Atomic Scale Coupling of Electromagnetic Radiation to Single Molecules. Wilson Ho University of California, Irvine
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1
2 Atomic Scale Coupling of Electromagnetic Radiation to Single Molecules Wilson Ho University of California, Irvine
3 Surface Photochemistry
4
5 Direct Adsorbate Excitation
6 Photoelectron Mechanism
7 Objective How to achieve atomic scale resolution in probing matter with electromagnetic radiation? Spectroscopy Optical Phenomena
8 Resolution of Optical Spectroscopy
9 Tip-Induced Plasmon Modes ε t Plasmon ε s Plasmon size : dr
10 Combination of Electromagnetic Radiation With Spatial Resolution of the STM
11 Molecules in Double Barrier Junctions The oxide film spacer increases the lifetime of the transient charged molecular state created after electron injection/withdrawal.
12 Single Molecule Electroluminescence
13 Photon Emission from Single Molecules: Zn-Etioporphyrin on Partially Oxidized NiAl(110) Oxide NiAl(110) Zn-Etioporphyrin
14 Zn(II) Etioporphyrin on Al 2 O 3 & NiAl(110)
15 Mechanism of STM-induced Electroluminescence : Step 1
16 Mechanism of STM-induced Electroluminescence : Step 2
17 Mechanism of STM-induced Electroluminescence : Step 3
18 Light collection setup (electroluminescence) Focusing Lens Mirror 2 Collection Lens Sample Spectrometer & hv CCD Camera Mirror 1 Viewport STM Tip Collection Efficiency: 1% UHV chamber
19 Photon Emission From Molecules on Oxide Films
20 Ag tip Ag tip Photon Energy (ev) Wavelength (nm) TIF Ag vs. W Tips Peak Sequence W tip Ag tip Ag tip W tip Photon Count (arb. unit) Peak Energy (ev)
21 Tunneling Electron Induced Single Molecule Fluorescence: Zn-Etioporphyrin
22 Spatial Dependence of Single Molecule Fluorescence
23 Tunneling Electron Induced Single Molecule Fluorescence
24 LUMO & LUMO + 1: MgP
25 TIF Mechanism 2.0 Energy (ev) Tip evbias -4.0 NiAl Vacuum Oxide
26 RF Induced Rectification Current
27
28 STM Apparatus Low temperature (10 K) ultrahigh vacuum STM
29 Origin of Rectification Current ) cos( 2 t V V V J B ω + = +L + + = ) ( cos ) cos( 2 ) ( ) ( t V dv I d t V dv di V I V I J V J V B B B ω ω +K = 2 ) cos(2 1 ) cos( 2 ) ( ) ( t V dv I d t V dv di V I V I J V J V B B B ω ω + L + = + = V B J B J B R B J B dc dv I d V V I V V I V I V V I ) ( ), ( ) ( ), ( V B J J B R dv I d V V V I ), (
30 Spatial Localization of RF Field
31 Double Modulation Vibrational Rectification
32 Vibrational Rectification Current: C 2 D 2 and C 2 H 2 on Cu(001)
33 Vibrational Rectification Microscopy: C 2 D 2 and C 2 H 2 on Cu(001)
34 Rectification of Single Mn Atom
35 Photon Induced Tunneling
36 Single Molecule Electron Transfer
37 Mechanism of Photon-Induced Electron Transfer to a Single Molecule
38 Photon-Induced Electron Transfer Threshold
39 Photon Induced Tunneling
40 Spatial Variations of Electron Transfer within a Single Molecule
41 Ultrafast Optical Spectroscopy with Spatial Resolution of the STM Femtosecond Lasers: Chemistry at the Temporal Limit Scanning Tunneling Microscopes: Chemistry at the Spatial Limit
42 Acknowledgment Past Present Xi Chen Chi Chen Jennifer Gaudioso Ungdon Ham Jae Ryang Hahn Kiyeo Kim Martin Janson Markus Lackinger Lincoln Lauhon Gary Mikaelian Hyojune Lee George Nazin Joonhee Lee Freddy Toledo Ning Liu Xiuwen Tu Niklas Nilius Shiwei Wu Naoki Ogawa Nilay Pradhan Xiaohui Qiu Mohammad Rezaei Christophe Silien Barry Stipe Mitch Wallis Nicolas Lorente Shiwu Gao Mats Persson
43
44 Prospects Instrumentation Development Electron Spin - microwave-rf excitation - T sub-k, B 10 Tesla Zeeman spectroscopy - spin interactions: Kondo, nanomagnetism Laser-STM - simultaneous spatial + temporal limits 1 Å 10 fs - sub-molecular photochemistry, non-linear optics Non-Vacuum Environment - biological systems
45 < 1 K, 9 Tesla UHV STM
46 Mn Chains: 1 to 16 Atoms
47 Spin-Dependent Tunneling
48
49
50
51 Acknowledgment Past Present Jennifer Gaudioso Chi Chen Jae Ryang Hahn Xi Chen Lincoln Lauhon Ungdon Ham Hyojune Lee Martin Janson Joonhee Lee John Karnes Ning Liu Kiyeo Kim Niklas Nilius Markus Lackinger Nilay Pradhan Gary Mikaelian Xiaohui Qiu George Nazin Mohammad Rezaei Naoki Ogawa Christophe Silien Xiuwen Tu Barry Stipe Shiwei Wu Mitch Wallis Nicolas Lorente Shiwu Gao Mats Persson
52 Atomic Scale Photochemistry Wilson Ho University of California, Irvine
53 Photon Emission from molecules on metal surfaces Photon Count (arb. unit) 400 Ag tip/nial Ag tip/znetioi/nial Metal Molecule Wavelength (nm)
54 Tunneling Electron Induced Single Molecule Fluorescence
55 IET vs. Single Molecule Fluorescence: Inelastic Electron Tunneling Fluorescence
56 Inelastic Electron Tunneling Spectroscopy (STM-IETS)
57
58 Frequency Dependence of RF Voltage Across Junction
59 RF Voltage Across STM Junction: VJ
60 Monitoring Photon-Induced Electron Transfer in a Single Molecule
61 Single Molecule Photon Induced Electron Transfer with Sub-Molecular Spatial Resolution
62 Mg-Porphine Orbitals
63 Single Molecule Vibronic States: MgP
64 Neutral and Charged States: MgP
65 Experimental Setup Focusing Lens Mirror 2 Collection Lens Sample Spectrometer & hv CCD Camera Mirror 1 Viewport STM Tip Collection Efficiency: 0.1% UHV chamber
66 Plasmon modes in the STM junction
67 Double Modulation Spectroscopy Modulate RF Signal at ω c f ( t) = 4 1 sin( nωct) π n (Square Wave 1 to +1 at ω c ) n= 1,3,5... f ( t) = sin( n ω t C ) + π n 2 (Square Wave 0 to +1 at ω c ) n= 1,3, = I( t) I0( VB ) I R sin( nωct) + π n= 1,3,5L n 2 (Modulated Current) 2 I1( t) = I R sin( ωct) π (First Harmonic Signal) 2 1 X 1 ( RMS) = I R π 2 (First Harmonic rms Amplitude) = π 1 (Absolute Rectification Current) I R X 2 Lock-in Sensitivity: 1 na/1 V I R 1 pa I 0 (V B ) 1 na
68 Vibrational Rectification: Single 12 C 16 O & 13 C 18 O
69 Single Molecule Photon Induced Electron Transfer
70 Single Molecule Photon Induced Electron Transfer with Sub-Molecular Spatial Resolution
71 Monitoring Photon-Induced Electron Transfer in a Single Molecule
72 Single Molecule Electron Transfer
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