Designing Principles of Molecular Quantum. Interference Effect Transistors
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1 Suorting Information for: Designing Princiles of Molecular Quantum Interference Effect Transistors Shuguang Chen, GuanHua Chen *, and Mark A. Ratner * Deartment of Chemistry, The University of Hong Kong, Pokfulam Road, Hong Kong Deartment of Chemistry, Northwestern University, Evanston IL, AUTHOR INFORMATION Corresonding Author * ghc@everest.hku.hk * ratner@northwestern.edu S1. Methodology The systems investigated are molecular devices comosed of a π-conjugated ring connected to two semi-infinite electrodes. The Hückel tye Hamiltonian of the total system can be written in the second quantized form as, + ( ) ò + H = d d t d d d 1 d + c c ( V c d + H. c.) k k k k k k, k, S1
2 Where is the onsite energy of the system; t is the hoing between nearest neighboring sites; òk is the energy of the k-th eigen state of electrode ; Vk is the couling matrix element between site of the molecule and the k-th eigen state of electrode ; d, d, ck, ck are the creation and annihilation oerators for the molecular sites and electrodes, resectively. The time-deendent current is obtained via the time-deendent density functional theory for oen system (TDDFT-OS) method. 1-4 The equations of motion of reduced single electron density (RSDM) and the dissiation matrices reads, i t h t t t t (1) D( ) = [ D( ), D( )] [ ( ) ( )] i (, t) = [ h ( t) ( t)] (, t) + [ f ( ) ] ( ) + d ' (, ', t) (2) D D, ' i (, ', t) = [ + ( t) ' ( t)] + ( ') (, t) ( ', t) ( ) (3), ' ', ' ' ' Where hd () t and D () t are the Fock oerator and RSDM of the device at time t, resectively; (, t) is the energy resolved first-tier dissiation matrix of electrode α with ( t) = d (, t) ; f = e + is the Fermi-Dirac distribution ( ) ( ) 1/[ 1] function for electrode, where is the inverse temerature and is the equilibrium Fermi energy; ( t) = V ( t) is the energy shift caused by alied voltage for all single-electron levels in electrode ; ( ) is the line-width matrix due to S2
3 electrode ; (, ', t), ' is the second-tier dissiation matrix. The time-deendent electric current through electrode can be obtained by taking the trace of the dissiative term, ( ) ( ) ( ) I t = itr t t (4) The steady state currents through the electrodes are evalutated through the Landauer- Büttiker formula, i.e., 2e I = d ( fl( ) fr( )) T( ) h (5) The time-deendent local current from site m to site n can be exressed in terms of lesser Green s function, 2e I ( t) ( V G = ( t, t) V G ( t, t) ) (6) mn ij ji ji ij im jn, nm Where Vij is the hoing element (i, j) in Fock matrix; lesser Green s function in time domain. G t t = i c t c t is the ij (, ') j ( ') i( ) The Büttiker robe aroach is used to control the state of the molecular device through dehasing effect, 5-6 which is described by a self-energy term = i and an r associated chemical otential, where = 1,2,, N with N being the total number of Büttiker robes. As a result, another set of dissiation matrices () are generated, which can be solved in the same way as () t for source and drain electrodes. Usually, there will be net currents assing through the Büttiker robes. However, by carefully adjusting the chemical otential, the current conservation law can be conserved and t S3
4 the net currents through the Büttiker robes will be zero. Such values of chemical otentials can be easily obtained by solving a set of linear equations when bias voltage is small and temerature is low. 7 S2. The effect of varying the couling strength between the molecular junction and the Büttiker robe on current. Figure S1. Steady state current versus the source-drain voltage with büttiker robes of different couling strengths on osition 3 and 4 for 2, 5-linked erylene junction. The decoherence effect of Büttiker robe can be achieved by scanning tunneling microscoe (STM) techniques, where the couling strength γ P between the molecular junction and Büttiker robe is a function of the distance between the STM ti and the substrate where molecular junction is located. We investigate the effect of varying the couling strength of the Büttiker robe on current. Fig. S1 shows the steady state current through the electrode of the 2, 5-linked erylene junction with two Büttiker robes laced at osition 3 and 4. Since the wideband-limit aroximation is adoted on the electronic structure of the electrode, the largest bias voltage is confined to 0.01 V and the I-V curves are exected to be in the linear resonse region. The couling strength is tuned from 0.2 ev to 2.5 ev, which mimics the situation of different searations between the STM ti and the molecule junction on substrate. It can be found from Fig. S1 that the enhancement on the couling strength indeed induces a larger source-drain current. The results are consistent with our theoretical analysis. When the couling strength is enhanced, more electrons will go into the Büttiker robes and lose their hases when exit. As a result, the destructive interference is suressed and the source-drain current increases. S4
5 S3. The resonse of the transient current to switching on/off the Büttiker robes for a 2, 5-linked erylene based molecular junction. Figure S2. Time-deendent source/drain current of the 2, 5-linked erylene molecule with two Büttiker robes at osition 3 and 4 being switched off at t=20fs then switched on again at t=100fs. The resonse of the transient current to switching on/off the Büttiker robes laced at osition 3 and 4 for a 2, 5-linked erylene based molecular junction is shown in Fig. S2. At the initial time, the Büttiker robes are switched on and the source/drain current increases after bias voltage is alied. It takes about 10 fs for the current to reach its steady state. At t=20 fs, the Büttiker robes are suddenly switched off and the current begins to dro due the recovery of the destructive interference. The oscillations of the current followed take about 30 fs before a very small residue current (~0.36 na) is reached. At t=100 fs, the Büttiker robes are switched on again, and the current recovers to its original steady state value in about 20 fs. The on/off ratio for this setu is between 10 3 and Reference (1) Zheng, X.; Wang, F.; Yam, C. Y.; Mo, Y.; Chen, G. Time-deendent densityfunctional theory for oen systems. Phys. Rev. B 2007, 75, (2) Zheng, X.; Chen, G.; Mo, Y.; Koo, S.; Tian, H.; Yam, C.; Yan, Y. Time-deendent density functional theory for quantum transort. J. Chem. Phys. 2010, 133, (3) Xie, H.; Jiang, F.; Tian, H.; Zheng, X.; Kwok, Y.; Chen, S.; Yam, C.; Yan, Y.; Chen, G. Time-deendent quantum transort: an efficient method based on liouvillevon-neumann equation for single-electron density matrix. J. Chem. Phys. 2012, 137, S5
6 (4) Chen, S.; Xie, H.; Zhang, Y.; Cui, X.; Chen, G. Quantum transort through an array of quantum dots. Nanoscale 2013, 5, (5) Büttiker, M. Role of quantum coherence in series resistors. Phys. Rev. B 1986, 33, (6) Chen, S.; Zhang, Y.; Koo, S.; Tian, H.; Yam, C.; Chen, G.; Ratner, M. A. Interference and molecular transort a dynamical view: time-deendent analysis of disubstituted benzenes. J. Phys. Chem. Lett. 2014, 5, (7) Kilgour, M.; Segal, D. Inelastic effects in molecular transort junctions: The robe technique at high bias. J. Chem. Phys. 2016, 144, S6
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