Daniel J. Auerbach
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View article: An Experimental Benchmark for the Barrier Height of an On-Surface Reaction: Hydrogen Oxidation on Pt(332)
An Experimental Benchmark for the Barrier Height of an On-Surface Reaction: Hydrogen Oxidation on Pt(332) Open
Developing predictive theories for the rates of reactions between surface-bound molecules is a central challenge to understanding many important phenomena including: heterogeneous catalysis, electrocatalysis, nanofabrication, and corrosion…
View article: The Mechanism and Rate-Determining Step of Catalytic Ammonia Oxidation on Pd(332) at High Temperatures
The Mechanism and Rate-Determining Step of Catalytic Ammonia Oxidation on Pd(332) at High Temperatures Open
Despite its immense practical importance in industrial production of nitric acid, the mechanisms of catalytic ammonia oxidation on platinum group metals remain controversial. In this work, we employ velocity-resolved kinetics to study ammo…
View article: An ion-imaging detector for high count rates
An ion-imaging detector for high count rates Open
The emergence of high-power ionizing light sources with repetition rates greater than 100 kHz promises vastly improved data acquisition times for electron and ion imaging experiments; however, optimal means to record ion images at high ave…
View article: Multi-mass velocity-resolved kinetics of surface reactions at 100 kHz acquisition rate
Multi-mass velocity-resolved kinetics of surface reactions at 100 kHz acquisition rate Open
Velocity-resolved kinetics (VRK) employs a pulsed molecular beam that initiates reactions at a surface and a pulsed ionization-laser that detects desorbed products, exploiting ion-imaging-based, velocity-sensitive detection to derive the p…
View article: Quantum interference observed in state-resolved molecule-surface scattering
Quantum interference observed in state-resolved molecule-surface scattering Open
Although the dynamics of collisions between a molecule and a solid surface are ultimately quantum mechanical, decohering effects owing to the large number of interacting degrees of freedom typically obscure the wavelike nature of these eve…
View article: Thermal Rates and High-Temperature Tunneling from Surface Reaction Dynamics and First-Principles
Thermal Rates and High-Temperature Tunneling from Surface Reaction Dynamics and First-Principles Open
Studying dynamics of the dissociative adsorption and recombinative desorption of hydrogen on copper surfaces has shaped our atomic-scale understanding of surface chemistry, yet experimentally determining the thermal rates for these process…
View article: Cooperative adsorbate binding catalyzes high-temperature hydrogen oxidation on palladium
Cooperative adsorbate binding catalyzes high-temperature hydrogen oxidation on palladium Open
Atomic-scale structures that account for the acceleration of reactivity by heterogeneous catalysts often form only under reaction conditions of high temperatures and pressures, making them impossible to observe with low-temperature, ultra-…
View article: Predicting Adhesion Energies of Metal Nanoparticles to Support Surfaces, Which Determines Metal Chemical Potential versus Particle Size and Thus Catalyst Performance
Predicting Adhesion Energies of Metal Nanoparticles to Support Surfaces, Which Determines Metal Chemical Potential versus Particle Size and Thus Catalyst Performance Open
Improved catalysts and electrocatalysts composed of transition metal nanoparticles dispersed on high-area supports are essential for energy and environmental technologies. The chemical potential of the metal atoms in these supported nanopa…
View article: Identification of reaction intermediates in the decomposition of formic acid on Pd
Identification of reaction intermediates in the decomposition of formic acid on Pd Open
We report an approach to identify intermediates for the formic acid decomposition reaction on Pd(111) and Pd(332) based on accurate measurements of isotopologue specific thermal reaction rates.
View article: Calorimetric Energies and Chemical Potentials of Metal Atoms in Catalytic Nanoparticles on Oxide and Carbon Supports: Improved Size Dependencies and Adhesion Energies
Calorimetric Energies and Chemical Potentials of Metal Atoms in Catalytic Nanoparticles on Oxide and Carbon Supports: Improved Size Dependencies and Adhesion Energies Open
The chemical potential of metal atoms, μM, in supported metal nanoparticles is an important descriptor related to both the catalytic activity and the stability of the nanoparticles. Here, we derive an expression relating μM to the radius o…
View article: Surface-induced vibrational energy redistribution in methane/surface scattering depends on catalytic activity
Surface-induced vibrational energy redistribution in methane/surface scattering depends on catalytic activity Open
Recent state-to-state experiments of methane scattering from Ni(111) and graphene-covered Ni(111) combined with quantum mechanical simulations suggest an intriguing correlation between the surface-induced vibrational energy redistribution …
View article: Quantum state-resolved methane scattering from Ni(111) and NiO(111) by bolometer infrared laser tagging: The effect of surface oxidation
Quantum state-resolved methane scattering from Ni(111) and NiO(111) by bolometer infrared laser tagging: The effect of surface oxidation Open
We describe a novel ultrahigh vacuum state-to-state molecule/surface scattering apparatus with quantum state preparation of the incident molecular beam and angle-resolved quantum state detection of the scattered molecules. State-resolved d…
View article: Highly Rotationally Excited N<sub>2</sub> Reveals Transition-State Character in the Thermal Decomposition of N<sub>2</sub>O on Pd(110)
Highly Rotationally Excited N<sub>2</sub> Reveals Transition-State Character in the Thermal Decomposition of N<sub>2</sub>O on Pd(110) Open
We employ time-slice and velocity map ion imaging methods to explore the quantum-state resolved dynamics in thermal N2O decomposition on Pd(110). We observe two reaction channels: a thermal channel that is ascribed to N2 products initially…
View article: Spin-dependent reactivity and spin-flipping dynamics in oxygen atom scattering from graphite
Spin-dependent reactivity and spin-flipping dynamics in oxygen atom scattering from graphite Open
The formation of two-electron chemical bonds requires the alignment of spins. Hence, it is well established for gas-phase reactions that changing a molecule’s electronic spin state can dramatically alter its reactivity. For reactions occur…
View article: Low-Energy Ion Scattering Intensities from Supported Nanoparticles: The Spherical Cap Model
Low-Energy Ion Scattering Intensities from Supported Nanoparticles: The Spherical Cap Model Open
Supported nanoparticles are of great importance to many technologies like fuel processing and chemical synthesis using catalysts and electrocatalysts, energy storage and generation using fuel cells and batteries, electrochemistry, magnetic…
View article: Supplementary Data for "Spin-dependent reactivity and spin-flipping dynamics in O atom scattering from graphite"
Supplementary Data for "Spin-dependent reactivity and spin-flipping dynamics in O atom scattering from graphite" Open
Datasets for "Spin-dependent reactivity and spin-flipping dynamics in O atom scattering from graphite", Nature Chemistry, 2023.
View article: Binding Energy and Diffusion Barrier of Formic Acid on Pd(111)
Binding Energy and Diffusion Barrier of Formic Acid on Pd(111) Open
Velocity-resolved kinetics is used to measure the thermal rate of formic acid desorption from Pd(111) between 228 and 273 K for four isotopologues: HCOOH, HCOOD, DCOOH, DCOOD. Upon molecular adsorption, formic acid undergoes decomposition …
View article: Steric Hindrance of NH<sub>3</sub> Diffusion on Pt(111) by Co-Adsorbed O-Atoms
Steric Hindrance of NH<sub>3</sub> Diffusion on Pt(111) by Co-Adsorbed O-Atoms Open
A detailed velocity-resolved kinetics study of NH3 thermal desorption rates from p(2 × 2) O/Pt(111) is presented. We find a large reduction in the NH3 desorption rate due to adsorption of O-atoms on Pt(111). A physical model describing the…
View article: Quantum effects in thermal reaction rates at metal surfaces
Quantum effects in thermal reaction rates at metal surfaces Open
There is wide interest in developing accurate theories for predicting rates of chemical reactions that occur at metal surfaces, especially for applications in industrial catalysis. Conventional methods contain many approximations that lack…
View article: Kinetics of NH<sub>3</sub> Desorption and Diffusion on Pt: Implications for the Ostwald Process
Kinetics of NH<sub>3</sub> Desorption and Diffusion on Pt: Implications for the Ostwald Process Open
We report accurate time-resolved measurements of NH3 desorption from Pt(111) and Pt(332) and use these results to determine elementary rate constants for desorption from steps, from (111) terrace sites and for diffusion on (111) terraces. …
View article: The Barrier for CO<sub>2</sub> Functionalization to Formate on Hydrogenated Pt
The Barrier for CO<sub>2</sub> Functionalization to Formate on Hydrogenated Pt Open
Understanding heterogeneous catalysis is based on knowing the energetic stability of adsorbed reactants, intermediates, and products as well as the energetic barriers separating them. We report an experimental determination of the barrier …
View article: The puzzle of rapid hydrogen oxidation on Pt(111)
The puzzle of rapid hydrogen oxidation on Pt(111) Open
We have known for over 200 years that hydrogen undergoes rapid oxidation to water on Pt catalysts; yet the reaction mechanism remains unclear. Here, we report high temporal resolution measurements of the production rate of H2O from hydroge…
View article: Highly Efficient Activation of HCl Dissociation on Au(111) via Rotational Preexcitation
Highly Efficient Activation of HCl Dissociation on Au(111) via Rotational Preexcitation Open
The probability for dissociation of molecules on metal surfaces, which often controls the rate of industrially important catalytic processes, can depend strongly on how energy is partitioned in the incident molecule. There are many example…
View article: Random Force in Molecular Dynamics with Electronic Friction
Random Force in Molecular Dynamics with Electronic Friction Open
The Langevin equation includes a random force to maintain equilibrium and prevent friction from bringing motion to a standstill; but for ballistic motion, the random force is often neglected. Here, we use the Langevin equation for molecula…
View article: Chemical dynamics from the gas‐phase to surfaces
Chemical dynamics from the gas‐phase to surfaces Open
The field of gas‐phase chemical dynamics has developed superb experimental methods to probe the detailed outcome of gas‐phase chemical reactions. These experiments inspired and benchmarked first principles dynamics simulations giving acces…
View article: CO<sub>2</sub>conversion by plasma: how to get efficient CO<sub>2</sub>conversion and high energy efficiency
CO<sub>2</sub>conversion by plasma: how to get efficient CO<sub>2</sub>conversion and high energy efficiency Open
Plasma technology, combined with activation on surfaces, is a novel way to convert CO2using green electricity.
View article: Velocity-resolved kinetics of site-specific carbon monoxide oxidation on platinum surfaces
Velocity-resolved kinetics of site-specific carbon monoxide oxidation on platinum surfaces Open
Catalysts are widely used to increase reaction rates. They function by stabilizing the transition state of the reaction at their active site, where the atomic arrangement ensures favourable interactions 1 . However, mechanistic understandi…