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	Preface	XV
	List of Contributors	XVII
	Polymer Brushes: On the Way to Tailor-Made Surfaces Jürgen Rühe	1
1	Growth of Polymer Molecules at Surfaces: Introductory Remarks	1
2	Coatings: From First Principles to High-Tech Applications	3
3	Surface-Coating Techniques	6
4	Surface-Attached Polymers	10
5	Polymer Brushes: General Features	13
6	Theory of Polymer Brushes	15
7	Synthesis of Polymer Brushes	18
8	Polymer Brushes as Functional Materials	22
9	Microstructured Polymer Brushes	24
10	Surface-Initiated Polymerization: The Overall Picture	28

Part I	Synthesis	33

1	Recent Advances in Polymer Brush Synthesis Anthony M. Granville and William J. Brittain	35
1.1	Introduction	35
1.2	"Grafting To" Synthesis Technique	37
1.3	"Grafting From" Synthesis Technique	41
2	Polymer Brushes by Atom Transfer Radical Polymerization Jeffrey Pyun, Tomasz Kowalewski, and Krzysztof Matyjaszewski	51
2.1	Introduction	51
2.2	Polymer Brushes on Flat Surfaces	52
2.2.1	Controlled ATRP from Flat Surfaces	53
2.2.2	Block Copolymer Brushes on Flat Surfaces	54
2.2.3	Stimuli-Responsive Ultrathin Films from "Grafting To" Approach	55
2.3	Polymer Brushes from Particles	57
2.3.1	Spherical Brushes from Inorganic Colloids	58
2.3.2	Multilayered Core-Shell Colloids	58
2.3.3	Imaging of Individual Spherical Brushes	61
2.3.4	Modification of Carbon Black Fillers	63
2.4	Molecular Brushes	63
2.4.1	Synthesis of Molecular Brushes from Linear Polymeric Macroinitiators	64
2.4.2	Molecular Brushes from Dendritic Macroinitiators	65
3	Polymer Brushes by Atom Transfer Radical Polymerization Initiated from Macroinitiator Synthesized on the Surface Viktor Klep, Bogdan Zdyrko, Yong Liu, and Igor Luzinov	69
3.1	Introduction	69
3.2	Experimental	72
3.3	Results and Discussion	73
3.3.1	Synthesis of Macroinitiator for ATRP	73
3.3.2	ATRP from Macroinitiator	77
4	Synthesis of Polypeptide Brushes Henning Menzel and Peter Witte	87
4.1	Introduction	87
4.2	Preparation of Peptide Brushes by "Grafting To"	88
4.3	Preparation of Peptide Brushes by Grafting From Polymerization	90
4.3.1	Mechanisms of NCA Polymerization	90
4.3.2	Amine-Initiated Grafting From Polymerizations in Solution	93
4.3.3	Other Techniques for Amine-Initiated Grafting From Polymerizations	94
4.4	Preparation of Peptide Brushes by Living Grafting From Polymerization	95
4.4.1	Copolymerization Approach	95
4.4.2	Alloc-Amide Approach	99
5	Bottle Brush Brushes: Ring-Opening Polymerization of Lactide from Poly(hydroxyethyl methacrylate) Surfaces Jong-Bum Kim, Wenxi Huang, Chun Wang, Merlin Bruening, and Gregory L. Baker	105
5.1	Introduction	105
5.2	Synthesis of PHEMA-g-PLA	109
5.3	Conclusions and Implications for Future Studies	114
5.4	Experimental Section	115
5.4.1	Materials	115
5.4.2	Preparation of Monomer Solution and Substrates	115
5.4.3	Ring-Opening Polymerization from PHEMA Surface	115
5.4.4	Analytical Methods	115
6	Preparation of Well-Defined Organic-Inorganic Hybrid Nanostructures using Living Cationic Surface-Initiated Polymerization from Silica Nanoparticles Il-Jin Kim, Su Chen, and Rudolf Faust	119
6.1	Introduction	119
6.2	Experimental Section	120
6.2.1	Materials	120
6.2.2	Characterization	120
6.2.3	Synthesis of Immobilized Macroinitiators	121
6.3	Results and Discussion	122
6.3.1	Living Cationic Surface-Initiated Polymerization of IB from Silica Nanoparticles in the Presence of Sacrificial Free Initiator	122
6.3.2	Living Cationic Surface-Initiated Polymerization of IB from Silica Macroinitiators	125
7	Photoinitiated Polymerization from Self-Assembled Monolayers Daniel J. Dyer, Jianxin Feng, Charles Fivelson, Rituparna Paul, Rolf Schmidt, and Tongfeng Zhao	129
7.1	Introduction	129
7.2	Substrates	131
7.2.1	Silicon, Silica and Glass	131
7.2.2	Planar Gold	131
7.2.3	Nanoparticles	133
7.3	Photoinitiated Radical Polymerization Mechanisms	133
7.3.1	Free Radicals	133
7.3.2	Photosensitizers	134
7.3.3	Photo-Iniferters	135
7.4	Polymerization from AIBN-type SAMs	135
7.4.1	Design and Synthesis	135
7.4.2	Monolayer Characterization	137
7.4.3	Polymerization of Styrene	138
7.5	Conclusions and Future Studies	143
7.6	Experimental	144
7.6.1	Initiator Synthesis	144
7.6.2	Polymerizations	145
7.6.3	Reflection Absorption Infrared Spectroscopy (FT-RAIRS) Measurements	146
7.6.4	Ellipsometry	146
7.6.5	X-Ray Photoelectron Spectroscopy (XPS)	146
7.6.6	Molecular Weight Measurements	147
7.6.7	Molecular Modeling	147
8	Recent Advances in the Synthesis and Rearrangement of Block Copolymer Brushes Stephen G. Boyes, Anthony M. Granville, Marina Baum, Bulent Akgun, Brian K. Mirous, and William J. Brittain	151
8.1	Introduction and Background	151
8.2	Controlled/"Living" Free Radical Polymerization	153
8.2.1	Atom Transfer Radical Polymerization (ATRP)	153
8.3	Synthesis of Block Copolymer Brushes	154
8.3.1	Diblock Copolymer Brushes	154
8.3.2	Triblock Copolymer Brushes	158
8.4	Rearrangement of Block Copolymer Brushes	160
8.4.1	Rearrangement of Diblock Copolymer Brushes	160
9	Surface-Grafted Hyperbranched Polymers Hideharu Mori and Axel H. E. Müller	167
9.1	Introduction	167
9.2	"Grafting To" Approach	170
9.2.1	Synthesis of 2D Hybrids by "Grafting To"	170
9.2.2	Synthesis of 3D Hybrids by "Grafting To"	171
9.3	Multi-Step Grafting Approach	172
9.3.1	"Grafting To-Grafts"	172
9.3.2	"Grafting From-Grafts"	173
9.4	"Grafting From" Approach	173
9.4.1	Synthesis of 2D Hybrids by Surface-Initiated, Self-Condensing Vinyl (Co)polymerization	175
9.4.2	Synthesis of 3D Hybrids by Surface-Initiated Self-Condensing Vinyl (Co)polymerization	178
9.4.3	Theoretical Considerations	181
9.4.4	Other Systems	182

Part II	Characterization	187

10	The Analysis and Characterization of Polymer Brushes: From Flat Surfaces to Nanoparticles Rigoberto C. Advincula	189
10.1	Introduction	190
10.1.1	Polymer Brushes	190
10.1.2	SIP on Flat Surfaces and Particle Substrates	192
10.2	Characterization of Ultrathin Polymer Films and Polymer Brushes	193
10.2.1	Spectroscopy and Optical Techniques	194
10.2.2	Microscopy	195
10.2.3	Other Methods	196
10.3	Investigating Polymer Brush Systems	198
10.3.1	Characterization of the Step-by-Step Procedure	198
10.3.2	Investigating the Different Regimes of Polymer Brush Conformation on Surfaces	199
10.3.3	Investigating Phase Segregation and Formation of Patterns	200
10.3.4	Polymerization Mechanism	201
10.3.5	Patterning Using Nonlithographic Methods	204
10.4	The Importance of Characterizing Particles and Nanoparticles	204
10.5	Characterization and Analysis Methods for Polymer Brushes on Particles	205
10.5.1	In-Situ Investigations on Particles	206
10.5.2	Degrafted Polymers from Particles	208
11	Characterization of Polymer Brushes on Nanoparticle Surfaces Thomas A. P. Seery, Mark Jordi, Rosette Guino, and Dale Huber	213
11.1	Introduction	213
11.2	Experimental	215
11.2.1	Materials	215
11.2.2	Instrumentation	215
11.2.3	Pyrolysis GC-MS	216
11.2.4	Infrared Monitoring of Polymer Formation	216
11.2.5	Synthesis of Alkanethiol-Stabilized Gold Nanoparticles	217
11.2.6	Synthesis of Stober Silica Nanoparticles	218
11.2.7	Synthesis of NCSEOS	218
11.2.8	Synthesis of BCH, NCSEOS, and TMEOS-Coated Nanoparticles	218
11.2.9	Synthesis of TMEOS Silica-Polymer Mixture	219
11.2.10	Synthesis of Silica-Poly(norbornene) Nanocomposites	219
11.2.11	Isolation of Grafted Polymer Chains	220
11.2.12	Polymer Stability Test	220
11.3	Results and Discussion	221
12	Spherical Polyelectrolyte Brushes Matthias Ballauff	231
12.1	Introduction	231
12.2	Synthesis and Characterization	234
12.2.1	Determination of Core Radius R, Contour Length LC, and Grafting Density	234
12.2.2	Titration Curve	235
12.3	Experimental Verification of Theoretical Predictions	236
12.3.1	Confinement of the Counterions	237
12.3.2	Correlation of the Counterions to the Macroion	238
12.4	Flow Behavior	240
12.5	Applications	242
12.5.1	Interaction with Charged Surfaces	242
12.5.2	Interaction with Proteins in Solution	243
13	Weak Polyelectrolyte Brushes: Complex Formation and Multilayer Build-up with Oppositely Charged Polyelectrolytes Rupert Konradi, Haining Zhang, Markus Biesalski, and Jürgen Rühe	249
13.1	Introduction	249
13.2	Synthesis and Data Evaluation	251
13.2.1	Synthesis	251
13.2.2	Multiple-Angle Nulling Ellipsometry	252
13.3	Swelling Behavior of Weak Polyelectrolyte Brushes in Aqueous Environments	253
13.3.1	The Influence of pH Value	254
13.3.2	Interaction with Monovalent Cations	254
13.3.3	Interaction with Divalent Cations	257
13.3.4	Interaction with a Trivalent Cation: Aluminum	263
13.3.5	A Classification	264
13.4	Interaction Between Polyelectrolyte Brushes and Oppositely Charged Polyelectrolytes in Solution	265
13.4.1	The Formation of Surface-Attached PEL-PEL Complexes	265
13.4.2	The Formation of PEL Multilayer Assemblies	268
14	Structure and Properties of High-Density Polymer Brushes Yoshinobu Tsujii, Muhammad Ejaz, Shinpei Yamamoto, Kohji Ohno, Kenji Urayama, and Takeshi Fukuda	273
14.1	Introduction	273
14.2	Controlled Synthesis of High-Density Polymer Brush by ATRP	274
14.3	Structure and Properties of High-Density PMMA Brushes	277
14.3.1	Swollen Brushes	277
14.3.2	Dry Brushes	279
14.4	Application of High-Density Polymer Brushes	282
15	Behavior of Surface-Anchored Poly(acrylic acid) Brushes with Grafting Density Gradients on Solid Substrates Tao Wu, Jan Genzer, Peng Gong, Igal Szleifer, Petr Vlek, and Vladimír ubr	287
	Glossary	287
15.1	Introduction	288
15.2	Experimental Section	292
15.2.1	Formation of the Gradient of the Polymerization Initiator	292
15.2.2	Preparation of PtBA and Hydrolysis into PAA	293
15.2.3	Polymer Characterization	294
15.3	Theory Section	296
15.4	Experimental Results	300
15.5	Discussion	304
15.5.1	Surface Hydrolysis of PtBA	304
15.5.2	Dependence of H on Ionic Strength	306
15.5.3	Dependence of H on the PAA Grafting Density	308
15.5.4	Molecular Insight from Calculations	310
16	Kinetics of Polymer Brush Formation With and Without Segmental Adsorption Lynn S. Penn, Heqing Huang, Roderic P. Quirk, and Tae H. Cheong	317
16.1	Introduction	317
16.2	Experimental	320
16.2.1	Synthesis and Characterization of Amine Chain-End Functionalized Polystyrene	320
16.2.2	Introduction of Active Sites to Surface of Solid	320
16.2.3	Tethering Reactions in Good Solvent	320
16.2.4	Tethering Reactions in Poor Solvent	321
16.2.5	Monitoring the Tethering Reactions	321
16.3	Results and Discussion	323
16.3.1	Results in Absence of Segmental Adsorption	323
16.3.2	Results in the Presence of Segmental Adsorption	325

Part III	Applications	329

17	Applications of Polymer Brushes and Other Surface-Attached Polymers Kenneth C. Caster	331
17.1	Introduction	331
17.2	Surface Modification and Functionalization	332
17.2.1	Polymerization Methodologies for Surface-Attached Polymers	332
17.2.2	Property Control	336
17.2.3	Impact on Types of Materials	336
17.3	Applications	336
17.3.1	Adhesion	337
17.3.2	Tribology	341
17.3.3	Stabilization and Compatiblization	341
17.3.4	Surface Coatings	343
17.3.5	Stimuli-Responsive and Switchable Surfaces	345
17.3.6	Separations	346
17.3.7	Nanofabrication	349
17.3.8	Surfaces for Electronics	350
17.3.9	Other Uses	351
17.4	Future Prospects	351
	Appendix	353
18	Polymer Brushes: Towards Applications Gregory L. Whiting, Tamer Farhan, and Wilhelm T. S. Huck	371
18.1	Introduction	371
18.2	Experimental	372
18.2.1	Materials	372
18.2.2	Characterization	373
18.2.3	Synthesis of Triphenylamine Acrylate (TPAA) Monomer	373
18.2.4	Synthesis and Deposition of Trichlorosilane ATRP Initiator	373
18.2.5	Surface-Initiated Polymerizations	373
18.3	Results and Discussion	374
18.3.1	Kinetics of Surface-Initiated ATRP of MMA from Silicon	374
18.3.2	Surface-Initiated ATRP from Polymeric Substrates	375
18.3.3	Synthesis of Conjugated Polymer Brushes from ITO	377
19	Polymerization, Nanopatterning and Characterization of Surface-Confined, Stimulus-Responsive Polymer Brushes Marian Kaholek, Woo-Kyung Lee, Bruce LaMattina, Kenneth C. Caster, and Stefan Zauscher	381
19.1	Introduction	381
19.2	Experimental	382
19.2.1	Materials	382
19.2.2	Substrates	383
19.2.3	Preparation of Initiator Monolayers	383
19.2.4	Nanopatterning of Initiator	383
19.2.5	NIPAAM Polymerization	384
19.2.6	Polymer Characterization	385
19.3	Results and Discussion	386
19.3.1	Surface-Initiated Bulk Polymerization	386
19.3.2	Phase Behavior and Mechanical Characterization	390
19.3.3	Surface Force Measurements	393
19.3.4	Nano-Patterning	396
20	Mixed Polymer Brushes: Switching of Surface Behavior and Chemical Patterning at the Nanoscale Sergiy Minko, Marcus Müller, Valeriy Luchnikov, Mikhail Motornov, Denys Usov, Leonid Ionov, and Manfred Stamm	403
20.1	Introduction	403
20.2	Theory of Mixed Polymer Brushes	404
20.3	Synthesis of Mixed Brushes	409
20.3.1	The "Grafting To" Method	409
20.3.2	The "Grafting From" Method	411
20.4	Experimental Study of Phase Segregation in Mixed Brushes	412
20.5	Adaptive Responsive Behavior: Regulation of Wetting and Adhesion	417
20.6	Patterning of Mixed Brushes	420
21	Local Chain Organization of Switchable Binary Polymer Brushes in Selective Solvents Melbs C. LeMieux, Denys Usov, Sergiy Minko, Manfred Stamm, and Vladimir V. Tsukruk	427
21.1	Introduction	427
21.1.1	Polymer Surface Modification	427
21.1.2	Polymer Brushes	428
21.1.3	Binary Polymer Brushes	429
21.2	Experimental	431
21.2.1	Materials and Synthesis	431
21.2.2	Methods	432
21.3	Results and Discussion	433
21.3.1	Dry State Analysis	433
21.3.2	Morphology in Solvent	434
21.3.3	Mechanical Response in Solvent	437
22	Motion of Nano-Objects Induced by a Switchable Polymer Carpet Svetlana Prokhorova, Alexey Kopyshev, Ayothi Ramakrishnan, and Jürgen Rühe	441
22.1	Introduction	441
22.2	Materials	443
22.3	Results and Discussion	444
23	Photochemical Strategies for the Preparation and Microstructuring of Densely Grafted Polymer Brushes on Planar Surfaces Oswald Prucker, Rupert Konradi, Martin Schimmel, Jörg Habicht, In-Jun Park, and Jürgen Rühe	449
23.1	Introduction	449
23.1.1	Topological and Chemical Patterning of Surfaces	449
23.1.2	Photochemical Pathways for Grafting Polymers onto Surfaces: A Literature Survey	451
23.2	General Features of Surface-Initiated Polymerization from Monolayers of Azo Initiators	453
23.3	Photolithographic Procedures for the Generation of Microstructured Polymer Brushes on Planar Surfaces	455
23.3.1	Photoablation of Polymer Brushes	455
23.3.2	Photoablation/Photodecomposition of the Initiator Layer followed by Thermal Polymerization	460
23.3.3	Patterning by Photopolymerization	462
23.4	Multifunctional Patterns	465
23.5	Applications of Photostructured Polymer Brushes	466
	Index	471

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