Publications by Francesco Ambrosio

Evaluation of Photocatalysts for Water Splitting through Combined Analysis of Surface Coverage and Energy-Level Alignment

Alfredo Pasquarello, Zhendong Guo, Francesco Ambrosio

To examine whether suitable conditions occur for the water splitting reaction at their interfaces with liquid water, we determine the pH-dependent surface coverage for a series of semiconductors, including GaAs, GaP, GaN, CdS, ZnO, SnO2, and rutile and ana ...

2020

On the Electronic and Optical Properties of Metal-Organic Frameworks: Case Study of MIL-125 and MIL-125-NH2

Alfredo Pasquarello, Gloria Capano, Berend Smit, Francesco Ambrosio, Kyriakos Stylianou, Stavroula Kampouri

The photo-active MIL-125 and MIL-125-NH2 metal-organic frameworks (MOFs), despite having a very similar crystalline structure, exhibit different optical behaviors. Luminescence in MIL-125 decays in about 1 ns, while for its amino counterpart, the lifetime ...

2020

Picture of the wet electron: a localized transient state in liquid water

Alfredo Pasquarello, Francesco Ambrosio, Michele Pizzochero

A transient state of the excess electron in liquid water preceding the development of the solvation shell, the so-called wet electron, has been invoked to explain spectroscopic observations, but its binding energy and atomic structure have remained highly ...

2019

Extrinsic Defects in Amorphous Oxides: Hydrogen, Carbon, and Nitrogen Impurities in Alumina

Alfredo Pasquarello, Zhendong Guo, Francesco Ambrosio

We present a procedure for addressing extrinsic defects in amorphous oxides, in which the most stable defect configurations are identified through ab initio molecular dynamics in various charge states and studied through hybrid functional calculations. The ...

American Physical Society (APS)2019

Absolute band alignment at semiconductor-water interfaces using explicit and implicit descriptions for liquid water

Alfredo Pasquarello, Nicola Marzari, Oliviero Andreussi, Zhendong Guo, Francesco Ambrosio

Quantum mechanical simulations that include the effects of the liquid environment are highly relevant for the characterization of solid-liquid interfaces, which is crucial for the design of a wide range of devices. In this work we present a rigorous and sy ...

2019

Effect of the Solvent on the Oxygen Evolution Reaction at the TiO2-Water Interface

Alfredo Pasquarello, Francesco Ambrosio, Patrick Gono

We investigate the solvation effect of water on the overpotentials of the oxygen evolution reaction on rutile TiO2 by applying the thermodynamic integration method on atomistic model interfaces with and without the water molecules. We compare the results a ...

2019

Reactivity and energy level of a localized hole in liquid water

Alfredo Pasquarello, Francesco Ambrosio

We study the reactivity and the energy level associated with the reduction of the H2O+ radical cation in liquid water by combining ab initio molecular dynamics simulations at the hybrid functional level, a grand-canonical formulation of solutes in aqueous ...

2018

Absolute Energy Levels of Liquid Water

Alfredo Pasquarello, Zhendong Guo, Francesco Ambrosio

2018

Alignment of Redox Levels at Semiconductor-Water Interfaces

Alfredo Pasquarello, Wei Chen, Zhendong Guo, Francesco Ambrosio, Patrick Gono

2018

Hole diffusion across leaky amorphous TiO2 coating layers for catalytic water splitting at photoanodes

Alfredo Pasquarello, Zhendong Guo, Francesco Ambrosio

Royal Society of Chemistry2018

pH-Dependent Surface Chemistry from First Principles: Application to the BiVO4(010)-Water Interface

Alfredo Pasquarello, Francesco Ambrosio, Julia Anna Wiktor

2018

Role of Polarons in Water Splitting: The Case of BiVO4

Alfredo Pasquarello, Francesco Ambrosio, Julia Anna Wiktor

2018

Surface Polarons Reducing Overpotentials in the Oxygen Evolution Reaction

Alfredo Pasquarello, Francesco Ambrosio, Julia Anna Wiktor, Patrick Gono

2018

Mechanism suppressing charge recombination at iodine defects in CH3NH3PbI3 by polaron formation

Alfredo Pasquarello, Francesco Ambrosio, Julia Anna Wiktor

Metal-halide perovskites exhibit high efficiencies in photovoltaic applications and low recombination rates, despite the high concentrations of intrinsic defects. We here study the hole trapping at the negative iodine interstitial, which corresponds to the ...

Royal Society of Chemistry2018

pH-Dependent Catalytic Reaction Pathway for Water Splitting at the BiVO4−Water Interface from the Band Alignment

Alfredo Pasquarello, Francesco Ambrosio, Julia Anna Wiktor

We align the band edges of BiVO4 at the interface with liquid water by combining advanced electronic-structure calculations, molecular dynamics simulations, and a computational hydrogen electrode. After accounting for spin–orbit coupling and thermal and nu ...

2018

Origin of low electron-hole recombination rate in metal halide perovskites

Alfredo Pasquarello, Francesco Ambrosio, Julia Anna Wiktor

To address the slow recombination of photogenerated charges in tetragonal CH 3 NH 3 PbI 3 , the evolution of extra electrons and holes is simulated through advanced ab initio molecular dynamics. We show that the localization of the charge carriers and thei ...

2018

Electronic Levels of Excess Electrons in Liquid Water

Alfredo Pasquarello, Giacomo Francesco Leonardo Miceli, Francesco Ambrosio

We provide a consistent description of the electronic levels associated with localized and delocalized excess electrons in liquid water by combining hybrid-functional molecular dynamics simulations with a grand canonical formulation of solutes in aqueous s ...

Amer Chemical Soc2017

Electronic and structural characterization of barrier-type amorphous aluminium oxide

Patrik Schmutz, Alfredo Pasquarello, Claudia Cancellieri, Raheleh Partovi Nia, Fabio Evangelisti, Francesco Ambrosio, Roland Hauert

The structural, electronic, and dielectric properties of barrier -type anodic Al oxides prepared with various thicknesses have been investigated. The planar and cross morphologies as well as the surface charge distribution were investigated as a function o ...

Elsevier2017

Comprehensive modeling of the band gap and absorption spectrum of BiVO4

Alfredo Pasquarello, Francesco Ambrosio, Julia Anna Wiktor, Igor Reshetnyak

We present first-principles calculations of the electronic structure of BiVO4 at various levels of theory. In the calculations, we take into account a series of effects that affect the band gap, i.e., spin-orbit coupling, electron-hole interaction, nuclear ...

2017

Note: Assessment of the SCAN+rVV10 functional for the structure of liquid water

Alfredo Pasquarello, Francesco Ambrosio, Julia Anna Wiktor

American Institute of Physics2017