Ligand coated metal nanoparticles and quantum dots

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1 The Supramolecular Nano Materials Group Ligand coated metal nanoparticles and quantum dots Francesco Stellacci Department of Materials Science and Engineering

2 Outline Self-Assembled Monolayers SAM coated nanomaterials Mixed SAM coated nanomaterials Quantum dots

3 Self-Assembly

4 Protein Self-Assembly

5 Molecular Self-Assembly

6 Thiolated Monolayers on Gold S δ- -Au δ+ bond energy = 1.34 ev However, 2 S - Au bonds are not much stronger than one S - S disulfide bond and one Au - Au metallic bond A monolayer in solution therefore develops an equilibrium dodecane solution 2 * RS - Au RS -SR + Au -Au (surface)

7 Molecular Self-Assembly

8 Commensurate vs. Incommensurate

9 Wetting Properties

10 Wetting Properties II

11 Etch Pits and Defects

12 Phase Separation

13 Metal Nanoparticles Synthesis Metal Salt (AuHCl 4 ) + HS HS + Reducing Agent (NaBH 4 ) Direct mixed ligands reaction ** Ligand exchange reaction * F. Stellacci, et al. Adv. Mat. 2002, 14, 194 A. C. Templeton, M. P. Wuelfing and R. W. Murray, Accounts Chem. Res. 2000, 33, 27

14 Characterizing Metal Nanoparticles 3 nm TEM shows atoms in the core STM shows ligands in the shell 2.7 nm

15 Mixed Self-Assembled Monolayers Au (111) MPA Randomly distributed domains of OT form in a surrounding matrix of MPA HS COOH HS 5 nm OT STM Height Image of OT/MPA Mixed Monolayer on Au(111) R. Smith, S. Reed, P. Lewis, J. Monnell, R. Clegg, K. Kelly, L. Bumm, J. Huthison, P. Weiss. J. Phys. Chem. B 2001, 105,

16 Ordered Domains on NPs Hydrophobic/ Hydrophilic Ripples Form by Spontaneous Self- Assembly HS HS MPA COOH OT

17 Hydrophobic/Hydrophilic Ripples Hydrophilic Region: Carboxylic Acid Terminated Molecules Hydrophobic Region: Methyl Terminated Molecules

18 Particle Interdigitation Solid interdigitated state ΔH de-int Solid de-interdigitated state

19 X-Ray Diffraction 2:1 OT:MPA Au np (5:1 Au:ligand) 2:1 OT:MPA (Ag np) (2:1 Au:ligand)

20 Phase Separation on Nanoparticles HS H S NH 2 Hexanethiol: p-aminothiophenol Ag core OT:MPA O HS OH HS OH OT:Mercaptohexanol OT:MUA HS HS

21 Core Effect 3 nm

22 Ripple Spacing in OT:MPA System Morphology ranges from discretely packed domains to defect rich ripples to perfect ripples.

23 Evolution of Surface Morphology DT:MPA 2:1 OT:MPA 10:1

24 Solubility and Morphology 4 Domains Ripples Domains 3 Defect-Rich Perfect Ordering Defect-Rich Solubility Note: Solubility Decreases with Increasing %MPA due to Morphology MPA / (OT+MPA)

25 Ripple Spacing in OT:MPA System Morphology ranges from discretely packed domains to defect rich ripples to perfect ripples.

26 Surface Chemistry Modification HS OH O HS HS OH O Highly soluble in Toluene Highly soluble in Ethanol

27 Protein Nonspecific Absorption Proteins can assume a few possible conformations as determined by molecular structure 1) Maximizes exposure of hydrophobic region 2) Minimizes exposure of hydrophobic region Hydrophilic region Hydrophobic region Hydrophilic Surface Hydrophobic Surface Surface composed of Hydrophilic/Hydrophobic Domains

28 The Nano Lotus Leaf Effect Size of hydrophobic/hydrophilic regions of protein are greater than size scale of ligand domains on the nanoparticles. Proteins are conformationally frustrated and cannot adsorb to nanoparticle surface.

29 Cytochrome C: a large Protein Protein 24 h Extensive Adsorption of Protein onto Monolayer 3.6 x 3.6 x 13.7 nm Protein 24 h No Adsorption of Protein

30 Lysozyme: a small Protein Protein 24 h Extensive Adsorption of Protein onto Monolayer 4.5 x 3.0 x 3.0 nm Protein 24 h No Adsorption of Protein

31 Curvature Effects OT:MPA Mixed Monolayers formed on surfaces of varying curvatures Increasing Curvature 10 nm 10 nm 5 nm 5 nm Flat Au (111) on Mica Au on Si, with 20 nm hemispheres Au film with Au crystals ~ 10 nm Au film with Au crystals ~ 4 nm

32 Synthesis and Conformation Metal Salt (AuHCl 4 ) + Metal Salt (AuHCl 4 ) + HS HS HS COOH NaBH 4 (AuSR) n NaBH 4 HS COOH Nanoparticles obtained via the two-step method Nanoparticles obtained via the one-step method

33 Kinetic Effect Au thermally evaporated on Si SAM formed in the absence of (AuSR) n SAM formed in the presence of (AuSR) n

34 Other Monolayers

35 Other Monolayers II

36

37 Size Control

38 Optical Properties

39 Artificial Atoms

40

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