Transport Calculations with TranSIESTA T SIESTA

Pablo Ordejn
Instituto de Ciencia de Materiales de Barcelona - CSIC, , Spain p

M B M. Brandbyge, db K St K. Stokbro kb and dJ J. T Taylor l

Mikroelectronik Centret - Technical Univ. Denmark

Jose L. Mozos and Frederico D. Novaes

Instituto de Ciencia de Materiales de Barcelona - CSIC, Spain

The SIESTA team

E. Anglada, E. Artacho, A. Garca, J. Gale. J. Junquera, D. Snchez-Portal, J. M. Soler, ....

Outline
1 Electronic transport in the nanoscale: Basic theory 1. 2. Modeling: the challenges and our approach: The problem at equilibrium (zero voltage) Non-equilibrium (finite voltage) 3. Practicalities

1. Electronic Transport p in the Nanoscale: Basic Theory

L
Scattering in nano-scale systems:
electron-electron interactions phonons impurities, defects elastic scattering by the potential of the contact

d << Lm d

Semiclassical theory breaks down QM solution needed Landauer formulation: Conductance as transmission probability S. Datta, Electronic transport in mesoscopic systems (Cambridge)

Narrow constriction (meso(meso-nanoscopic)

E

kx Transversal confinement QUANTIZATION

(x, y) = m (y ) e

ik x x

2k 2 x Em ( (k x ) = m + 2 2m

Landauer formulation - no scattering

E +

= eV
2e 2 I = 2e d k f ( k ) v g ( k , i) V N bands (E F ) h BZ i
bands

2e 2 12.9 12 9 k QUANTUM OF CONDUCTANCE GO = h

I 2e 2 G = = N bands = N bands G0 V h

Landauer formulation - scattering

Transmission probability of an incoming electron at energy :

T ( ) =Tr [ t t ] ( )

Current:

transmission matrix:

out = t in

eV

2e 2 I = d (fL ( ) fR ( ))T ( ) h

P f t conductance Perfect d t ( (one channel): h l) T=1 T 1

2e 2 GO = h

2. Modeling: g The Challenges and Our Approach

Model the molecule-electrode system from first principles: No parameters fitted to the particular system DFT Model a molecule coupled to bulk (infinite) electrodes Electrons out of equilibrium (do not follow the thermal Fermi occupation) Include finite bias voltage/current and determine the potential profile Calculate the conductance (quantum transmission through the molecule) Determine geometry: Relax the atomic positions to an energy minimum

Restriction: Ballistic conduction

Ballistic conduction: consider only the scattering of the incoming electrons by the potential created by the contact

Two terminal devices (three terminals in progress)

Effects not described: inelastic scattering electron-electron interactions (Coulomb blockade) phonons h ( (current-induced ti d d phonon h excitations) it ti )

First Principles: DFT

Many y interacting-electrons g problem mapped p pp to a one particle problem in an external effective potential (Hohemberg-Kohn, Kohn-Sham)

Veff =Vext +Vps +VH +VXC

Charge density as basic variable:

Veff =Veff [ ( r )]
Self-consistency: Ground G d state t t th theory:

Veff

VXC

SIESTA

http://www uam es/siesta http://www.uam.es/siesta

Soler, Artacho, Gale, Garca, Junquera, Ordejn and Snchez-Portal J. Phys.: Cond. Matt. 14, 2745 (2002) Self consistent DFT code (LDA, GGA, LSD) Self-consistent Pseudopotentials (Kleinman-Bylander) LCAO approximation: B i set: Basis t Confined Numerical Atomic Orbitals Sankeys fireballs

(r )

Order N methodology (in the calculation and the solution of the Order-N DFT Hamiltonian)

TRANSIESTA
Implementation of non-equilibrium electronic transport in SIESTA Atomistic description (both contact and electrodes) Infinite electrodes Electrons out of equilibrium Include finite bias and determine the potential profile Calculates the conductance (both linear and non non-linear) linear) Forces and geometry Brandbyge, Mozos, Ordejn, Taylor and Stokbro Phys. Rev. B. 65, 165401 (2002) Mozos, Ordejn Mozos Ordejn, Brandbyge Brandbyge, Taylor and Stokbro Nanotechnology 13, 346 (2002)

The problem at Equilibrium (Zero Bias)

Challenge:
Coupling the finite contact to infinite electrodes

Solution:
Greens Functions

G (z ) = (z - H )1 1 ( ) = Im G ( + i )

(r ) =

d ( ) nF ( F ) (r ) (r )

Setup ( (zero bias) )

L
Contact:

G ( ) = ( H ) =
1

... -VL

-VL + - H L -VLC -V VCL - HC -VRC

-V VCR - HR -VR

-VR+ ...

Contains the molecule, and part of the Right and Left electrodes Sufficiently large to include the screening

B L

Solution in finite system:

R B

H L L VLC V G ( ) = HC CL VRC

VCR HR R

( ) = Selfenergies Selfenergies. Can be obtained from the bulk Greens functions

Lopez-Sancho et al. J. Phys. F 14, 1205 (1984)

Calculations ( (zero bias): )

Bulk Greens functions and self-energies (unit cell calculation) Hamiltonian of the Contact region:

SCF PBC
Solution of GFs equations (r) Landauer-Bttiker: transmission probability:

T ( ) =Tr t t ( )
1/2

[ ]

t ( ) = (Im [ R ( )])

1/2

G ( )

(Im [L ( )])

The problem at NonNon-Equilibrium (Finite Bias)

L
L
2 add additional to a p problems: ob e s
Non-equilibrium situation: current flow two different chemical potentials Electrostatic potential with boundary conditions

C
e-

R
R

NonNon -equilibrium formulation:

Scattering states (from the left) Lippmann-Schwinger Lippmann Schwinger Eqs.: Non-equilibrium Density Matrix:

l = lo + G (o ) VL lo

D = d [ L ( ) nF ( L ) + R ( ) nF ( R )]

1 ( ) = ( G ( + i ) Im [ L ( + i )]G t ( + i ))
L

Electrostatic Potential
Given (r), VH(r) is determined except up to a linear term:

VH (r ) = (r ) + a r + b
+V/2
Au 12 au

( r): particular solution of

P i Poissons equation ti a and b: determined imposing BC: the shift V between electrodes ( (r) ) computed p using g FFTs Linear term:

-V/2
Au

V L

L z 2

3. TranSIESTA Practicalities
3 Step process:
1. SIESTA calculation of the bulk electrodes, to get H, , and Self-energies Self energies 2. SIESTA calculation for the open system reads the electrode data builds H from solves the open problem using Greens Functions (TranSIESTA) builds b ild new 3. Postprocessing: compute T(E), I, ...

 H L L VLC G ( ) = HC VCL VRC

VCR HR R

Supercell - PBC
H, DM fixed to bulk in L and R DM computed in C from Greens functions HC, VLC and VCR computed in a supercell approach (with potential ramp) B (buffer) does not enter directly in the calculation (only in the SC calc. for VHartree)

Contour integration g

Contour Integration

SolutionMethod Transiesta

GENGF OPTIONS -3.0 Ry 6 20 3 -3.0 Ry 2.d0 Ry 100

TS.ComplexContour.Emin TS.ComplexContour.NPoles TS.ComplexContour.NCircle TS.ComplexContour.NLine TS.RealContour.Emin TS.RealContour.Emax TS.TBT.Npoints

# TS OPTIONS TS.Voltage S l 1 000000 eV 1.000000 TS.UseBulkInElectrodes .True. TS.BufferAtomsLeft 0

TS.BufferAtomsRight 0

# TBT OPTIONS TS.TBT.Emin -5.5 eV TS TBT Emax +0 TS.TBT.Emax +0.5 5 eV TS.TBT.NPoints 100 TS.TBT.NEigen 3