Tailoring Electrical Contact Resistivity at Metal-Thermoelectric Interfaces Using a Molecular Nanolayer

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1 Tailoring Electrical Contact Resistivity at Metal-Thermoelectric Interfaces Using a Molecular Nanolayer Thomas J. Cardinal Graduate Student Department of Materials Science & Engineering Rensselaer Polytechnic Institute, Troy, NY, USA Professor Ganpati Ramanath Devender, Professor Theo Borca-Tasciuc 2014 Rensselaer Nanotechnology Center Research Symposium Wednesday, October 29, 2014

2 Nanomolecular monolayers (NML) Self assembly Diffusion barriers in Cu- based systems [1] [1] P. G Ganesan et al., Appl. Phys. Lett., (2004) Improve thermal conductivity [2] and mechanical strength [3] of Cu-SiO 2 interfaces [2] P. O Brien et al., Nat Mat. (2012) [3] D.D. Gandhi et al., Nature (2007) Organosilanes found to improve Au/Ni- Bi 2 interface resistivity [4] [4] S.P. Feng et al., PCCP (2013) Adsorption from liquid solution substrate APPROACH: Double Sulfur-terminated NML 1,8-octanedithiol (ODT) S-Metal bonds known to form [1,2,3] S-Bi, S-Te bonds known to form as well [5] [5] R.J. Mehta et al., Nat. Mat (2012)

3 Intensity (a.u.) (a.u.) NML-Functionalized Bi 2 FUNCTIONALIZATION PROCEDURE 5 mm ODT in ethanol prepared n-bi 2 samples polished with 1200 grit SiC Samples immersed in solution for 60 min Low humidity glovebox Sonicate in ethanol to remove physisorbed species GOAL: Achieve a single edge-standing layer of ODT 1.5 nm [1] [1] Jun et al., Langmuir (2006) Take-off angle (degrees) Take-off angle (degrees) BiO x 4f 7/2 source x-rays MNL Oxide n-bi 2 d / sinα detector electron take-off angle α Variable take-off angle XPS measures MONOLAYER of ODT BiO x 4f 7/2 d ODT = 1.6 ± 0.3 nm d ODT = 1.6 ± 0.3 nm (sin ) -1 (sin ) -1 ln I = 1 sin α d MNL λ MNL + k

4 Intensity (a.u.) Intensity Ratios Intensity (a.u.) NML Characterization on Bi 2 Surfaces 1.5 BiO x 4f to Bi 2 4f Bi 4f 5 mm ODT 60 min 166 S 2s 5 mm ODT 60 min S-Te Bi BiO x 4f 5/2 4f 7/ Binding energy (ev) S-Bi Binding energy (ev) Nanoscale oxide formation on Bi 2 surface. Sulfur bonding with Bi 2 surface Min BiO x, O & Max S for 5 mm, 60 min O 1s to Bi 2 4f 2.5 mm 15 mm 5 mm S 2p to Bi 2 4f Functionalization time (min)

5 Resistance ( ) Contact conductivity, Σ c via Cox & Strack method R t = R sm 2π ln a b R sm 4π 1 b2 a 2 + 4R c π t 1 a 2 + ρ πa tan 1 4t a + R o Probe tip b a Contact metal Bi 2 Indium backing μm Cu-ODT-Bi Contact conductivity c M -1 m ODT-Bi 2 Bi 2 ODT-Bi 2 Bi 2 Cu Ni Pad diameter (cm -1 )

6 Intensity (a.u.) Bonding characteristics of S-Cu & S-Ni S 2s Ni Cu EXPERIMENT: Cu, Ni pellets immersed in 5 mm solution of 1-Octanethiol for 1 hour, rinsed & sonicated in ethanol XPS characterization immediately afterward S 2p Cu Ni Stronger S signal on Cu vs Ni S readily bonds with Cu O 1s O scavenged by S in Cu system Ni Cu Binding energy (ev)

7 Intensity (a.u.) Bonding characteristics of S-Cu & S-Ni C 1s Ni Cu Broader C 1s signal on Ni Presence of C bonds other than - [CH 2 ]- groups 294 Ni 2p N i Ni O x Ni 3 C, CO-Ni, CO, CO 2 NiO x band clearly present in Ni 2p Cu 2p band shows only Cu 0 state. No oxide detected. P.G. Ganesan, et al., Applied Physics Letters 87, (2005). 1/2 3/ Cu 2p 1/2 3/ Binding energy (ev)

8 Intensity (a.u.) Diffusion characteristics of Cu-ODT-Bi 2 via RBS Cu SUR Te SUR Bi SUR Te SUB Cu/ODT/Bi 2 = 125 C Cu/Bi 2 = 125 C Cu/ODT/Bi 2 = 100 C Cu/Bi 2 = 100 C Cu/ODT/Bi 2 = 50 C Cu/Bi 2 = 50 C Bi SUB Energy (MeV) Very little interdiffusion upon annealing at 50 ºC and 100 ºC Almost no Cu on surface without ODT after anneal at 125 ºC Considerable amount of Cu on surface with ODT after 125 ºC anneal Some Bi & Te are at surface for system with ODT Cu-Bi 2 Cu-ODT-Bi 2 ODT is inhibiting Cu diffusion upon annealing. 50 ºC 100 ºC 125 ºC

9 Intensity (a.u.) Intensity (a.u.) Intensity (a.u.) Grazing Incidence XRD (GID) Cu-Bi 2 Bi 2 (101) Cu-ODT-Bi 2 Cu 2 Te As deposited = (degrees) GID reveals Cu 2 Te phases not detected via standard θ - 2θ diffraction. Cu 2 Te signal suppressed when ODT is present at interface upon annealing. Bi 2 (101) 50 C anneal = 1 Bi 2 (101) 150 C anneal = 1 Cu-Bi 2 Cu 2 Te Cu 2 Te Cu-Bi 2 Cu-ODT-Bi (degrees) Cu-ODT-Bi (degrees)

10 Concluding remarks ODT able to self-assemble on Bi 2 surface Interfacial chemistry impacts electric contact conductivity Σ c 10 times higher when ODT at Cu-Bi 2 interface 20% decrease in Σ c when ODT at Ni-Bi 2 interface Strong Cu-S bonding in comparison to Ni-S bonding Σ c enhancement for Cu-Bi 2 system due to interfacial preservation ODT found to be diffusion barrier Cu 2 Te formation suppressed Careful selection of NML with interfacial system critical to achieve desired properties

11 Acknowledgements Professor Ganpati Ramanath Professor Theo Borca-Tascuic Indira Seshadri Devender Matt Kwan Andrew Gaul Alex Clement Kelly Lofgreen Ravi Mahajan Jelena Culic-Viskota

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