Surface-Charge Dependent Orientation of Water at the Interface of a Gold Electrode: A Cluster Study
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Gianluca Fazio
Abstract
A gold/water interface has been investigated with the DFT-based self-consistent-charge density-functional tight-binding (SCC-DFTB) method using a cluster model. Born–Oppenheimer molecular-dynamics simulations for mono-, bi-, and trilayers of water on the surface of a Au55 cluster have been computed. We have demonstrated the applicability of this method to the study of the structural and dynamical properties of the gold/water-multilayer interface. The results of the simulations clearly show the charge-dependent orientation and the corresponding polarization of the water sphere around the gold cluster. However, it was also shown that this polarization is restricted almost only to the first solvation shell. This illustrates the rather short-range screening behavior of water. The present study builds the basis for further investigations of metal/electrolyte interfaces on a reliable atomistic level, avoiding the problems of spurious artifacts in models using periodic boundary conditions.
Dedicated to:
Prof. Alexander Eychmüller on the occasion of his 60th birthday.
Acknowledgements
On the occasion of his 60th birthday, GS and JOJ acknowledge a long-term fruitful collaboration and friendship with their colleague Alexander Eychmüller. JOJ enjoyed especially their joint participation in the LVB project (project number 18/59/74/95/127/130-133/135). Furthermore, the authors acknowledge computational time by the Zentrum für Informationsdienste und Hochleistungsrechnen (ZIH) at TU Dresden for project TransPheMat.
References
1. H. Helmholtz, Annalen der Physik 243 (1879) 337.10.1002/andp.18792430702Search in Google Scholar
2. M. Gouy, J. Phys. Theor. Appl. 9 (1910) 457.10.1051/jphystap:019100090045700Search in Google Scholar
3. D. L. Chapman, Lond. Edinb. Dubl. Phil. Mag. 25 (1913) 475.10.1080/14786440408634187Search in Google Scholar
4. P. Debye, E. Huckel, Z. Phys. 24 (1923) 185.Search in Google Scholar
5. W. Schmickler, D. Henderson, Prog. Surf. Sci. 22 (1986) 323.10.1016/0079-6816(86)90005-5Search in Google Scholar
6. R. Parsons, Chem. Rev. 90 (1990) 813.10.1021/cr00103a008Search in Google Scholar
7. K.-i. Ataka, T. Yotsuyanagi, M. Osawa, J. Phys. Chem. 100 (1996) 10664.10.1021/jp953636zSearch in Google Scholar
8. Y. Tong, F. Lapointe, M. Thämer, M. Wolf, R. K. Campen, Angew. Chem. Int. Ed. 56 (2017) 4211.10.1002/anie.201612183Search in Google Scholar PubMed
9. J.-J. Velasco-Velez, C. H. Wu, T. A. Pascal, L. F. Wan, J. Guo, D. Prendergast, M. Salmeron, Science 346 (2014) 831.10.1126/science.1259437Search in Google Scholar PubMed
10. Y. Xue, J. Chem. Phys. 136 (2012) 024702.10.1063/1.3675494Search in Google Scholar PubMed
11. G. Seifert, J. Phys. Chem. A. 111 (2007) 5609.10.1021/jp069056rSearch in Google Scholar PubMed
12. G. Seifert, D. Porezag, T. Frauenheim, Int. J. Quantum Chem. 58 (1996) 185.10.1002/(SICI)1097-461X(1996)58:2<185::AID-QUA7>3.0.CO;2-USearch in Google Scholar
13. M. Elstner, D. Porezag, G. Jungnickel, J. Elsner, M. Haugk, Th. Frauenheim, S. Suhai, G. Seifert, Phys. Rev. B 58 (1998) 7260.10.1103/PhysRevB.58.7260Search in Google Scholar
14. Q. Cui, M. Elstner, Phys. Chem. Chem. Phys. 16 (2014) 14368.10.1039/C4CP00908HSearch in Google Scholar
15. D. Selli, G. Fazio, G. Seifert, C. Di Valentin, J. Chem. Theory Comput. 13 (2017) 3862.10.1021/acs.jctc.7b00479Search in Google Scholar
16. N. Tarrat, M. Rapacioli, J. Cuny, J. Morillo, J.-L. Heully, F. Spiegelman, Comput. Theor. Chem. 1107 (2017) 102.10.1016/j.comptc.2017.01.022Search in Google Scholar
17. A. Fihey, C. Hettich, J. Touzeau, F. Maurel, A. Perrier, C. Köhler, B. Aradi, T. Frauenheim, J. Comput. Chem. 36 (2015) 2075.10.1002/jcc.24046Search in Google Scholar
18. L. Martínez, R. Andrade, E. G. Birgin, J. M. Martínez, J. Comput. Chem. 30 (2009) 2157.10.1002/jcc.21224Search in Google Scholar
19. M. Connolly, Science 221 (1983) 709.10.1126/science.6879170Search in Google Scholar
20. P. Jungwirth, Faraday Discuss. 141 (2009) 9.10.1039/B816684FSearch in Google Scholar
21. A. P. Willard, S. K. Reed, P. A. Madden, D. Chandler, Faraday Discuss. 141 (2009) 423.10.1039/B805544KSearch in Google Scholar
©2018 Walter de Gruyter GmbH, Berlin/Boston
Articles in the same Issue
- Frontmatter
- Preface
- Congratulations to Alexander Eychmüller
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- Controlled Aqueous Synthesis of CdSe Quantum Dots using Double-Hydrophilic Block Copolymers as Stabilizers
- Fabrication of Ag2S/CdS Heterostructured Nanosheets via Self-Limited Cation Exchange
- Ion-Selective Ligands: How Colloidal Nano- and Micro-Particles Can Introduce New Functionalities
- TEM, FTIR and Electrochemistry Study: Desorption of PVP from Pt Nanocubes
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- Gelation-Assisted Layer-by-Layer Deposition of High Performance Nanocomposites
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- Fluorescence Quenching of CdTe Quantum Dots with Co (III) Complexes via Electrostatic Assembly Formation
- Colloidal Photoluminescent Refractive Index Nanosensor Using Plasmonic Effects
- Towards Low-Toxic Colloidal Quantum Dots
- Color-Enrichment Semiconductor Nanocrystals for Biorhythm-Friendly Backlighting
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- Chemical Routes to Surface Enhanced Infrared Absorption (SEIRA) Substrates
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- Single Particle Spectroscopy of Radiative Processes in Colloid-to-Film-Coupled Nanoantennas
- Coupled Plasmon Resonances and Gap Modes in Laterally Assembled Gold Nanorod Arrays
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Articles in the same Issue
- Frontmatter
- Preface
- Congratulations to Alexander Eychmüller
- Halogens in the Synthesis of Colloidal Semiconductor Nanocrystals
- Controlled Aqueous Synthesis of CdSe Quantum Dots using Double-Hydrophilic Block Copolymers as Stabilizers
- Fabrication of Ag2S/CdS Heterostructured Nanosheets via Self-Limited Cation Exchange
- Ion-Selective Ligands: How Colloidal Nano- and Micro-Particles Can Introduce New Functionalities
- TEM, FTIR and Electrochemistry Study: Desorption of PVP from Pt Nanocubes
- Incorporation of CdTe Nanocrystals into Metal Oxide Matrices Towards Inorganic Nanocomposite Materials
- Diatoms – A “Green” Way to Biosynthesize Gold-Silica Nanocomposites?
- Evidence for Photo-Switchable Carrier Mobilities in Blends of PbS Nanocrystals and Photochromic Dithienylcyclopentene Derivatives
- Gelation-Assisted Layer-by-Layer Deposition of High Performance Nanocomposites
- Enhancement of the Fluorescence Quantum Yield of Thiol-Stabilized CdTe Quantum Dots Through Surface Passivation with Sodium Chloride and Bicarbonate
- Fluorescence Quenching of CdTe Quantum Dots with Co (III) Complexes via Electrostatic Assembly Formation
- Colloidal Photoluminescent Refractive Index Nanosensor Using Plasmonic Effects
- Towards Low-Toxic Colloidal Quantum Dots
- Color-Enrichment Semiconductor Nanocrystals for Biorhythm-Friendly Backlighting
- Transient Absorption Studies on Nanostructured Materials and Composites: Towards the Development of New Photocatalytic Systems
- Transient Spectroscopy of Glass-Embedded Perovskite Quantum Dots: Novel Structures in an Old Wrapping
- Energy Transfer Between Single Semiconductor Quantum Dots and Organic Dye Molecules
- Chemical Routes to Surface Enhanced Infrared Absorption (SEIRA) Substrates
- Plasmonic Cu/CuCl/Cu2S/Ag and Cu/CuCl/Cu2S/Au Supports with Peroxidase-Like Activity: Insights from Surface Enhanced Raman Spectroscopy
- n-Type Cu2O/α-Fe2O3 Heterojunctions by Electrochemical Deposition: Tuning of Cu2O Thickness for Maximum Photoelectrochemical Performance
- The Photoelectrochemistry of Assemblies of Semiconductor Nanoparticles at Interfaces
- Surface-Charge Dependent Orientation of Water at the Interface of a Gold Electrode: A Cluster Study
- Single Particle Spectroscopy of Radiative Processes in Colloid-to-Film-Coupled Nanoantennas
- Coupled Plasmon Resonances and Gap Modes in Laterally Assembled Gold Nanorod Arrays
- Anisotropy of Structure and Optical Properties of Self-Assembled and Oriented Colloidal CdSe Nanoplatelets
- Simple Electroless Synthesis of Cobalt Nanoparticle Chains, Oriented by Externally Applied Magnetic Fields
- Functionalization of Graphene Aerogels and their Applications in Energy Storage and Conversion
- Macroscopic Aerogels with Retained Nanoscopic Plasmonic Properties
- Application of Aqueous-Based Covalent Crosslinking Strategies to the Formation of Metal Chalcogenide Gels and Aerogels
- Cellulose-Based Hydrogels with Controllable Electrical and Mechanical Properties
- Naphthalenetetracarboxylic Diimide Derivatives: Molecular Structure, Thin Film Properties and Solar Cell Applications
- Metal-Phenolic Encapsulated Mesoporous Silica Nanoparticles for pH-Responsive Drug Delivery and Magnetic Resonance Imaging
- Extraction of K2CO3 from Low Concentration [K+] Solutions with the Aid of CO2: A Study on the Metastable Phase Equilibrium of K2CO3-Na2CO3-H2O Ternary System
