© Copyright National University of Singapore. All Rights Reserved. ENHANCING THERMOELECTRIC EFFICIENCY FOR NANOSTRUCTURES AND QUANTUM DOTS Jian-Sheng Wang.

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© Copyright National University of Singapore. All Rights Reserved. ENHANCING THERMOELECTRIC EFFICIENCY FOR NANOSTRUCTURES AND QUANTUM DOTS Jian-Sheng Wang Department of Physics, National University of Singapore

© Copyright National University of Singapore. All Rights Reserved. OUTLINE Seebeck effect & thermoelectric efficiency Disordered graphene/graphane Quantum master equation: electron-phonon interaction to thermoelectric efficiency in quantum dots Enhancing thermoelectric efficiency by time- dependent driven Conclusion 1 ST CONFERENCE ON CONDENSED MATTER PHYSICS, JULY

© Copyright National University of Singapore. All Rights Reserved. SEEBECK EFFECT Seebeck coefficient: how much voltage difference can one generate per temperature difference? S =  dV/dT How efficient is it comparing to Carnot engine, W/Q = 1 – T c /T h ? Ans: Determined by a material parameter called ZT = S 2  T/  : electric conductivity, : thermal conductivity, T: absolute temperature From “Physics Today,” June 2014, p.14 3

© Copyright National University of Singapore. All Rights Reserved. ENHANCING ZT BY DISORDERING Ni, Liang, Wang & Li, Appl. Phys. Lett. 95, (2009). ZT at 300K for graphene/graphane calculated using ballistic NEGF formulation for the armchair ribbons with fraction of H- bond disorder, with DFT structure determination. graphane graphene 4

© Copyright National University of Singapore. All Rights Reserved. QUANTUM DOT ELECTRON-PHONON INTERACTION 5

© Copyright National University of Singapore. All Rights Reserved. QUANTUM MASTER EQUATION APPROACH Advantage of NEGF: any strength of system- bath coupling V; disadvantage: difficult to deal with nonlinear systems. QME: advantage - center can be any form of Hamiltonian, in particular, nonlinear systems; disadvantage: weak system-bath coupling, small system. Can we improve? WANG, ET AL, FRONT. PHYS. 9, 673 (2014); THINGNA, ET AL, J. CHEM. PHYS. (2014) 6

© Copyright National University of Singapore. All Rights Reserved. DYSON EXPANSIONS 7

© Copyright National University of Singapore. All Rights Reserved. DIVERGENCE 8

© Copyright National University of Singapore. All Rights Reserved. UNIQUE ONE-TO-ONE MAP,  0 ↔  ; ORDERED CUMULANTS 9

© Copyright National University of Singapore. All Rights Reserved. ORDER-BY-ORDER SOLUTION 10

© Copyright National University of Singapore. All Rights Reserved. TIME-DEPENDENT DRIVEN Nonequilibrium Green’s function (NEGF), we use Jauho, Wingreen, Meir (PRB 1994) theory Master equation case - drive change the eigenvalues but not eigenvectors, easily generalize 11

© Copyright National University of Singapore. All Rights Reserved. ELECTRON CURRENT ZHOU, ET AL, PHYS REV B 90, (2015). 12

© Copyright National University of Singapore. All Rights Reserved. REDUCTION OF ZT UNDER ELECTRON- PHONON INTERACTION 13

© Copyright National University of Singapore. All Rights Reserved. WHY DRIVE THE SYSTEM? CAN HAVE HIGHER EFFICIENCY Far from thermal equilibrium Break down of Onsager relation (due to break down of time translational invariance) 14

© Copyright National University of Singapore. All Rights Reserved. HOW TO QUANTIFY EFFICIENCY IN TIME- DEPENDENT SITUATION? 15  T or  Current I Do this analysis for each fixed t.

© Copyright National University of Singapore. All Rights Reserved. MEASURING EFFICIENCY SEE, EG., H J GOLDSMID, “INTRO TO THERMOELECTRICITY.” Work done to load Entropy flow Peltier heat Joule heat flow back 16

© Copyright National University of Singapore. All Rights Reserved. EFFICIENCY ENHANCEMENT BY DRIVEN ZHOU, ET AL, ARXIV:

© Copyright National University of Singapore. All Rights Reserved. WITH EP INTERACTION, ARXIV: Wave form of drive. Entropy transport Breakdown of Onsager relation Displacement current Normalized efficiency 18

© Copyright National University of Singapore. All Rights Reserved. SUMMARY Structure change does bring in higher ZT, e.g., disorder, or go down to 0-dimension (quantum dot) Electron-phonon interaction reduces ZT Dynamic drive (forcing) improves ZT, up to a factor of 4 19

© Copyright National University of Singapore. All Rights Reserved. ACKNOWLEDGEMENTS Students: Hangbo Zhou, Juzar Thingna, Xiaoxi Ni Collaborators: Peter Hänggi, Baowen Li, Albert Liang GC 20

© Copyright National University of Singapore. All Rights Reserved. THANK YOU