Electron transport through molecular junctions and FHI-aims
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1 STM m metallic surface Electron transport through molecular junctions and FHI-aims Alexei Bagrets Inst. of Nanotechnology (INT) & Steinbuch Centre for Computing Karlsruhe Institute of Technology (KIT), Germany 1 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
2 Why transport calculations for molecules? Technological reason (molecular electronics) use of molecular building blocks for the fabrication of electronic components design suitable molecular complexes with required functionality, e.g. memory elements, switches, diods or transistors data trasnfer by charge (or spin) transport required (transport) theories with predicative power: computer aided device design (Fundamental) scientific reason molecules are quantum dots with unexplored parameters regimes and symmetry properties attempt to understand and predict qualitatively new transport phenomena 2 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
3 Single molecule electronics : experiments STM break junctions mechanically controlled break junctions Xu & Tao, Science '03 Weber, Mayor, v. Löhneysen, et al. PRL 02 3 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
4 Single molecule electronics : experiments Electromigrated junctions: Coulomb blockade di(v)/dv Park, McEuen, Ralph, et al. Nature 02 4 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
5 Single molecule electronics : experiments Excitation lines: electronic fingerprints of molecular vibrations Osorio et al. Adv. Materials 07 5 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
6 Single molecule electronics : experiments Electromigrated junctions: Kondo effect di-vanadium-complex di(v)/dv Liang et al. Nature 02 6 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
7 1. Essentials of ab initio transport simulations 7 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
8 Transport in the scattering picture 8 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
9 Attaching reservoirs to nanosystem Green s function formalism 9 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
10 Attaching reservoirs to nanosystem Green s function formalism 10 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
11 Charge exchange and life-time effects µ µ µ µ 11 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
12 Classical dilemma level broadening level spacing 12 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
13 2. Self-energy as absorbing boundary condition 13 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
14 Gedankenexperiment: Σ em as absorb. boundary condition 14 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
15 Gedankenexperiment: Σ em as absorb. boundary condition 15 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
16 Gedankenexperiment: Σ em as absorb. boundary condition F Evers & A Arnold, CFN Lectures on Functional Nanostructures Vol.2, Lecture Notes in Physics Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
17 Test cases: tight-binding chain Parameterization of the self-energy 128 F Evers & A Arnold, CFN Lectures on Functional Nanostructures Vol.2, Lecture Notes in Physics Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
18 Test cases: tight-binding chain Parameterization of the self-energy 128 F Evers & A Arnold, CFN Lectures on Functional Nanostructures Vol.2, Lecture Notes in Physics Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
19 Recipe to perform transport calculation -iη(x n ) 19 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
20 AITRANSS module: library of electrodes fcc Au clusters: - chaotic cavities, left/right assymetric, - gradualy increasing size, - abc are active at grey atoms, parametrized by a local leakage function x3 x3a x4 x4a 15 x 2 19 x 2 29 x 2 41 x 2 -iη(x)δ(x-x ) AITRANSS (ab initio transport simulations): transport module developed at Inst. of Nanotech. (INT) at KIT (by F Evers, A Arnold, F Weigend & AB) interfaced to FHI-aims & TURBOMOLE 20 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
21 AITRANSS module: library of electrodes fcc Au clusters: - chaotic cavities, left/right assymetric, - gradualy increasing size, - abc are active at grey atoms, parametrized by a local leakage function x3 x3a x4 x4a 15 x 2 19 x 2 29 x 2 41 x 2 -iη(x)δ(x-x ) AITRANSS hands-on tutorial Today, Wed, 29 August 14:00-16:00, Math. Instutute, Room 0.30 AITRANSS (ab initio transport simulations): transport module developed at Inst. of Nanotech. (INT) at KIT (by F Evers, A Arnold, F Weigend & AB) interfaced to FHI-aims & TURBOMOLE 21 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
22 3. Paradigmatic studies: benzene-dithiol & alkyl chains 22 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
23 Archetypical example: transmission through BDT fhi-aims: tier2,convergence vs system size x3 Transmission T(E) E F HOMO* x3a x4 E E F [ev] x4a η ~ 0.1 Ha 23 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
24 Archetypical example: transmission through BDT Gaussian basis sets (tzvp, TURBOMOLE) vs numerical AOs (tier2, FHI-aims) Transmission T(E) E F HOMO* LUMO* x4a η ~ 0.1 Ha E E F [ev] 24 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
25 Alkanedithiols: wide band-gap insulators Conductance of n-alkanedithiol: G( n) = 2e h 2 T ( E F ) ~ exp[ β n] Theory: β N = 0.85 Experiment: β N ~ 1.00 (Jülich) Ch Li, I Pobelov, Th Wandlowski, AB, A Arnold & F Evers JACS 130 (2008) 318 N 25 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
26 Challenges in DFT based transport calculations Koentopp, Burke & Evers, PRB 04 LUMO transport: missing derivative discontinuity of the local XC functional local XC exact XC 26 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
27 Challenges in DFT based transport calculations Koentopp, Burke & Evers, PRB 04 LUMO transport: missing derivative discontinuity of the local XC functional local XC exact XC HOMO transport: spirious self-interaction of local XC func 27 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
28 Spin transport & magnetoresistance across H 2 Pc extended molecule spin-polarized STM tip magnetic substrate Key observation: magnetoresistance ~ 60% through H 2 Pc in STM setup Nature Nano 6, 185 (2011) by S.Schmaus, AB, Y.Nahas, et al. 28 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
29 Spin transport & magnetoresistance across H 2 Pc extended molecule spin-polarized STM tip magnetic substrate Key observation: magnetoresistance ~ 60% through H 2 Pc in STM setup Nature Nano 6, 185 (2011) by S.Schmaus, AB, Y.Nahas, et al. 29 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
30 Thanks to Florian Weigend Ferdinand Evers Michiel van Setten Funding: DFG Center for Functional Nanostructures (CFN) SPP1243 Quantum transport at the molecular scale DFG BA4265 Electron transport & magnetism in single molecules 30 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
31 Thank you for your kind attention! Florian Weigend Ferdinand Evers Michiel van Setten Funding: DFG Center for Functional Nanostructures (CFN) SPP1243 Quantum transport at the molecular scale DFG BA4265 Electron transport & magnetism in single molecules 31 Alexei Bagrets FHI-aims Developers' and Users' Meeting - August 28-31, 2012
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