Index. 2DACH, see two dimensional auto-correlation histogram
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1 Index 2DACH, see two dimensional auto-correlation histogram acceptor , , 289, , 310, 332 action spectroscopy , 244 adiabatic , 165, 168, 185, , 255, 303, 362, 384 adsorbates, molecular 195, 330 AFM 46, 52 53, 56, 68, 86 87, 89, 91, 104, 106, 309, 331, 334, 336 see atomic force microscopy alkane 56 57, , 122, 125, 288 alkanedithiols 420 alkanedithol 119 anchoring groups 109, 111, 126, 132 asymmetric bias profile 422 asymmetric molecule electrode contacts 133 asymmetric molecule electrode interface 131 asymmetric potential profile 414 atomic force microscopy (AFM) 46, 52, 68, 104, 309, 331, 336 Au electrodes 104, 111, 113, 115, 122, 244, 298, 300, 304 Au nanoelectrodes 237 Au(111) 297, 303, 305, 329, , 340, 346 auto-correlation histogram 136 azobenzene 67 69, 82 85, 87 88, 91 azobenzene derivatives 68, 85 azobenzene molecules 68, 91 azurin , 325, 327, , barrier height 15 19, 90, 138, 288, 299, barrier model , 407, barrier-shape conjecture 402, 404, 417, 424 BDA BDT, see benzenedithiol benzene , 334, 394 benzenedithiol (BDT) , , 229, 234, bi-potentiostat 329, 344 bias asymmetry factor bioelectronics 282 biomolecules 67, 70 71, 294, , 313, 331, 333 biosensors 70 71, 345 biphenyl 124 Born-Oppenheimer approximation 362, 382 Bose Einstein distribution function 379, 392 break junction technique 224, 237 break junctions 101, 106, 139, 410, 419 4,4 -bypiridine 107, 114
2 440 Index C-AFM 52 53, 68, 87, 89, 91 C8DA, see octanediamine C8DT, see octanedithiol C60 126, 227, 286, CAFM, see conducting atomic force microscopy CAFMBJ, see conducting-afm break junction carbon nanotube (CNT) 126, 251, 309, 313 cation-binding switchable molecular junction charge transport (CT) 51, 57, 106, 133, 140, 255, 281, 284, , 294, 296, 298, chemical linkers chemical potential 5, 180, 183, 194, 199, 254, 258, 263, 265, , 356, 363, , 380, 387 CMOS see complementary metal oxide semiconductor see complementary metal-oxide semiconductor CNT, see carbon nanotube co-factors , 330, 332, 334, 336, 338, 340, 342, co-tunneling processes 180, 183, 188 coherent tunneling 14 15, 18, 288 complementary metal oxide semiconductor (CMOS) 66, 398 complementary metal-oxide semiconductor (CMOS) 66 67, 92, 398 complexation 71, 77 82, conductance contact 90, 106 cytochrome 302 higher 26, 68 ohmic 397, 405 single-azurin 301 zero bias 228, 241 conductance attenuation factor 409 conductance histogram 107, , 124, , , 312, 419 conductance of DNA duplexes conductance traces 105, 107, 110, 116, 118, , 137 conducting-afm break junction (CAFMBJ) 106, 119 conducting atomic force microscopy (CAFM) 117 conducting probe AFM 52, 56 conductor 6 7, 252, 256, 265, 268, 270, , 366, 399 conjugation 124, 287 contact angle 73, 77 79, contact geometries 24, 112, 119, 287 contacts metal molecule 51 molecular-electrode 110 molecule electrode 124, 421 physisorbed 15 single-molecule 171 continuous-stretch mode 118, corrected Simmons (model, prefactor) 408 coupling asymmetric metal molecule 239 electrode molecule 413 coupling between the molecule and the electrode 241 cross-correlation , 139 CT, see charge transport current-induced force 373
3 Index 441 current-voltage 1, 302, 374, 387, 394 current-voltage spectroscopy 421 CV, see cyclic voltammetry cytochrome b cytochrome c data analysis 102, 110, 116, 122, , 139 decay constant 125, 138, 288 degree of coupling 138 density functional theory (DFT) 240, 353, , 362, 372, 382, 394 density-functional theory (DFT) , , 361, 385, 394, 400, 411, 415, 417 density functional theory, time-dependent 362 DFT, see density-functional theory DFT calculations 411 diarylethene dihedral angle 114, , 287 direct tunneling 26, 56, 138, 368, 399, , 424 DNA 70 71, 129, 140, 293, 295, electronic properties of DNA-based molecular junctions 129 DNA conductance 129, 307, 310, 314 DNA duplexes , 309, 311 donor , , 289, , 310, 332 double-barrier 133 dynamic molecular junction 65 68, 70 72, 74, 76, 78, 80, 82, 84, 86, 88, Dyson equation , 175, 177 EC-STM 305, , , 332, 334, 336, 338, 340, 342, 344, ECSTM, see electrochemical STM ECSTM/STS 327, 335, 343, 345, 347 ECSTS 327, 339, 344 EDLs, see electrochemical double layer egain 80, 87 88, 91 electrical characterization 55, 65 electrochemical double layer (EDLs) 292 electrochemical etching and deposition 109 electrochemical scanning tunneling microscope electrochemical STM (ECSTM) , 304, 327, , 339, 343, 345, 347 electrodes asymmetric 51, 132 macroscopic 2, 20, 67, 281 nanogap 224, electromigration 56, 109 electromigration nanogap junctions 56 electron-phonon interactions 134 electron transfer metalloproteins electron transport 50 52, , 104, 106, , , 118, , , , , 204, 327, , 394 non-equilibrium 394 resonant 179 electron tunneling, coherent 287, 342, 398 electron electron interactions 160, 166, 169, , 190, , 201
4 442 Index electronic devices hybrid molecular 104 molecular 58, 92, 281, 314, 399 electronic-vibrational coupling 161, 166, 171, 181, , , 196, ellipsometry 73, energetic alignment (of the HOMO or LUMO) 397, 399 energy gap 102, 138 environment 9, 38, 54, 66, 101, 129, , 298, , 308, 310, 328, 330, 344, 347 exchange-correlation , 361, 363 energy 361 kernel 361 local-density approximation 363 potential , 363 fabrication approaches 42, 46 47, 49, 51, 53 FC-2DCCH, see force-conductance two dimensional cross-correlation histogram Fermi level 5 6, 16, 19, 56, 133, 181, 190, 195, 202, 239, , 399, 401, 409, 412 Fermi wavelength 6, 354, 356, 359 Fermi Dirac distribution function 375, 378, 387 FET, see field-effect transistor field-effect transistor (FET) 290 field-effect transistor, single-molecule 291 field emission 18 20, 56, 138, 424 field-emission tunneling 402, 403, 424 Floquet theory 252 force-conductance trace 122 force-conductance two dimensional cross-correlation histogram (FC-2DCCH) 136 Fowler Nordheim diagram 401 Fowler Nordheim tunneling 14, 18, 26 Franck Condon blockade 188 Franck Condon contribution 242 Friedel oscillation 356 frontier molecular orbitals 111, 288, 292, 397, 399 graphene 47, 54, 68 69, 71, 290, 344 graphene electrode 68 Green 157, , , 252, 258, , 265, 361, Green operator, molecular 260, 262 Green s functions 168, 173, 175, 252, 364 vibrational 172, , Hamiltonian , , , 258, , 355, , 365, 381, , 392 Heisenberg equation of motion 168, Hellmann-Feynman theory 372 Herzberg Teller contributions 242 highest occupied molecular orbital (HOMO) 15 16, 19, 56, 102, 133, 241, 243, 288, ,
5 Index 443 HOMO, see highest occupied molecular orbital hydroquinone 345, 347 Kirchhoff s laws 127 Kondo effects 109, 140, 156 I(s) technique 108 IETS, see inelastic electron tunneling spectroscopy image charge 16 17, 134, 404, 406, 408, 410 image charge effect 16, 134, 406 image effects 410 inelastic electron tunneling spectroscopy (IETS) 131, 204, , 229, 231, 244, 387 inelastic tunneling spectroscopy 42 infrared spectroscopy 43, 45 interfacial electron transport 327 ion scattering spectroscopy (ISS) 57 ions 54, 71, 92, 129, 292, , 334, , irradiation 84 89, 249, 251 isomerization 67, 69, 82, 84 86, isotope effect 227, 232, 244 ISS, see ion scattering spectroscopy jellium model 355, 357, 371 junction conformations 110, 113, 119 junction lifetime Keldysh equations , 175, 177 Labview program 119 Landauer 7, , 253, , 264, 367, 406, 412 Landauer formula , 259, 412 Landauer theory 7 lateral confinement 406, 425 leads Lippmann Schwinger equation , , 372, 385, 394 liquid metal contacts 48 local heating , 156, 193, 195, , 251, 385, 390, 394 Lorentzian transmission 411 lowest unoccupied molecular orbital (LUMO) 15 16, 19, 26, 102, 133, , LUMO, see lowest unoccupied molecular orbital MCBJ, see mechanically controlled break-junction mechanically controllable break junction 224 mechanically controlled break junction 106 mechanically controlled break-junction (MCBJ) 107, 123, 126, 237 memory 66 67, 69 71, mercury drops 48, 68, 103
6 444 Index metal-molecule interactions 42, 241 metallization metalloprotein electrochemical behavior 302 micropore 68 (MO) energy offset 410, 416, 421, 424 molecular bridge 71, 156, 158, , 164, 168, , , 183, , , 196, 296 non-interacting 164, 175 molecular conformations 105, 115 molecular-electrode contact 110 molecule-electrode interfaces 101, 113, 115, , 123, , molecular electronic junctions 38, 45 46, 50, molecular junction 19 20, 65 68, 71 72, 77 83, , , 162, , , , , , , , molecular junctions 41 42, 44, 46 47, 51 54, 57 59, 65 66, 70 72, , , , , , , , molecular monolayers 46 48, 284 molecular orbitals 2, 15, 26, 56, 81, 89 90, 102, 111, , 159, 288, 292, molecular orientations 115 molecular rectifier , 133, 285 molecular rectifiers , 133, molecular structures 68, 101, 104, 123, 125, 128, 139, 282 molecular transistors 290, 343 molecular transport junctions 165 molecular wires 70, 137, , 327 molecule electrode coupling 115, 135, 413 molecule electrode interface 101, 113, 115, , 123, , molecule lead coupling 166, 169, 172, 174 moments of current counting statistics 370 shot noise 370 Moore s prediction 102 nanoelectronic devices 155, 398 nanoparticles 38, 68, 71, 109, 233 nanopore 42, 103 NDR, see negative differential resistance negative differential resistance (NDR) 131, 134, 156, NEGF, see non-equilibrium Green s function Newns Anderson model 343, 397, 400, , 414, 420, nitrite reductase 332 non-adiabatic 161, 252 non-equilibrium Green s function (NEGF) 157, 165, 177, 252, 361 non-monotonic 134 nonresonant tunneling 56, 90
7 Index 445 octanediamine (C8DA) octanedithiol (C8DT) , 114, , 131, 288, 409, octanethiol 20 21, 23, 27 oligophenylene vinylene (OPV) 236, 335, optical switch molecular junction OPV, see oligophenylene vinylene OPV-derivatized quinone organic molecules 4, 125, 131, 300 organic monolayers 42 44, 58 pulses 249, , 257, 271 PVS, see peak voltage spectroscopy PZT, see piezoelectric transducer quantum dot quantum scattering theory 250, 252 quantum transport quaterthiophene 73 74, quinones 327, , PCS, see point-contact spectroscopy peak voltage spectroscopy (PVS) 426 phononic heat conductance current photo-assisted , 253 photo-inert 253 photo-suppressed 253 photoisomerisable 83 photoisomerization 67 68, 88, 90, 92 piezoelectric transducer (PZT) planar electrodes 16 point-contact spectroscopy (PCS) , 229, 231, 244 Poisson equation 162, , 362, 364 Poisson Schrödinger equation preformed metal contacts Pt electrodes 227 Pt nanowires 20 21, 23 pulse 3, 23, , , 256, 258, 260, 262, 264, 266, , 296 Raman scattering 233, 236, 242, 331 surface-enhanced 223 Raman spectrum 224, 233, rectification 50, , 138, , 285 rectification ratio (RR) 133, 138, , , 391 rectifying effect 131 redox co-factor 327, 334 redox metalloprotein 288, 293, , , , 342, 344, 346, 348 resonant tunneling 90, 188, 193, , 300, 422 room temperature 20, 26, 50, 123, , 233, 243, 344 rotaxane 70 rotaxane molecules 70 RR, see rectification ratio SAMs, see self-assembled monolayers pristine 83, 86 88
8 446 Index saw-tooth scanning probe microscopy (SPM) 109, , 305 scanning probe microscopy break junction (SPMBJ) 107, 109, 111, , scanning tunneling microscope break junction (STMBJ) 70, 224, 286, 300, 302 scanning tunneling microscopy (STM) 3 4, 21 24, 68 69, , 108, , 239, , , 302, , 336, 338, , scanning tunneling microscopy break junction (STMBJ) 70, , 114, 120, 126, 301 scattering 6 9, 157, , 233, , 242, , , 259, , , , , , 389 electron phonon 392 inelastic electron vibration 389 scattering theory 157, 164, 250, , Schrödinger equation 362, 382 Seebeck coefficient , 379, , 426 self-assembled monolayers (SAMs) 46 49, 52, 57, 73 76, 78, 83, 85 88, 91, self-breaking 238 sensors 38, 71, 314 SERS, see surface-enhanced Raman scattering silicon 39, 43 45, 58 Simmons approach , 407, 409 Simmons model , 398, 404, 411, 419, 425 simulation , 140, 240, 363 single-level tunneling model 241 single-molecule break junction (SMBJ) , 106, 111, 113, , , , 129, 131, 133, 135, 137, single-molecule circuits 102, 127 single-molecule conductance 27, , , 109, 111, 113, 124, 126, 136, 286, 307, 314 single-molecule device 1 2, 4, 6, 8, 10, 12, 14, 16, 18, 20, 22, 24, 26, 28 29, 102 single molecule dynamics 224, 239 single-walled carbon nanotube (SWNT) 68, SMBJ, see single-molecule break junction SMBJs, see single-molecule break junction spectroscopic characterization 57 SPM, see scanning probe microscopy SPMBJ, see scanning probe microscopy break junction statistical analysis 106, 109, 308, 419 stimulus 27, 65 67, 69 71, 92 STM, see scanning tunneling microscopy STMBJ, see scanning tunneling microscope break junction stochastic fluctuations 397, Stokes components 236 stretch-hold sulfur 20, 75, 79, 83 superexchange 15, 289, 310, 399 surface-enhanced Raman scattering (SERS) 224, , 242, 244
9 Index 447 SWNT, see single-walled carbon nanotube template 39, 53 terahertz 249, 251 theory of electron transport , 357, 359, 361, 363 thermal fluctuations 105, 238 thermoelectric nanojunctions 374 thermoelectricity 242 inelastic Seebeck coefficient 390 nano-refrigerator 395 self-powered transistor 395 thermoelectric figure of merit ZT 374, , 390, thermopower 373, 376, 427 thioacetate 335, 345 Tien Gordon , 253, 259, , 271 time-dependent fields 249 time-periodic 250, 252, 257 time series analysis 136 trace 1, 21 22, 25, 107, , , 388 transient 38, , , , , 257, 271, 301 transient dynamics 249, 252 transistors single-molecule 2, 20, 27 single-particle transition voltage 19, 56, 81 82, 89 90, , 224, 291, , , , 410, 412, , , transition voltage spectroscopy (TVS) 89, , 397, , , 413, 415, 417 trapezoidal barrier 402 triangular barrier 402, 410 tunneling direct 138, 368, 399, incoherent 17 off-resonant sequential , 192, 288, 312 tunneling barrier 17, 26, 48, 90, 138, 299, 303, 402, 404, , 414, 424 tunneling current 21, 23 24, 108, , 298, , 336, , TVS, see transition voltage spectroscopy two dimensional auto-correlation histogram (2DACH) two-step coherent electron transfer 338 uncorrected Simmons 425 universality class 423 UV irradiation UV light 69, 84 85, vacuum 15, 19, 22, 28, 114, 123, 305, , , , 398, 404, 410, 425, 427 vacuum break junctions 410 vibration spectroscopy , 233, 244 vibrational excitation 179, , , , 201, 203
10 448 Index current-induced 157, 189, vibrational spectroscopy 42 43, 58, 88 vibronic coupling 183, 271, 382, 384 vibronic effects 157, 186, 202, , 383, 385, 387, 389, 391, 393 vibronic interactions 255 electron-vibration interactions 381 inelastic electron tunneling spectroscopy 387 local heating 385 vibronic transport 181, 186, 189, viologen 327 vitamins 334 voltage division factor 162, , 416 wide band , 264, 270 wide-band approximation 412 wide-band limit , 400 WKB approximation WKB method work function 15, 26, 52, 57, 404 working electrode 298, 328, 330 X-ray photoelectron spectroscopy 42, 57 XPS 57, 73, 75 79, 83 84, 331, 333
11 Prof. Mark A. Reed Yale University, USA Molecular electronics, an emerging research field at the border of physics, chemistry, and material sciences, has attracted great interest in the past decade. It aims at fabricating devices with sizes of nanometers under atomic control, by developing novel bottom-up approaches, as opposed to the classical top-bottom approaches. To achieve the ultimate goal of designing molecular electronic devices with desired functionality and experimental manipulation at the singlemolecule level, the microscopic understanding of electron transport at the nanoscale is an important prerequisite. This book, a multi-authored volume comprising reviews written by leading scientists, discusses recent advances in the field. To make the book useful for scientists of various disciplines interested in learning by doing, each chapter is written in a scientific/tutorial hybrid style, with its own introduction, presenting fundamental concepts and frameworks. Adopting a pedagogical, self-contained manner of presentation, the chapters provide guidelines for young scientists (physicists, chemists, and engineers) planning to actively contribute, as experimentalists or theorists, to molecular electronics. Still, a series of results are new and can certainly be inspiring and of interest to specialists in the field. The content reflects the strong transdisciplinary efforts needed for substantial progress. V471 ISBN Bâldea Ioan Bâldea is principal investigator at the Chair of Theoretical Chemistry, University of Heidelberg (Germany), and full research professor of theoretical physics at the Institute of Space Sciences, National Institute for Lasers, Plasma, and Radiation Physics, Bucharest (Romania). His research work comprises general theory of condensed matter physics, materials science, and quantum chemistry. In recent years, he has mainly focused on molecular electronics and nanotransport, with emphasis on quantum dots, quantum dots nanoarrays, transition voltage spectroscopy, solvent effects and reorganization effects in molecules with floppy degrees of freedom. Molecular Electronics This book contains state-of-the-art reviews of some of the most important experimental and theoretical aspects of electronic transport at the molecular level. The blend of tutorial aspects with cutting-edge results and approaches makes it an important reference for those interested in working in the field. Molecular Electronics An Experimental and Theoretical Approach edited by Ioan Bâldea
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