn, 1 i harm k = k = g j Here, g is the spring constant Then, define the harmonic matrix H as H = k ij 1 M M i j ij, no index summation

26 Harmonic Matrix H 2 f f = f 2 f f f 2 f f is spring constant divided by atomic mass 1. H is not the same dynamical matrix used to determine dispersion curve (that matrix is the Fourier transform of H). 2. H is symmetric. 3. Sum of all elements in any row or sum of all elements in any column is zero, except in the first and last row/column.

27 Green s Functions In general, systems of equations can be written in operator form 2 Lx [ ] I H x 0 = ω = Green s functions are often used in such situations to determine general solutions of (usually) linear operators

28 Green s Functions, cont d The Green s function g is the solution that results from the addition of a perturbation to the problem L[g] = δ In the present (matrix) problem, the unperturbed Green s function becomes ( 2 i) g= ω +δ I H Where δ is called the broadening constant, and i is the unitary imaginary number 1

29 Toward Realistic Problems So far, we have not made much progress in solving real problems To solve most practical problems, we need to incorporate different materials and interfaces Device Thermal Reservoir 1 T1 T2 Thermal Reservoir 2

30 Why Green s Functions? We can model connections among different materials through the use of a different Green s function G 1 2 T T G = ω I H d τ { 1g1τ1 τ2g2τ2 Σ1 Σ superscript T = conjugate transpose This matrix function includes self-energy matrices (Σ 1, Σ 2 ) that involve unperturbed Green s functions (g s) associated with contacts (i.e., boundaries) in a transport problem τ matrices handle connections between different system elements (materials, interfaces) The full derivation is beyond the scope of this presentation, so we will simply use the results for computational purposes Very efficient in the ballistic regime but requires significant effort to implement scattering

31 Phonon Transport through a Device between Two Contacts Reservior 1 Reservoir 2 Device Transmission function, Ξ Hot T 1 Cold T 2

32 1D Atomic Chain Can be visualized as an atomic chain between two isothermal contacts (Note: contacts are still atomic chains in this example)

33 Transmission and Heat Flux ω J = h ΔN( ω) Ξ( ω) dω 2π 0 Phonon energy Phonon occupation difference B hω / kt B + hω e Δ N = N N ΔT 2 2 k T ( hω / kt e 1) (units = W) Transmission We need to evaluate transmission in order to calculate heat flux B

34 Transmission and Green s Functions Some definitions of convenience A = i g g Γ T j j j =τ A τ T j j j j The transmission function T T Ξω ( ) = Trace Γ 1GΓ2G = Trace Γ 2GΓ1G

35 The AGF Algorithm Establish atomic positions and potential parameters U and x i Assemble harmonic matrices (H) Calculate the Green s function (g) of uncoupled contacts Uses decimation algorithm Calculate device G and phonon transmission (Ξ) Integrate (Ξ) over phonon frequencies and k to obtain the thermal conductance

36 Results for Simple Atomic Chains heavy device light device Homogeneous chain density of states Homogeneous vs heterogeneous

37 Strained Silicon PMOS T. Ghani, et al. at IEDM 2003 NMOS 25 % drive current increase in PMOS; 10 % drive current increase in NMOS

38 Thin Films Transport along the (100) direction (i.e., the z direction)

39 Convert Ge/Si/Ge Model/Code Validation 1976 Ge Si Ge to Ge/Si/Si Ge Si Si to create a single interface. Zhang et al., J. Heat Trans. in review AMM is known to work well at low temperatures

40 Thermal Conductance Conductance reduced by 30 to 50% at room temperatures due to heterogeneous interfaces At low temperatures, conductance converges to that of the bulk contacts Convergence of conductance Reduction of conductance

41 Multilayer Effects Ge Si Ge Replace the Si device with a multi-layer structure Ge Ge Asymptotic behavior is similar to that of radiation shields

42 Conclusions The AGF method is an effective tool in simulating ballistic phonon transport through relevant interfaces involving bulk and nanoscale materials Strain effects are small compared to heterogeneousmaterial effects A heterogeneous device layer reduces thermal conductance significantly at room temperature Increasing film thickness decreases thermal conductance The first few heterogeneous interfaces are most responsible for decreasing thermal conductance

Ongoing Work Numerical construction of harmonic matrices (H) Enables the use of more complicated atomic configurations as well as advanced interatomic potentials Implemented with EDIP potentials and

43 Ongoing Work Numerical construction of harmonic matrices (H) Enables the use of more complicated atomic configurations as well as advanced interatomic potentials Implemented with EDIP potentials and benchmarked against bulk silicon dispersion curves Phonon transport through a nanowire and bulk contacts The size mismatch between a nanowire and its bulk contact limits heat flow (100) nanowire is being benchmarked

44 Acknowledgements Wei Zhang, PhD (August 2006) Dr. Natalio Mingo, NASA AMES Funding from the Purdue NASA Institute of Nanoelectronics and Computing

45 References Cahill et al., Journal of Applied Physics 93, 793 (2003) Mingo, Physical Review B 68, (2003) Cheeke, Canadian Journal of Physics 54, 1749 (1976) C. Kittel, Introduction to Solid State Physics, Wiley, Zhang et al. The Atomistic Green s Function Method: An Efficient Simulation Approach for Nanoscale Phonon Transport, Num Heat Trans-B, in review. S. Datta, Electronic Transport in Mesoscopic Systems. Cambridge University Press, 1st ed., Zhang et al., Simulation of Phonon Interfacial Transport in Strained Si-Ge Heterostructures, J Heat Transfer, in press.

46 Classes ME 597F: Micro and Nanoscale Energy Transfer Processes ME 595M: Computational Nanoscale Heat Transfer (with J. Murthy)

Atomistic Green s Function Method: Density of States and Multi-dimensionality

Atomistic Green s Function Method: Density of States and Multi-dimensionality Timothy S. Fisher Purdue University School of Mechanical Engineering, and Birck Nanotechnology Center tsfisher@purdue.edu Based