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1
2 A4 A4
3
4 Ubiquitous
5 * ) * ),,,, 1-4 (2002).
6 Bashforth-Adams Fitting
7 versus Insensible at sensible distances (Laplace, Pierre-Simon ( )) The attractive forces were left to perform impossible feat of balancing themselves (Lord Rayleigh (John William Strutt, ( )) J. S. Rowlinson and B. Widom, Molecular Theory of Capillarity, Clarendon Press, (1982). [Dover ]
8 van der Waals 1873 J. S. Rowlinson, Cohesion A Scientific History of Intermolecular Forces, Cambridge Univ. Press, (2002).
9 etc etc etc (e.g.,
10 B. Alberts, A. Johnson, J. Lewis, M. Raff, K. Roberts, and P. Walter, Molecular Biology of the Cell, 4 th ed., Garland, (2001).
11 B. Alberts, A. Johnson, J. Lewis, M. Raff, K. Roberts, and P. Walter, Molecular Biology of the Cell, 4 th ed., Garland, (2001).
12 nm (10-9 m )
13
14
15 Properties of of Gold Surface STM (Scanning Tunneling Microscope)
16 (Scanning Tunneling Microscope, STM) FromR. Wiesendanger, Scanning Probe Microscopy and Spectroscopy, (1994).
17 1986
18 FromR. Wiesendanger, Scanning Probe Microscopy and Spectroscopy, (1994).
19 FromR. Wiesendanger, Scanning Probe Microscopy and Spectroscopy, (1994).
20 STM STM images of gold substrates prepared by vapor-deposition on mica: a) Before annealing, b) after annealing at 798 K, c) magnified view of b).
21 R. I. Masel, Principles of Adsorption and Reaction on Solid Surfaces, Wiley (1996), Chap.2.
22
23 Properties of of Self-assembled Monolayers Thiol-derivatives on on Gold SH SAM)
24 Self-assembled monolayer (SAM) of thiol derivatives on Au(111) --- Thiol solution Au Simple! ( ) ο 3 3 R30
25 S. Chon, W. Paik, Phys. Chem. Chem. Phys., 3, 3405 (2001).
26 STM images of undecanethiol SAM on Au(111) STM
27 Au(111) STM STM images of undecanethiol SAM on Au(111)
28 Orientation of of thiolates on on Au(111)? Au(111) STM S
29 +
30 All-trans Model Tilt φ~30º Rotation ϕ~50º for long chain alkanethiol SAM on Au θ odd (φ, ϕ) = 27º θ even (φ, ϕ) = 58º
31 Sum Frequency Generation SF light only from interface Molecular orientation
32 Broad-bandwidth SFG L. J. Richter, T. P. Petralli-Mallow, J. C. Stephenson, Opt. Let. 23, 1594 (1998). Conventional SFG SFG Broad-bandwidth SFG Sweep of ω IR correction needed (intensity, path) No sweep of ω IR
33 SFG System (Tokyo Instruments, Inc. )
34 Assignment of vibrational modes 1 (a) n=14 ν / cm -1 Mode Abbreviation 2964 r - CH 3 ν as SF intensity / a.u. 0 1 (b) n= CH 3 ν s (FR) r + FR 2877 CH 3 ν s r tch 2 ν s d + ω No methylene vibrational modes (should appear at 2850 and 2920 cm -1 ) Wavenumber / cm -1 Fig. Sum frequency vibrational spectra for SAM of (a) PDT (n=14) and (b) HDT (n=15) on Au(111) surface. Depth of r + and r - is different for odd and even
35 V V r+ r 4 cosθ cosθ cos 3 θ Chain-length Dependence of θ V V r r+ 3 < cos cos θ > = D = < cosθ > 4 θ 2 Dsin θ (delta distribution) (D = 3.5) Vr- / Vr even odd Vr-,calc / Vr+,calc Number of methylene unit Methyl angle, Increase in θ even, constant θ odd for shorter chain length N. Nishi, D. Hobara, M. Yamamoto, and T. Kakiuchi, J. Chem. Phys., 118, (2003).
36 Pretty good picture
37 pk pk = -log K d K d CH 3 COOH K d = [CH 3 COO - ][H + ]/[CH 3 COOH] 4.8
38 Another example: Acid-base equilibrium is is dramatically altered on on SAM surface pk 4.8
39 T. Kakiuchi, M. Iida, S. Imabayashi, and K. Niki, Langmuir, 16, 5397 (2000).
40 pk aq. solution SAM surface -COOH NH T. Kakiuchi, M. Iida, S. Imabayashi, and K. Niki, Langmuir, 16, 5397 (2000).
41 Properties of of Two-component SAMs H + H + H + H + H + H Au - - -
42 Multi-component SAMs SAMs Binary Binary Ternary, etc etc + Miscibility? or
43 U AA, U BB, U AB U AA, U BB << U AB Phase-separation U AA ~ U BB ~ U AB Homogeneous mixing: ideal U AA,, U BB >> U AB Homogeneous mixing: non-ideal
44 STM images of MUA-UDT binary SAMs MUA UDT SAM STM SAMs prepared from 0.5 mm MUA mm UDT EtOH T. Kakiuchi, M. Iida, N. Gon, D. Hobara, S. Imabayashi, and K. Niki, Langmuir, 17, 1599 (2001).
45 STM images of MPA-HDT binary SAMs MPA SAM STM U AA, U BB << U AB D. Hobara, M. Ohta, S. Imabayashi, K. Niki, and T. Kakiuchi, J. Electroanal. Chem., 444, 113 (1998).
46
47 Two-dimensional surfactants SAM Two-dimensional solubilization
48 SAM
49
50
51 Nanometer-scale engineering of of SAM SAM domains SAM
52 Selective replacement of of thiol domains Selective removal of MPOH domains
53 MPA UDT MPA HDT Prepared from MPA:UDT 7:1 Insertion of HDT Prepared from MPA:UDT 10:1 D. Hobara, T. Sasaki, S. Imabayashi, and T. Kakiuchi, Langmuir, 15, 5073 (1999).
54 Skip some other interesting features: Domain size Mutual solubility Replacement by exchange reactions Effects of solvent and temperature on SAM formation Rate of surface diffusion Microscopic aspect of wetting Double layer structure on SAM Electron transfer on SAM Also skip some other important techniques: in-situ STM Atomic Force Microscopy FT-IR X-ray diffraction LEED EELS XPS Voltammetry Surface Plasmon Resonance etc
55 Immobilization of of proteins on on SAMs SAMs SAM
56 Selective immobilization of of horse horse heart heart cytochrome c on on MPA MPA domains
57 HRP Selective removal of MPOH domains Refill the space with DTSP
58 AFM HRP HRP
59 D. Hobara, Y. Uno, and T. Kakiuchi, Phys. Chem. Chem. Phys., 3, 3437 (2001).
60
61
62 MD)
63 X
64
65 (N m -1 ) (J m -2 ) > 0 cf. mayonnaise
66 Spontaneous Emulsification Long standing riddle
67
68 Spontaneous emulsification is related to the thermodynamic instability of the interface. Electrochemical Instability
69 Any interface is is more or or less electrified. Oil Water Surface charge Alignment of dipoles Phase-boundary potential
70 Electrified Interfaces Electrocapillary equation : excess surface charge density : potential drop across the interface
71 Violation of the stability condition Electrochemical Instability
72 Stability is externally controllable. Instability window Counterintuitive! pzc
73 Electrochemical instability can explain the potential-dependent chaotic current and predicts a certain regularity in the process.
74 DCE W + dodecanesulfonate
75 W dodecanesulfonate DCE
76
77
78
79 R-S-Au?! R-SH + Au = R-S-Au + H + OK? R-SH + Au{ } = R-S-Au { } + H + + e - (Au{ } ) W.K. Paik, (1998) OK? R-SH H + H + H + H + H + OK? Au H Au e- Le Chatelier s principle OK?
80
81
82 A4 A4
83
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