Yukihiro Ozaki, Katrin Kneipp, Ricardo Aroca
Frontiers of Surface-Enhanced Raman Scattering
Single Nanoparticles and Single Cells
Yukihiro Ozaki, Katrin Kneipp, Ricardo Aroca
Frontiers of Surface-Enhanced Raman Scattering
Single Nanoparticles and Single Cells
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A comprehensive presentation of Surface-Enhanced Raman Scattering (SERS) theory, substrate fabrication, applications of SERS to biosystems, chemical analysis, sensing and fundamental innovation through experimentation. Written by internationally recognized editors and contributors.
Relevant to all those within the scientific community dealing with Raman Spectroscopy, i.e. physicists, chemists, biologists, material scientists, physicians and biomedical scientists.
SERS applications are widely expanding and the technology is now used in the field of nanotechnologies, applications to biosystems, nonosensors, nanoimaging and nanoscience.…mehr
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A comprehensive presentation of Surface-Enhanced Raman Scattering (SERS) theory, substrate fabrication, applications of SERS to biosystems, chemical analysis, sensing and fundamental innovation through experimentation. Written by internationally recognized editors and contributors.
Relevant to all those within the scientific community dealing with Raman Spectroscopy, i.e. physicists, chemists, biologists, material scientists, physicians and biomedical scientists.
SERS applications are widely expanding and the technology is now used in the field of nanotechnologies, applications to biosystems, nonosensors, nanoimaging and nanoscience.
Relevant to all those within the scientific community dealing with Raman Spectroscopy, i.e. physicists, chemists, biologists, material scientists, physicians and biomedical scientists.
SERS applications are widely expanding and the technology is now used in the field of nanotechnologies, applications to biosystems, nonosensors, nanoimaging and nanoscience.
Produktdetails
- Produktdetails
- Verlag: Wiley & Sons
- 1. Auflage
- Seitenzahl: 336
- Erscheinungstermin: 31. März 2014
- Englisch
- Abmessung: 244mm x 165mm x 23mm
- Gewicht: 666g
- ISBN-13: 9781118359020
- ISBN-10: 111835902X
- Artikelnr.: 40552984
- Verlag: Wiley & Sons
- 1. Auflage
- Seitenzahl: 336
- Erscheinungstermin: 31. März 2014
- Englisch
- Abmessung: 244mm x 165mm x 23mm
- Gewicht: 666g
- ISBN-13: 9781118359020
- ISBN-10: 111835902X
- Artikelnr.: 40552984
EDITORS YUKIHIRO OZAKI, School of Science & Technology, Kwansei Gakuin University, Japan KATRIN KNEIPP, Department of Physics, Technical University of Denmark, Denmark RICARDO AROCA, Department of Chemistry & Biochemistry, University of Windsor, Canada
List of Contributors xi Preface xv 1. Calculation of Surface-Enhanced Raman
Spectra Including Orientational and Stokes Effects Using TDDFT/Mie Theory
QM/ED Method 1 George C. Schatz and Nicholas A. Valley 1.1 Introduction:
Combined Quantum Mechanics/Electrodynamics Methods 1 1.2 Computational
Details 3 1.3 Summary of Model Systems 4 1.4 Azimuthal Averaging 5 1.5 SERS
of Pyridine: Models G, A, B, S, and V 6 1.6 Orientation Effects in SERS of
Phthalocyanines 11 1.7 Two Particle QM/ED Calculations 13 1.8 Summary 15
Acknowledgment 16 References 16 2. Non-resonant SERS Using the Hottest Hot
Spots of Plasmonic Nanoaggregates 19 Katrin Kneipp and Harald Kneipp 2.1
Introduction 19 2.2 Aggregates of Silver and Gold Nanoparticles and Their
Hot Spots 21 2.2.1 Evaluation of Plasmonic Nanoaggregates by Vibrational
Pumping due to a Non-resonant SERS Process 21 2.2.2 Probing Plasmonic
Nanoaggregates by Electron Energy Loss Spectroscopy 24 2.2.3 Probing Local
Fields in Hot Spots by SERS and SEHRS 25 2.3 SERS Using Hot Silver
Nanoaggregates and Non-resonant NIR Excitation 26 2.3.1 SERS Signal vs.
Concentration of the Target Molecule 26 2.3.2 Spectroscopic Potential of
Non-resonant SERS Using the Hottest Hot Spots 30 2.4 Summary and
Conclusions 31 References 32 3. Effect of Nanoparticle Symmetry on
Plasmonic Fields: Implications for Single-Molecule Raman Scattering 37 Lev
Chuntonov and Gilad Haran 3.1 Introduction 37 3.2 Methodology 38 3.3
Plasmon Mode Structure of Nanoparticle Clusters 39 3.3.1 Dimers 39 3.3.2
Trimers 40 3.4 Effect of Plasmon Modes on SMSERS 47 3.4.1 Effect of the
Spectral Lineshape 47 3.4.2 Effect of Multiple Normal Modes 49 3.5
Conclusions 54 Acknowledgment 54 References 54 4. Experimental
Demonstration of Electromagnetic Mechanism of SERS and Quantitative
Analysis of SERS Fluctuation Based on the Mechanism 59 Tamitake Itoh 4.1
Experimental Demonstration of the EM Mechanism of SERS 59 4.1.1
Introduction 59 4.1.2 Observations of the EM Mechanism in SERS Spectral
Variations 60 4.1.3 Observations of the EM Mechanism in the Refractive
Index Dependence of SERS Spectra 62 4.1.4 Quantitative Evaluation of the EM
Mechanism of SERS 64 4.1.5 Summary 72 4.2 Quantitative Analysis of SERS
Fluctuation Based on the EM Mechanism 72 4.2.1 Introduction 72 4.2.2
Intensity and Spectral Fluctuation in SERS and SEF 73 4.2.3 Framework for
Analysis of Fluctuation in SERS and SEF 73 4.2.4 Analysis of Intensity
Fluctuation in SERS and SEF 76 4.2.5 Analysis of Spectral Fluctuation in
SERS and SEF 78 4.2.6 Summary 82 4.3 Conclusion 82 Acknowledgments 83
References 83 5. Single-Molecule Surface-Enhanced Raman Scattering as a
Probe for Adsorption Dynamics on Metal Surfaces 89 Mai Takase, Fumika
Nagasawa, Hideki Nabika and Kei Murakoshi 5.1 Introduction 89 5.2
Simultaneous Measurements of Conductance and SERS of a Single-Molecule
Junction 90 5.3 SERS Observation Using Heterometallic Nanodimers at the
Single-Molecule Level 96 5.4 Conclusion 101 Acknowledgments 101 References
101 6. Analysis of Blinking SERS by a Power Law with an Exponential
Function 107 Yasutaka Kitahama and Yukihiro Ozaki 6.1 Introduction 107 6.2
Materials and Methods 110 6.3 Power Law Analysis 110 6.4 Plasmon Resonance
Wavelength Dependence 117 6.4.1 Power Law Exponents for the Bright and Dark
Events 117 6.4.2 Truncation Time for the Dark Events 123 6.5 Energy Density
Dependence 123 6.5.1 Power Law Exponents for the Bright and Dark Events 123
6.5.2 Truncation Time for the Dark Events 125 6.5.3 Comparison with Other
Analysis 126 6.6 Temperature Dependence 129 6.6.1 Power Law Exponents for
the Bright and Dark Events 129 6.6.2 Truncation Time for the Dark Events
129 6.6.3 Comparison with Other Analysis 130 6.7 Summary 132
Acknowledgments 132 References 133 7. Tip-Enhanced Raman Spectroscopy
(TERS) for Nanoscale Imaging and Analysis 139 Taka-aki Yano and Satoshi
Kawata 7.1 Crucial Difference between TERS and SERS 139 7.2 TERS-Specific
Spectral Change as a Function of Tip-Sample Distance 141 7.3 Mechanical
Effect in TERS 143 7.4 Application to Analytical Nano-Imaging 144 7.5
Metallic Probe Tip: Design and Fabrication 149 7.6 Spatial Resolution 154
7.7 Real-Time and 3D Imaging: Perspectives 155 References 156 8.
Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy (SHINERS) 163
Jian-Feng Li and Zhong-Qun Tian 8.1 Introduction 163 8.2 Synthesis of
Various Shell-Isolated Nanoparticles (SHINs) 167 8.3 Characterizations of
SHINs 169 8.3.1 Correlation of the SHINERS Intensity and Shell Thickness
169 8.3.2 Characterization of the Ultra-Thin Uniform Silica Shell 171 8.3.3
Influence of the SHINs on the Surface 172 8.4 Applications of SHINERS 173
8.4.1 Single-Crystal Electrode Surface 173 8.4.2 Non-Metallic Material
Surfaces 175 8.4.3 Single Particle SHINERS 178 8.5 Different Strategies of
SHINERS Compared to Previous SERS Works Using Core-Shell or Overlayer
Structures 178 8.6 Advantages of Isolated Mode over Contact Mode 180 8.7
Concluding Discussion 184 8.8 Outlook 185 Acknowledgments 186 References
186 9. Applying Super-Resolution Imaging Techniques to Problems in
Single-Molecule SERS 193 Eric J. Titus and Katherine A. Willets 9.1
Introduction 193 9.1.1 Single-Molecule Surface-Enhanced Raman Scattering
(SM-SERS) 193 9.1.2 Super-Resolution Imaging 194 9.2 Experimental
Considerations for Super-Resolution SM-SERS 195 9.2.1 Sample Preparation
195 9.2.2 Instrument Set-up 196 9.2.3 Camera Pixels and Theoretical
Uncertainties 197 9.2.4 Correlated Imaging and Spectroscopy in
Super-Resolution SM-SERS 198 9.2.5 Correlated Optical and Structural Data
199 9.3 Super-Resolution SM-SERS Analysis 200 9.3.1 Mechanical Drift
Correction 201 9.3.2 Analysis of Background Nanoparticle Luminescence 202
9.3.3 Calculating the SM-SERS Centroid Position 202 9.4 Super-Resolution
SM-SERS Examples 204 9.4.1 Mapping SM-SERS Hot Spots 204 9.4.2 The Role of
Plasmon-Enhanced Electromagnetic Fields: Structure Correlation Studies 206
9.4.3 The Role of the Molecule: Isotope-Edited Studies 210 9.5 Conclusions
214 References 214 10. Lithographically-Fabricated SERS Substrates: Double
Resonances, Nanogaps, and Beamed Emission 219 Kenneth B. Crozier, Wenqi
Zhu, Yizhuo Chu, Dongxing Wang and Mohamad Banaee 10.1 Introduction 219
10.2 Double Resonance SERS Substrates 220 10.3 Lithographically-Fabricated
Nanogap Dimers 226 10.4 Beamed Raman Scattering 229 10.5 Conclusions 238
References 239 11. Plasmon-Enhanced Scattering and Fluorescence Used for
Ultrasensitive Detection in Langmuir-Blodgett Monolayers 243 Diogo Volpati,
Aisha Alsaleh, Carlos J. L. Constantino and Ricardo F. Aroca 11.1
Introduction 243 11.2 Surface-Enhanced Resonance Raman Scattering of Tagged
Phospholipids 245 11.2.1 Experimental Details 245 11.2.2 Langmuir and LB
films 246 11.2.3 Electronic Absorption 247 11.2.4 Characteristic
Vibrational Modes of the Tagged Phospholipid 248 11.2.5 Single Molecule
Detection 250 11.3 Shell-Isolated Nanoparticle Enhanced Fluorescence
(SHINEF) 251 11.3.1 Tuning the Enhancement Factor in SHINEF 251 11.3.2
SHINEF of Fluorescein-DHPE 253 11.4 Conclusions 254 Acknowledgments 255
References 255 12. SERS Analysis of Bacteria, Human Blood, and Cancer
Cells: a Metabolomic and Diagnostic Tool 257 W. Ranjith Premasiri, Paul
Lemler, Ying Chen, Yoseph Gebregziabher and Lawrence D. Ziegler 12.1
Introduction 257 12.2 SERS of Bacterial Cells: Methodology and Diagnostics
258 12.3 Characteristics of SERS Spectra of Bacteria 261 12.4 PCA Barcode
Analysis 263 12.5 Biological Origins of Bacterial SERS Signatures 265 12.6
SERS Bacterial Identification in Human Body Fluids: Bacteremia and UTI
Diagnostics 266 12.7 Red Blood Cells and Hemoglobin: Blood Aging and
Disease Detection 267 12.8 SERS of Whole Blood 269 12.9 SERS of RBCs 271
12.10 Malaria Detection 273 12.11 Cancer Cell Detection: Metabolic
Profiling by SERS 273 12.12 Conclusions 276 Acknowledgment 277 References
277 13. SERS in Cells: from Concepts to Practical Applications 285 Janina
Kneipp and Daniela Drescher 13.1 Introduction 285 13.2 SERS Labels and SERS
Nanoprobes: Different Approaches to Obtain Different Information 286 13.2.1
Highlighting Cellular Substructures with SERS Labels 286 13.2.2 Probing
Intrinsic Cellular Biochemistry with SERS Nanoprobes 288 13.3 Consequences
of Endocytotic Uptake and Processing for Intrinsic SERS Probing in Cells
289 13.4 Quantification of Metal Nanoparticles in Cells 292 13.5 Toxicity
Considerations 295 13.6 Applications 298 13.6.1 pH Nanosensors for Studies
in Live Cells 298 13.6.2 Following Cell Division with SERS 299
Acknowledgment 301 References 301 Index 309
Spectra Including Orientational and Stokes Effects Using TDDFT/Mie Theory
QM/ED Method 1 George C. Schatz and Nicholas A. Valley 1.1 Introduction:
Combined Quantum Mechanics/Electrodynamics Methods 1 1.2 Computational
Details 3 1.3 Summary of Model Systems 4 1.4 Azimuthal Averaging 5 1.5 SERS
of Pyridine: Models G, A, B, S, and V 6 1.6 Orientation Effects in SERS of
Phthalocyanines 11 1.7 Two Particle QM/ED Calculations 13 1.8 Summary 15
Acknowledgment 16 References 16 2. Non-resonant SERS Using the Hottest Hot
Spots of Plasmonic Nanoaggregates 19 Katrin Kneipp and Harald Kneipp 2.1
Introduction 19 2.2 Aggregates of Silver and Gold Nanoparticles and Their
Hot Spots 21 2.2.1 Evaluation of Plasmonic Nanoaggregates by Vibrational
Pumping due to a Non-resonant SERS Process 21 2.2.2 Probing Plasmonic
Nanoaggregates by Electron Energy Loss Spectroscopy 24 2.2.3 Probing Local
Fields in Hot Spots by SERS and SEHRS 25 2.3 SERS Using Hot Silver
Nanoaggregates and Non-resonant NIR Excitation 26 2.3.1 SERS Signal vs.
Concentration of the Target Molecule 26 2.3.2 Spectroscopic Potential of
Non-resonant SERS Using the Hottest Hot Spots 30 2.4 Summary and
Conclusions 31 References 32 3. Effect of Nanoparticle Symmetry on
Plasmonic Fields: Implications for Single-Molecule Raman Scattering 37 Lev
Chuntonov and Gilad Haran 3.1 Introduction 37 3.2 Methodology 38 3.3
Plasmon Mode Structure of Nanoparticle Clusters 39 3.3.1 Dimers 39 3.3.2
Trimers 40 3.4 Effect of Plasmon Modes on SMSERS 47 3.4.1 Effect of the
Spectral Lineshape 47 3.4.2 Effect of Multiple Normal Modes 49 3.5
Conclusions 54 Acknowledgment 54 References 54 4. Experimental
Demonstration of Electromagnetic Mechanism of SERS and Quantitative
Analysis of SERS Fluctuation Based on the Mechanism 59 Tamitake Itoh 4.1
Experimental Demonstration of the EM Mechanism of SERS 59 4.1.1
Introduction 59 4.1.2 Observations of the EM Mechanism in SERS Spectral
Variations 60 4.1.3 Observations of the EM Mechanism in the Refractive
Index Dependence of SERS Spectra 62 4.1.4 Quantitative Evaluation of the EM
Mechanism of SERS 64 4.1.5 Summary 72 4.2 Quantitative Analysis of SERS
Fluctuation Based on the EM Mechanism 72 4.2.1 Introduction 72 4.2.2
Intensity and Spectral Fluctuation in SERS and SEF 73 4.2.3 Framework for
Analysis of Fluctuation in SERS and SEF 73 4.2.4 Analysis of Intensity
Fluctuation in SERS and SEF 76 4.2.5 Analysis of Spectral Fluctuation in
SERS and SEF 78 4.2.6 Summary 82 4.3 Conclusion 82 Acknowledgments 83
References 83 5. Single-Molecule Surface-Enhanced Raman Scattering as a
Probe for Adsorption Dynamics on Metal Surfaces 89 Mai Takase, Fumika
Nagasawa, Hideki Nabika and Kei Murakoshi 5.1 Introduction 89 5.2
Simultaneous Measurements of Conductance and SERS of a Single-Molecule
Junction 90 5.3 SERS Observation Using Heterometallic Nanodimers at the
Single-Molecule Level 96 5.4 Conclusion 101 Acknowledgments 101 References
101 6. Analysis of Blinking SERS by a Power Law with an Exponential
Function 107 Yasutaka Kitahama and Yukihiro Ozaki 6.1 Introduction 107 6.2
Materials and Methods 110 6.3 Power Law Analysis 110 6.4 Plasmon Resonance
Wavelength Dependence 117 6.4.1 Power Law Exponents for the Bright and Dark
Events 117 6.4.2 Truncation Time for the Dark Events 123 6.5 Energy Density
Dependence 123 6.5.1 Power Law Exponents for the Bright and Dark Events 123
6.5.2 Truncation Time for the Dark Events 125 6.5.3 Comparison with Other
Analysis 126 6.6 Temperature Dependence 129 6.6.1 Power Law Exponents for
the Bright and Dark Events 129 6.6.2 Truncation Time for the Dark Events
129 6.6.3 Comparison with Other Analysis 130 6.7 Summary 132
Acknowledgments 132 References 133 7. Tip-Enhanced Raman Spectroscopy
(TERS) for Nanoscale Imaging and Analysis 139 Taka-aki Yano and Satoshi
Kawata 7.1 Crucial Difference between TERS and SERS 139 7.2 TERS-Specific
Spectral Change as a Function of Tip-Sample Distance 141 7.3 Mechanical
Effect in TERS 143 7.4 Application to Analytical Nano-Imaging 144 7.5
Metallic Probe Tip: Design and Fabrication 149 7.6 Spatial Resolution 154
7.7 Real-Time and 3D Imaging: Perspectives 155 References 156 8.
Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy (SHINERS) 163
Jian-Feng Li and Zhong-Qun Tian 8.1 Introduction 163 8.2 Synthesis of
Various Shell-Isolated Nanoparticles (SHINs) 167 8.3 Characterizations of
SHINs 169 8.3.1 Correlation of the SHINERS Intensity and Shell Thickness
169 8.3.2 Characterization of the Ultra-Thin Uniform Silica Shell 171 8.3.3
Influence of the SHINs on the Surface 172 8.4 Applications of SHINERS 173
8.4.1 Single-Crystal Electrode Surface 173 8.4.2 Non-Metallic Material
Surfaces 175 8.4.3 Single Particle SHINERS 178 8.5 Different Strategies of
SHINERS Compared to Previous SERS Works Using Core-Shell or Overlayer
Structures 178 8.6 Advantages of Isolated Mode over Contact Mode 180 8.7
Concluding Discussion 184 8.8 Outlook 185 Acknowledgments 186 References
186 9. Applying Super-Resolution Imaging Techniques to Problems in
Single-Molecule SERS 193 Eric J. Titus and Katherine A. Willets 9.1
Introduction 193 9.1.1 Single-Molecule Surface-Enhanced Raman Scattering
(SM-SERS) 193 9.1.2 Super-Resolution Imaging 194 9.2 Experimental
Considerations for Super-Resolution SM-SERS 195 9.2.1 Sample Preparation
195 9.2.2 Instrument Set-up 196 9.2.3 Camera Pixels and Theoretical
Uncertainties 197 9.2.4 Correlated Imaging and Spectroscopy in
Super-Resolution SM-SERS 198 9.2.5 Correlated Optical and Structural Data
199 9.3 Super-Resolution SM-SERS Analysis 200 9.3.1 Mechanical Drift
Correction 201 9.3.2 Analysis of Background Nanoparticle Luminescence 202
9.3.3 Calculating the SM-SERS Centroid Position 202 9.4 Super-Resolution
SM-SERS Examples 204 9.4.1 Mapping SM-SERS Hot Spots 204 9.4.2 The Role of
Plasmon-Enhanced Electromagnetic Fields: Structure Correlation Studies 206
9.4.3 The Role of the Molecule: Isotope-Edited Studies 210 9.5 Conclusions
214 References 214 10. Lithographically-Fabricated SERS Substrates: Double
Resonances, Nanogaps, and Beamed Emission 219 Kenneth B. Crozier, Wenqi
Zhu, Yizhuo Chu, Dongxing Wang and Mohamad Banaee 10.1 Introduction 219
10.2 Double Resonance SERS Substrates 220 10.3 Lithographically-Fabricated
Nanogap Dimers 226 10.4 Beamed Raman Scattering 229 10.5 Conclusions 238
References 239 11. Plasmon-Enhanced Scattering and Fluorescence Used for
Ultrasensitive Detection in Langmuir-Blodgett Monolayers 243 Diogo Volpati,
Aisha Alsaleh, Carlos J. L. Constantino and Ricardo F. Aroca 11.1
Introduction 243 11.2 Surface-Enhanced Resonance Raman Scattering of Tagged
Phospholipids 245 11.2.1 Experimental Details 245 11.2.2 Langmuir and LB
films 246 11.2.3 Electronic Absorption 247 11.2.4 Characteristic
Vibrational Modes of the Tagged Phospholipid 248 11.2.5 Single Molecule
Detection 250 11.3 Shell-Isolated Nanoparticle Enhanced Fluorescence
(SHINEF) 251 11.3.1 Tuning the Enhancement Factor in SHINEF 251 11.3.2
SHINEF of Fluorescein-DHPE 253 11.4 Conclusions 254 Acknowledgments 255
References 255 12. SERS Analysis of Bacteria, Human Blood, and Cancer
Cells: a Metabolomic and Diagnostic Tool 257 W. Ranjith Premasiri, Paul
Lemler, Ying Chen, Yoseph Gebregziabher and Lawrence D. Ziegler 12.1
Introduction 257 12.2 SERS of Bacterial Cells: Methodology and Diagnostics
258 12.3 Characteristics of SERS Spectra of Bacteria 261 12.4 PCA Barcode
Analysis 263 12.5 Biological Origins of Bacterial SERS Signatures 265 12.6
SERS Bacterial Identification in Human Body Fluids: Bacteremia and UTI
Diagnostics 266 12.7 Red Blood Cells and Hemoglobin: Blood Aging and
Disease Detection 267 12.8 SERS of Whole Blood 269 12.9 SERS of RBCs 271
12.10 Malaria Detection 273 12.11 Cancer Cell Detection: Metabolic
Profiling by SERS 273 12.12 Conclusions 276 Acknowledgment 277 References
277 13. SERS in Cells: from Concepts to Practical Applications 285 Janina
Kneipp and Daniela Drescher 13.1 Introduction 285 13.2 SERS Labels and SERS
Nanoprobes: Different Approaches to Obtain Different Information 286 13.2.1
Highlighting Cellular Substructures with SERS Labels 286 13.2.2 Probing
Intrinsic Cellular Biochemistry with SERS Nanoprobes 288 13.3 Consequences
of Endocytotic Uptake and Processing for Intrinsic SERS Probing in Cells
289 13.4 Quantification of Metal Nanoparticles in Cells 292 13.5 Toxicity
Considerations 295 13.6 Applications 298 13.6.1 pH Nanosensors for Studies
in Live Cells 298 13.6.2 Following Cell Division with SERS 299
Acknowledgment 301 References 301 Index 309
List of Contributors xi Preface xv 1. Calculation of Surface-Enhanced Raman
Spectra Including Orientational and Stokes Effects Using TDDFT/Mie Theory
QM/ED Method 1 George C. Schatz and Nicholas A. Valley 1.1 Introduction:
Combined Quantum Mechanics/Electrodynamics Methods 1 1.2 Computational
Details 3 1.3 Summary of Model Systems 4 1.4 Azimuthal Averaging 5 1.5 SERS
of Pyridine: Models G, A, B, S, and V 6 1.6 Orientation Effects in SERS of
Phthalocyanines 11 1.7 Two Particle QM/ED Calculations 13 1.8 Summary 15
Acknowledgment 16 References 16 2. Non-resonant SERS Using the Hottest Hot
Spots of Plasmonic Nanoaggregates 19 Katrin Kneipp and Harald Kneipp 2.1
Introduction 19 2.2 Aggregates of Silver and Gold Nanoparticles and Their
Hot Spots 21 2.2.1 Evaluation of Plasmonic Nanoaggregates by Vibrational
Pumping due to a Non-resonant SERS Process 21 2.2.2 Probing Plasmonic
Nanoaggregates by Electron Energy Loss Spectroscopy 24 2.2.3 Probing Local
Fields in Hot Spots by SERS and SEHRS 25 2.3 SERS Using Hot Silver
Nanoaggregates and Non-resonant NIR Excitation 26 2.3.1 SERS Signal vs.
Concentration of the Target Molecule 26 2.3.2 Spectroscopic Potential of
Non-resonant SERS Using the Hottest Hot Spots 30 2.4 Summary and
Conclusions 31 References 32 3. Effect of Nanoparticle Symmetry on
Plasmonic Fields: Implications for Single-Molecule Raman Scattering 37 Lev
Chuntonov and Gilad Haran 3.1 Introduction 37 3.2 Methodology 38 3.3
Plasmon Mode Structure of Nanoparticle Clusters 39 3.3.1 Dimers 39 3.3.2
Trimers 40 3.4 Effect of Plasmon Modes on SMSERS 47 3.4.1 Effect of the
Spectral Lineshape 47 3.4.2 Effect of Multiple Normal Modes 49 3.5
Conclusions 54 Acknowledgment 54 References 54 4. Experimental
Demonstration of Electromagnetic Mechanism of SERS and Quantitative
Analysis of SERS Fluctuation Based on the Mechanism 59 Tamitake Itoh 4.1
Experimental Demonstration of the EM Mechanism of SERS 59 4.1.1
Introduction 59 4.1.2 Observations of the EM Mechanism in SERS Spectral
Variations 60 4.1.3 Observations of the EM Mechanism in the Refractive
Index Dependence of SERS Spectra 62 4.1.4 Quantitative Evaluation of the EM
Mechanism of SERS 64 4.1.5 Summary 72 4.2 Quantitative Analysis of SERS
Fluctuation Based on the EM Mechanism 72 4.2.1 Introduction 72 4.2.2
Intensity and Spectral Fluctuation in SERS and SEF 73 4.2.3 Framework for
Analysis of Fluctuation in SERS and SEF 73 4.2.4 Analysis of Intensity
Fluctuation in SERS and SEF 76 4.2.5 Analysis of Spectral Fluctuation in
SERS and SEF 78 4.2.6 Summary 82 4.3 Conclusion 82 Acknowledgments 83
References 83 5. Single-Molecule Surface-Enhanced Raman Scattering as a
Probe for Adsorption Dynamics on Metal Surfaces 89 Mai Takase, Fumika
Nagasawa, Hideki Nabika and Kei Murakoshi 5.1 Introduction 89 5.2
Simultaneous Measurements of Conductance and SERS of a Single-Molecule
Junction 90 5.3 SERS Observation Using Heterometallic Nanodimers at the
Single-Molecule Level 96 5.4 Conclusion 101 Acknowledgments 101 References
101 6. Analysis of Blinking SERS by a Power Law with an Exponential
Function 107 Yasutaka Kitahama and Yukihiro Ozaki 6.1 Introduction 107 6.2
Materials and Methods 110 6.3 Power Law Analysis 110 6.4 Plasmon Resonance
Wavelength Dependence 117 6.4.1 Power Law Exponents for the Bright and Dark
Events 117 6.4.2 Truncation Time for the Dark Events 123 6.5 Energy Density
Dependence 123 6.5.1 Power Law Exponents for the Bright and Dark Events 123
6.5.2 Truncation Time for the Dark Events 125 6.5.3 Comparison with Other
Analysis 126 6.6 Temperature Dependence 129 6.6.1 Power Law Exponents for
the Bright and Dark Events 129 6.6.2 Truncation Time for the Dark Events
129 6.6.3 Comparison with Other Analysis 130 6.7 Summary 132
Acknowledgments 132 References 133 7. Tip-Enhanced Raman Spectroscopy
(TERS) for Nanoscale Imaging and Analysis 139 Taka-aki Yano and Satoshi
Kawata 7.1 Crucial Difference between TERS and SERS 139 7.2 TERS-Specific
Spectral Change as a Function of Tip-Sample Distance 141 7.3 Mechanical
Effect in TERS 143 7.4 Application to Analytical Nano-Imaging 144 7.5
Metallic Probe Tip: Design and Fabrication 149 7.6 Spatial Resolution 154
7.7 Real-Time and 3D Imaging: Perspectives 155 References 156 8.
Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy (SHINERS) 163
Jian-Feng Li and Zhong-Qun Tian 8.1 Introduction 163 8.2 Synthesis of
Various Shell-Isolated Nanoparticles (SHINs) 167 8.3 Characterizations of
SHINs 169 8.3.1 Correlation of the SHINERS Intensity and Shell Thickness
169 8.3.2 Characterization of the Ultra-Thin Uniform Silica Shell 171 8.3.3
Influence of the SHINs on the Surface 172 8.4 Applications of SHINERS 173
8.4.1 Single-Crystal Electrode Surface 173 8.4.2 Non-Metallic Material
Surfaces 175 8.4.3 Single Particle SHINERS 178 8.5 Different Strategies of
SHINERS Compared to Previous SERS Works Using Core-Shell or Overlayer
Structures 178 8.6 Advantages of Isolated Mode over Contact Mode 180 8.7
Concluding Discussion 184 8.8 Outlook 185 Acknowledgments 186 References
186 9. Applying Super-Resolution Imaging Techniques to Problems in
Single-Molecule SERS 193 Eric J. Titus and Katherine A. Willets 9.1
Introduction 193 9.1.1 Single-Molecule Surface-Enhanced Raman Scattering
(SM-SERS) 193 9.1.2 Super-Resolution Imaging 194 9.2 Experimental
Considerations for Super-Resolution SM-SERS 195 9.2.1 Sample Preparation
195 9.2.2 Instrument Set-up 196 9.2.3 Camera Pixels and Theoretical
Uncertainties 197 9.2.4 Correlated Imaging and Spectroscopy in
Super-Resolution SM-SERS 198 9.2.5 Correlated Optical and Structural Data
199 9.3 Super-Resolution SM-SERS Analysis 200 9.3.1 Mechanical Drift
Correction 201 9.3.2 Analysis of Background Nanoparticle Luminescence 202
9.3.3 Calculating the SM-SERS Centroid Position 202 9.4 Super-Resolution
SM-SERS Examples 204 9.4.1 Mapping SM-SERS Hot Spots 204 9.4.2 The Role of
Plasmon-Enhanced Electromagnetic Fields: Structure Correlation Studies 206
9.4.3 The Role of the Molecule: Isotope-Edited Studies 210 9.5 Conclusions
214 References 214 10. Lithographically-Fabricated SERS Substrates: Double
Resonances, Nanogaps, and Beamed Emission 219 Kenneth B. Crozier, Wenqi
Zhu, Yizhuo Chu, Dongxing Wang and Mohamad Banaee 10.1 Introduction 219
10.2 Double Resonance SERS Substrates 220 10.3 Lithographically-Fabricated
Nanogap Dimers 226 10.4 Beamed Raman Scattering 229 10.5 Conclusions 238
References 239 11. Plasmon-Enhanced Scattering and Fluorescence Used for
Ultrasensitive Detection in Langmuir-Blodgett Monolayers 243 Diogo Volpati,
Aisha Alsaleh, Carlos J. L. Constantino and Ricardo F. Aroca 11.1
Introduction 243 11.2 Surface-Enhanced Resonance Raman Scattering of Tagged
Phospholipids 245 11.2.1 Experimental Details 245 11.2.2 Langmuir and LB
films 246 11.2.3 Electronic Absorption 247 11.2.4 Characteristic
Vibrational Modes of the Tagged Phospholipid 248 11.2.5 Single Molecule
Detection 250 11.3 Shell-Isolated Nanoparticle Enhanced Fluorescence
(SHINEF) 251 11.3.1 Tuning the Enhancement Factor in SHINEF 251 11.3.2
SHINEF of Fluorescein-DHPE 253 11.4 Conclusions 254 Acknowledgments 255
References 255 12. SERS Analysis of Bacteria, Human Blood, and Cancer
Cells: a Metabolomic and Diagnostic Tool 257 W. Ranjith Premasiri, Paul
Lemler, Ying Chen, Yoseph Gebregziabher and Lawrence D. Ziegler 12.1
Introduction 257 12.2 SERS of Bacterial Cells: Methodology and Diagnostics
258 12.3 Characteristics of SERS Spectra of Bacteria 261 12.4 PCA Barcode
Analysis 263 12.5 Biological Origins of Bacterial SERS Signatures 265 12.6
SERS Bacterial Identification in Human Body Fluids: Bacteremia and UTI
Diagnostics 266 12.7 Red Blood Cells and Hemoglobin: Blood Aging and
Disease Detection 267 12.8 SERS of Whole Blood 269 12.9 SERS of RBCs 271
12.10 Malaria Detection 273 12.11 Cancer Cell Detection: Metabolic
Profiling by SERS 273 12.12 Conclusions 276 Acknowledgment 277 References
277 13. SERS in Cells: from Concepts to Practical Applications 285 Janina
Kneipp and Daniela Drescher 13.1 Introduction 285 13.2 SERS Labels and SERS
Nanoprobes: Different Approaches to Obtain Different Information 286 13.2.1
Highlighting Cellular Substructures with SERS Labels 286 13.2.2 Probing
Intrinsic Cellular Biochemistry with SERS Nanoprobes 288 13.3 Consequences
of Endocytotic Uptake and Processing for Intrinsic SERS Probing in Cells
289 13.4 Quantification of Metal Nanoparticles in Cells 292 13.5 Toxicity
Considerations 295 13.6 Applications 298 13.6.1 pH Nanosensors for Studies
in Live Cells 298 13.6.2 Following Cell Division with SERS 299
Acknowledgment 301 References 301 Index 309
Spectra Including Orientational and Stokes Effects Using TDDFT/Mie Theory
QM/ED Method 1 George C. Schatz and Nicholas A. Valley 1.1 Introduction:
Combined Quantum Mechanics/Electrodynamics Methods 1 1.2 Computational
Details 3 1.3 Summary of Model Systems 4 1.4 Azimuthal Averaging 5 1.5 SERS
of Pyridine: Models G, A, B, S, and V 6 1.6 Orientation Effects in SERS of
Phthalocyanines 11 1.7 Two Particle QM/ED Calculations 13 1.8 Summary 15
Acknowledgment 16 References 16 2. Non-resonant SERS Using the Hottest Hot
Spots of Plasmonic Nanoaggregates 19 Katrin Kneipp and Harald Kneipp 2.1
Introduction 19 2.2 Aggregates of Silver and Gold Nanoparticles and Their
Hot Spots 21 2.2.1 Evaluation of Plasmonic Nanoaggregates by Vibrational
Pumping due to a Non-resonant SERS Process 21 2.2.2 Probing Plasmonic
Nanoaggregates by Electron Energy Loss Spectroscopy 24 2.2.3 Probing Local
Fields in Hot Spots by SERS and SEHRS 25 2.3 SERS Using Hot Silver
Nanoaggregates and Non-resonant NIR Excitation 26 2.3.1 SERS Signal vs.
Concentration of the Target Molecule 26 2.3.2 Spectroscopic Potential of
Non-resonant SERS Using the Hottest Hot Spots 30 2.4 Summary and
Conclusions 31 References 32 3. Effect of Nanoparticle Symmetry on
Plasmonic Fields: Implications for Single-Molecule Raman Scattering 37 Lev
Chuntonov and Gilad Haran 3.1 Introduction 37 3.2 Methodology 38 3.3
Plasmon Mode Structure of Nanoparticle Clusters 39 3.3.1 Dimers 39 3.3.2
Trimers 40 3.4 Effect of Plasmon Modes on SMSERS 47 3.4.1 Effect of the
Spectral Lineshape 47 3.4.2 Effect of Multiple Normal Modes 49 3.5
Conclusions 54 Acknowledgment 54 References 54 4. Experimental
Demonstration of Electromagnetic Mechanism of SERS and Quantitative
Analysis of SERS Fluctuation Based on the Mechanism 59 Tamitake Itoh 4.1
Experimental Demonstration of the EM Mechanism of SERS 59 4.1.1
Introduction 59 4.1.2 Observations of the EM Mechanism in SERS Spectral
Variations 60 4.1.3 Observations of the EM Mechanism in the Refractive
Index Dependence of SERS Spectra 62 4.1.4 Quantitative Evaluation of the EM
Mechanism of SERS 64 4.1.5 Summary 72 4.2 Quantitative Analysis of SERS
Fluctuation Based on the EM Mechanism 72 4.2.1 Introduction 72 4.2.2
Intensity and Spectral Fluctuation in SERS and SEF 73 4.2.3 Framework for
Analysis of Fluctuation in SERS and SEF 73 4.2.4 Analysis of Intensity
Fluctuation in SERS and SEF 76 4.2.5 Analysis of Spectral Fluctuation in
SERS and SEF 78 4.2.6 Summary 82 4.3 Conclusion 82 Acknowledgments 83
References 83 5. Single-Molecule Surface-Enhanced Raman Scattering as a
Probe for Adsorption Dynamics on Metal Surfaces 89 Mai Takase, Fumika
Nagasawa, Hideki Nabika and Kei Murakoshi 5.1 Introduction 89 5.2
Simultaneous Measurements of Conductance and SERS of a Single-Molecule
Junction 90 5.3 SERS Observation Using Heterometallic Nanodimers at the
Single-Molecule Level 96 5.4 Conclusion 101 Acknowledgments 101 References
101 6. Analysis of Blinking SERS by a Power Law with an Exponential
Function 107 Yasutaka Kitahama and Yukihiro Ozaki 6.1 Introduction 107 6.2
Materials and Methods 110 6.3 Power Law Analysis 110 6.4 Plasmon Resonance
Wavelength Dependence 117 6.4.1 Power Law Exponents for the Bright and Dark
Events 117 6.4.2 Truncation Time for the Dark Events 123 6.5 Energy Density
Dependence 123 6.5.1 Power Law Exponents for the Bright and Dark Events 123
6.5.2 Truncation Time for the Dark Events 125 6.5.3 Comparison with Other
Analysis 126 6.6 Temperature Dependence 129 6.6.1 Power Law Exponents for
the Bright and Dark Events 129 6.6.2 Truncation Time for the Dark Events
129 6.6.3 Comparison with Other Analysis 130 6.7 Summary 132
Acknowledgments 132 References 133 7. Tip-Enhanced Raman Spectroscopy
(TERS) for Nanoscale Imaging and Analysis 139 Taka-aki Yano and Satoshi
Kawata 7.1 Crucial Difference between TERS and SERS 139 7.2 TERS-Specific
Spectral Change as a Function of Tip-Sample Distance 141 7.3 Mechanical
Effect in TERS 143 7.4 Application to Analytical Nano-Imaging 144 7.5
Metallic Probe Tip: Design and Fabrication 149 7.6 Spatial Resolution 154
7.7 Real-Time and 3D Imaging: Perspectives 155 References 156 8.
Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy (SHINERS) 163
Jian-Feng Li and Zhong-Qun Tian 8.1 Introduction 163 8.2 Synthesis of
Various Shell-Isolated Nanoparticles (SHINs) 167 8.3 Characterizations of
SHINs 169 8.3.1 Correlation of the SHINERS Intensity and Shell Thickness
169 8.3.2 Characterization of the Ultra-Thin Uniform Silica Shell 171 8.3.3
Influence of the SHINs on the Surface 172 8.4 Applications of SHINERS 173
8.4.1 Single-Crystal Electrode Surface 173 8.4.2 Non-Metallic Material
Surfaces 175 8.4.3 Single Particle SHINERS 178 8.5 Different Strategies of
SHINERS Compared to Previous SERS Works Using Core-Shell or Overlayer
Structures 178 8.6 Advantages of Isolated Mode over Contact Mode 180 8.7
Concluding Discussion 184 8.8 Outlook 185 Acknowledgments 186 References
186 9. Applying Super-Resolution Imaging Techniques to Problems in
Single-Molecule SERS 193 Eric J. Titus and Katherine A. Willets 9.1
Introduction 193 9.1.1 Single-Molecule Surface-Enhanced Raman Scattering
(SM-SERS) 193 9.1.2 Super-Resolution Imaging 194 9.2 Experimental
Considerations for Super-Resolution SM-SERS 195 9.2.1 Sample Preparation
195 9.2.2 Instrument Set-up 196 9.2.3 Camera Pixels and Theoretical
Uncertainties 197 9.2.4 Correlated Imaging and Spectroscopy in
Super-Resolution SM-SERS 198 9.2.5 Correlated Optical and Structural Data
199 9.3 Super-Resolution SM-SERS Analysis 200 9.3.1 Mechanical Drift
Correction 201 9.3.2 Analysis of Background Nanoparticle Luminescence 202
9.3.3 Calculating the SM-SERS Centroid Position 202 9.4 Super-Resolution
SM-SERS Examples 204 9.4.1 Mapping SM-SERS Hot Spots 204 9.4.2 The Role of
Plasmon-Enhanced Electromagnetic Fields: Structure Correlation Studies 206
9.4.3 The Role of the Molecule: Isotope-Edited Studies 210 9.5 Conclusions
214 References 214 10. Lithographically-Fabricated SERS Substrates: Double
Resonances, Nanogaps, and Beamed Emission 219 Kenneth B. Crozier, Wenqi
Zhu, Yizhuo Chu, Dongxing Wang and Mohamad Banaee 10.1 Introduction 219
10.2 Double Resonance SERS Substrates 220 10.3 Lithographically-Fabricated
Nanogap Dimers 226 10.4 Beamed Raman Scattering 229 10.5 Conclusions 238
References 239 11. Plasmon-Enhanced Scattering and Fluorescence Used for
Ultrasensitive Detection in Langmuir-Blodgett Monolayers 243 Diogo Volpati,
Aisha Alsaleh, Carlos J. L. Constantino and Ricardo F. Aroca 11.1
Introduction 243 11.2 Surface-Enhanced Resonance Raman Scattering of Tagged
Phospholipids 245 11.2.1 Experimental Details 245 11.2.2 Langmuir and LB
films 246 11.2.3 Electronic Absorption 247 11.2.4 Characteristic
Vibrational Modes of the Tagged Phospholipid 248 11.2.5 Single Molecule
Detection 250 11.3 Shell-Isolated Nanoparticle Enhanced Fluorescence
(SHINEF) 251 11.3.1 Tuning the Enhancement Factor in SHINEF 251 11.3.2
SHINEF of Fluorescein-DHPE 253 11.4 Conclusions 254 Acknowledgments 255
References 255 12. SERS Analysis of Bacteria, Human Blood, and Cancer
Cells: a Metabolomic and Diagnostic Tool 257 W. Ranjith Premasiri, Paul
Lemler, Ying Chen, Yoseph Gebregziabher and Lawrence D. Ziegler 12.1
Introduction 257 12.2 SERS of Bacterial Cells: Methodology and Diagnostics
258 12.3 Characteristics of SERS Spectra of Bacteria 261 12.4 PCA Barcode
Analysis 263 12.5 Biological Origins of Bacterial SERS Signatures 265 12.6
SERS Bacterial Identification in Human Body Fluids: Bacteremia and UTI
Diagnostics 266 12.7 Red Blood Cells and Hemoglobin: Blood Aging and
Disease Detection 267 12.8 SERS of Whole Blood 269 12.9 SERS of RBCs 271
12.10 Malaria Detection 273 12.11 Cancer Cell Detection: Metabolic
Profiling by SERS 273 12.12 Conclusions 276 Acknowledgment 277 References
277 13. SERS in Cells: from Concepts to Practical Applications 285 Janina
Kneipp and Daniela Drescher 13.1 Introduction 285 13.2 SERS Labels and SERS
Nanoprobes: Different Approaches to Obtain Different Information 286 13.2.1
Highlighting Cellular Substructures with SERS Labels 286 13.2.2 Probing
Intrinsic Cellular Biochemistry with SERS Nanoprobes 288 13.3 Consequences
of Endocytotic Uptake and Processing for Intrinsic SERS Probing in Cells
289 13.4 Quantification of Metal Nanoparticles in Cells 292 13.5 Toxicity
Considerations 295 13.6 Applications 298 13.6.1 pH Nanosensors for Studies
in Live Cells 298 13.6.2 Following Cell Division with SERS 299
Acknowledgment 301 References 301 Index 309