Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

Connectivity between Static Field and Continuous Wave Field Effects on Excitation-Induced H2 Activation

Journal Article · · Journal of Physical Chemistry. C
 [1];  [2]
  1. Kansas State University, Manhattan, KS (United States); Kansas State University
  2. Kansas State University, Manhattan, KS (United States)
+ Show Author Affiliations
Due to the tremendous applications of the plasmon resonance excitation process, such as improvements in catalytic efficiency due to plasmonic enhancement and/or hot-electron processes, understanding the mechanism behind these processes has become a popular topic in recent years. In this work, we focus on unraveling the mechanism of excitation-induced H2 activation using a simplified triangular Au6/Ag6 cluster to investigate the effects of the electric field on electron redistribution and bond activation. We applied both static and continuous wave fields to investigate how these fields affect the systems. Geometrical changes (such as bond lengthening), molecular orbital reordering (affecting the relative energies of orbitals corresponding to hot-electron and charge-transfer excited states), and electronic charge redistribution between the cluster and the adsorbate occur upon application of a static electric field. To study H2 activation, we apply Ehrenfest dynamics with real-time time-dependent density functional theory and examine how different excitation frequencies and polarizations affect bond activation. Moreover, electron-only dynamics are examined with real-time time-dependent density functional theory, and the time-dependent variations in the orbital populations and electronic transitions provide information about the excitation and relaxation processes of hot electrons with applied electric fields. Here, the static field results represent structures that can be accessed during the evolution of the systems when applying continuous wave fields. Through these studies, the effects of static and continuous wave field effects on plasmon-induced H2 activation can be understood.
Research Organization:
Kansas State University, Manhattan, KS (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012273
OSTI ID:
2337767
Journal Information:
Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 31 Vol. 127; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (60)

A Review of Surface Plasmon Resonance-Enhanced Photocatalysis journal October 2012
Photocatalytic Plasmon‐Enhanced Nitrogen Reduction to Ammonia journal February 2021
Real-time, real-space implementation of the linear response time-dependent density-functional theory journal April 2006
Real-time time-dependent electronic structure theory: Real-time electronic structure theory
  • Goings, Joshua J.; Lestrange, Patrick J.; Li, Xiaosong
  • Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 8, Issue 1 https://doi.org/10.1002/wcms.1341
journal September 2017
The U.S. Department of Energy's National Hydrogen Storage Project: Progress towards meeting hydrogen-powered vehicle requirements journal February 2007
Mechanistic Insights into Plasmonic Catalysis by Dynamic Calculations: O2 and N2 on Au and Ag Nanoparticles journal February 2023
Non-Noble Plasmonic Metal-Based Photocatalysts journal April 2022
Real-Time Electron Dynamics Study of Plasmon-Mediated Photocatalysis on an Icosahedral Al 13 –1 Nanocluster journal May 2021
Theoretical Insights into Excitation-Induced Oxygen Activation on a Tetrahedral Ag8 Cluster journal October 2021
Theory of Plasmonic Hot-Carrier Generation and Relaxation journal October 2021
Theoretical Investigations on the Plasmon-Mediated Dissociation of Small Molecules in the Presence of Silver Atomic Wires journal March 2023
Effects of Field Strength and Silver Nanowire Size on Plasmon-Enhanced N2 Dissociation journal June 2023
TD-DFT+TB: An Efficient and Fast Approach for Quantum Plasmonic Excitations journal March 2020
Electronic Structure and Nonadiabatic Dynamics of Atomic Silver Nanowire–N 2 Systems journal August 2020
Localized Surface Plasmon Resonance as a Tool to Study Protein Corona Formation on Nanoparticles journal November 2021
H2 Activation on Pristine and Substitutional ZnO(101̅0) and Cr2O3(001) Surfaces by Density Functional Theory Calculations journal May 2022
Photodissociation of H2 on Ag and Au Nanoparticles: Effect of Size and Plasmon versus Interband Transitions on Threshold Intensities for Dissociation journal February 2023
Interplay between Intra- and Interband Transitions Associated with the Plasmon-Induced Hot Carrier Generation Process in Silver and Gold Nanoclusters journal December 2019
Aluminum Nanocrystals as a Plasmonic Photocatalyst for Hydrogen Dissociation journal January 2016
Localized Orbital Excitation Drives Bond Formation in Plasmonic Catalysis journal December 2021
Charge Separation in Photocatalysts: Mechanisms, Physical Parameters, and Design Principles journal December 2021
What’s so Hot about Electrons in Metal Nanoparticles? journal June 2017
Challenges in Plasmonic Catalysis journal December 2020
Active Site Engineering on Plasmonic Nanostructures for Efficient Photocatalysis journal February 2023
Nonradiative Plasmon Decay and Hot Carrier Dynamics: Effects of Phonons, Surfaces, and Geometry journal December 2015
Watching Visible Light-Driven CO 2 Reduction on a Plasmonic Nanoparticle Catalyst journal July 2018
Plasmonic Hot-Carrier-Mediated Tunable Photochemical Reactions journal July 2018
Optical Studies of Dynamics in Noble Metal Nanostructures journal June 2011
Mechanistic Insights into Photocatalyzed H 2 Dissociation on Au Clusters journal July 2020
The Optical Properties of Metal Nanoparticles:  The Influence of Size, Shape, and Dielectric Environment journal January 2003
Kinetic Density Functional Theory for Plasmonic Nanostructures: Breaking of the Plasmon Peak in the Quantum Regime and Generation of Hot Electrons journal March 2015
Laser-Controlled Dissociation of C 2 H 2 2+ : Ehrenfest Dynamics Using Time-Dependent Density Functional Theory journal March 2009
CO Oxidation at the Interface between Doped CeO 2 and Supported Au Nanoclusters journal July 2012
Surface Plasmon Spectroscopy of Nanosized Metal Particles journal January 1996
Hot Electrons Do the Impossible: Plasmon-Induced Dissociation of H 2 on Au journal December 2012
Quantum plasmon resonances of individual metallic nanoparticles journal March 2012
Catalytic conversion of solar to chemical energy on plasmonic metal nanostructures journal September 2018
Single plasmon hot carrier generation in metallic nanoparticles journal May 2019
Plasmon-mediated chemical reactions journal February 2023
Theoretical analysis of the optical excitation spectra of silver and gold nanowires journal January 2012
Hot carriers generated by plasmons: where are they generated and where do they go from there? journal January 2019
Plasmon-induced hot-carrier generation differences in gold and silver nanoclusters journal January 2019
Plasmonic enhancement of molecular hydrogen dissociation on metallic magnesium nanoclusters journal January 2021
Ab initio Ehrenfest dynamics journal August 2005
A long-range-corrected density functional that performs well for both ground-state properties and time-dependent density functional theory excitation energies, including charge-transfer excited states journal February 2009
Ab initio effective core potentials for molecular calculations. Potentials for the transition metal atoms Sc to Hg journal January 1985
Ab initio effective core potentials for molecular calculations. Potentials for main group elements Na to Bi journal January 1985
Ab initio effective core potentials for molecular calculations. Potentials for K to Au including the outermost core orbitals journal January 1985
Quantum coherent plasmon in silver nanowires: A real-time TDDFT study journal June 2014
Plasmon-induced dynamics of H 2 splitting on a silver atomic chain journal August 2015
Ab initio two-component Ehrenfest dynamics journal September 2015
Comparing the nature of quantum plasmonic excitations for closely spaced silver and gold dimers journal February 2022
Plasmon-induced excitation energy transfer in silver nanoparticle dimers: A real-time TDDFTB investigation journal April 2022
Investigation of plasmon relaxation mechanisms using nonadiabatic molecular dynamics journal December 2022
Tight-binding approach to time-dependent density-functional response theory journal February 2001
Density-functional study of Au n ( n = 2 – 2 0 ) clusters: Lowest-energy structures and electronic properties journal July 2002
Static polarizabilities and optical absorption spectra of gold clusters ( Au n , n = 2 – 14 and 20) from first principles journal November 2007
Generalized Gradient Approximation Made Simple journal October 1996
Hot Charge Carrier Transmission from Plasmonic Nanostructures journal May 2017
Optical Properties and Excited-State Dynamics of Atomically Precise Gold Nanoclusters journal April 2021

Similar Records

Theoretical Investigations on the Plasmon-Mediated Dissociation of Small Molecules in the Presence of Silver Atomic Wires
Journal Article · Wed Mar 01 19:00:00 EST 2023 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory · OSTI ID:2337771
Effects of Field Strength and Silver Nanowire Size on Plasmon-Enhanced N2 Dissociation
Journal Article · Tue Jun 27 20:00:00 EDT 2023 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory · OSTI ID:2337765
Excitation of a plasma wave by a right-handed Gaussian EM beam
Journal Article · Wed Jan 31 23:00:00 EST 1979 · J. Appl. Phys.; (United States) · OSTI ID:6504193

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Electric fields
Gold
Metal clusters
Molecular orbitals
Polarization