Ari Paavo Seitsonen

Ari Paavo Seitsonen
Ecole Normale Supérieure de Paris | ENS · Département de Chimie

Dr. rer. nat.

About

246
Publications
48,236
Reads
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42,951
Citations
Citations since 2017
47 Research Items
26811 Citations
201720182019202020212022202301,0002,0003,0004,0005,000
201720182019202020212022202301,0002,0003,0004,0005,000
201720182019202020212022202301,0002,0003,0004,0005,000
201720182019202020212022202301,0002,0003,0004,0005,000
Additional affiliations
October 2013 - June 2014
University of Zurich
Position
  • Scientific co-worker
January 2005 - June 2009
Sorbonne Université
Position
  • Ingénieur de recherche
Education
September 1988 - May 1993
HUT
Field of study
  • Physics

Publications

Publications (246)
Article
We report an ab initio simulation study of changes in structural and dynamic properties of liquid Si at 7 pressures ranging from 10.2 GPa to 24.3 GPa along the isothermal line 1150 K, which is above the minimum of the melting line. The increase of pressure from 10.2 GPa to 16 GPa causes strong reduction in the tetrahedral ordering of the most close...
Article
The production of high‐quality hexagonal boron nitride (h‐BN) is essential for the ultimate performance of 2D materials‐based devices, since it is the key 2D encapsulation material. Here, a decisive guideline is reported for fabricating high‐quality h‐BN on transition metals. It is crucial to exclude carbon from the h‐BN related process, otherwise...
Preprint
Full-text available
The production of high-quality hexagonal boron nitride (h-BN) is essential for the ultimate performance of two-dimensional (2D) materials-based devices, since it is the key 2D encapsulation material. Here, a decisive guideline is reported for fabricating high-quality h-BN on transition metals: It is crucial to exclude carbon from h-BN related proce...
Article
Ru‐porphyrins act as convenient pedestals for the assembly of N‐heterocyclic carbenes (NHCs) on solid surfaces. Upon deposition of a simple NHC ligand on a close packed Ru‐porphyrin monolayer, an extraordinary phenomenon can be observed: Ru‐porphyrin molecules are transferred from the silver surface to the next molecular layer. We have investigated...
Article
Ru‐porphyrins act as convenient pedestals for the assembly of N‐heterocyclic carbenes (NHCs) on solid surfaces. Upon deposition of a simple NHC ligand on a close packed Ru‐porphyrin monolayer, an extraordinary phenomenon can be observed: Ru‐porphyrin molecules are transferred from the silver surface to the next molecular layer. We have investigated...
Article
Full-text available
Silicene, the two-dimensional (2D) allotrope of silicon, is a promising material for electronics. So far, the most direct synthesis strategy has been to grow it epitaxially on metal surfaces; however, the effect of the strong silicon-metal interaction on the structure and electronic properties of the metal-supported silicene is generally poorly und...
Preprint
Full-text available
The conformation of molecules on surfaces is decisive for their functionality. For the case of the endofullerene paramagnet Sc2TbN@C80 the conformation is linked to an electric and a magnetic dipole moment. Therefore a workfunction change of a substrate with adsorbed molecules, qualifies the system to be magnetoelectric. One monolayer of Sc2TbN@C80...
Article
Full-text available
Gold mobilization, transfer, and concentration in the Earth’s crust are controlled by hydrothermal sulfur- and chloride-bearing fluids. Yet the exact chemical identity, structure, and stability of Au-bearing species and, in particular, the respective contributions of the sulfide (HS−) and trisulfur ion (S3⋅−) ligands to Au transport lack direct in...
Article
Full-text available
Applying strong direct current (DC) electric fields on the apex of a sharp metallic tip, electrons can be radially emitted from the apex to vacuum. Subsequently, they magnify the nanoscopic information on the apex, which serves as a field emission microscope (FEM). When depositing molecules on such a tip, peculiar electron emission patterns such as...
Preprint
Full-text available
Applying strong direct current (DC) electric fields on the apex of a sharp metallic tip, electrons can be radially emitted from the apex to vacuum. Subsequently, they magnify the nanoscopic information on the apex, which serves as a field emission microscope (FEM). When depositing molecules on such a tip, peculiar electron emission patterns such as...
Article
Full-text available
We assess the crucial role of tetrapyrrole flexibility in the CO ligation to distinct Ru‐porphyrins supported on an atomistically well‐defined Ag(111) substrate. Our systematic real space visualisation and manipulation experiments with scanning tunnelling microscopy directly probe the ligation, while bond‐resolving atomic force microscopy and X‐ray...
Article
Full-text available
The CO ligation to two different ruthenium porphyrins on the Ag(111) surface under vacuum was investigated experimentally and theoretically. The electronic and geometric changes upon ligation as well as the energetics of the process were elucidated. The surface adaptability of the porphyrin macrocycle conformation proves crucial for CO binding. Ab...
Article
Significance Iron silicide (FeSi) provides multiple fascinating features whereby intriguing functional properties bearing significant application prospects were recognized. FeSi is understood notably as a correlated d -electron narrow-gap semiconductor and a putative Kondo insulator, hosting unconventional quasiparticles. Recently, metallic surface...
Article
The controlled arrangement of N-heterocyclic carbenes (NHCs) on solid surfaces is a current challenge of surface functionalization. We introduce a strategy of using Ru porphyrins in order to control both the orientation and lateral arrangement of NHCs on a planar surface. The coupling of the NHC to the Ru porphyrin is a facile process which takes p...
Article
The structure of a cyclic peptide with important biological functionalities, cyclosporin A (CsA), is investigated at the single molecule level. Its adsorption on Cu(111) under ultra-high vacuum is characterised with scanning tunnelling microscopy (STM) and density functional theory. With STM investigations, we demonstrate element specific on-surfac...
Article
Full-text available
The data presented here concern the photophysical characterization of luminescent MCM-41 nanoparticles doped with 3-hydroxyflavone and 7-hydroxyflavone, two fluorescent flavonoids. UV-Vis and fluorescence spectra obtained on freshly-prepared samples and aged (2 months exposed to air) samples are shown. The effect of light exposure is also studied....
Article
Flavones and flavonols are naturally-occurring organic molecules with interesting biological, chemical and photophysical properties. In recent years their interaction with silica surfaces has received increasing attention. In this work, the flavonol 3-hydroxyflavone (3HF) and the flavone 7-hydroxyflavone (7HF) have been encapsulated in MCM-41 mesop...
Preprint
Full-text available
We report an {\it ab initio} simulation study of changes in structural and dynamic properties of liquid Si at 7 pressures ranging from 10.2 GPa to 24.3 GPa along the isothermal line 1150~K, which is above the minimum of the melting line. The increase of pressure from 10.2 GPa to 16 GPa causes strong reduction in the tetrahedral ordering of the most...
Article
Ionic liquids (IL) are promising electrolytes for electrochemical applications due to their remarkable stability and high charge density. Molecular dynamics simulations are essential for a better understanding of the complex phenomena occurring at the electrode-IL interface. In this work, we have studied the interface between graphene and 1-ethyl-3...
Article
The image visualizes three parameters used to control the electronic structure of adsorbed metal‐organic complexes, namely the nanostructured hexagonal boron nitride support, the tip of a scanning probe microscope, and the molecular environment. The templating functionality of the atomically thin hexagonal boron nitride layer is highlighted by the...
Article
Full-text available
The use of molecular materials in solar cells and nano‐electronics demands a fundamental understanding and control of their electronic properties. Particularly relevant is the molecular response to the environment, that is, the interaction with the support and adjacent molecules, as well as the influence of electrostatic gating. Here, the control o...
Preprint
Full-text available
Non-monotonous changes in velocity autocorrelations across the transformation from molecular to atomic fluid in hydrogen under pressure are studied by ab initio molecular dynamics simulations at the temperature 2500 K. We report diffusion coefficients in a wide range of densities from purely molecular fluid up to metallic atomic fluid phase. An ana...
Article
We report the observation of a pressure-induced non-monotonic behavior of the long-wavelength asymptote of total charge density fluctuations right in the region of molecular-to-atomic fluid transformation from ab-initio molecular dynamics (AIMD) simulations of fluid hydrogen. Screening in the total charge density composed of point protons and distr...
Article
Full-text available
Non-monotonous changes in velocity autocorrelations across the transformation from molecular to atomic fluid in hydrogen under pressure are studied by ab initio molecular dynamics simulations at the temperature 2500 K. We report diffusion coefficients in a wide range of densities from purely molecular fluid up to metallic atomic fluid phase. An ana...
Preprint
Full-text available
Ionic liquids (IL) are promising electrolytes for electrochemical applications due to their remarkable stability and high charge density. Molecular dynamics simulations are essential for better understanding the complex phenomena occurring at the electrode-IL interface. In this work, we have studied the interface between graphene and 1-ethyl-3-meth...
Article
In situ preparation of oxotitanium tetraphenylporphyrin (TiO-TPP) on Ag(111) under ultra-high vacuum conditions was achieved in a multi-step procedure starting from adsorbed free-base tetraphenylporphyrin (2H-TPP). The final product as well as the intermediate titanium tetraphenylporphyrin (Ti-TPP) were characterized by a suite of surface-sensitive...
Article
Full-text available
The stability of magnetic information stored in surface adsorbed single‐molecule magnets is of critical interest for applications in nanoscale data storage or quantum computing. The present study combines X‐ray magnetic circular dichroism, density functional theory and magnetization dynamics calculations to gain deep insight into the substrate depe...
Article
There is enormous recent interest in weak, van der Waals-type (vdW) interactions due to their fundamental relevance for two-dimensional materials and the so-called vdW heterostructures. Tackling this problem using computer simulation is very challenging due to the nontrivial, nonlocal nature of these interactions. We benchmark different treatments...
Article
Extended organometallic honeycomb alkynyl-silver networks have been synthesized on a noble metal surface under ultrahigh vacuum conditions via a gas-mediated surface reaction protocol. Specifically, the controlled exposure to molecular oxygen efficiently deprotonates terminal alkyne moieties of 1,3,5-tris-(4-ethynylphenyl)benzene (Ext-TEB) precurso...
Article
Full-text available
Endohedral fullerenes, such as Dy2ScN@C80, are single-molecule magnets with long relaxation times of their magnetization. An open and anisotropic 4f electron shell in the lanthanides (here Dy) imposes a magnetic moment that maintains its orientation at liquid-helium temperatures for macroscopic times. If these molecules shall be used as single-bit...
Article
In article number 1804066, Hamid Oughaddou and co‐workers synthesize a single‐layer of blue phosphorene on Au(111) using molecular beam epitaxy. Scanning tunneling microscopy images show high‐quality and ordered monolayer phosphorene. Density functional theory calculations support a blue phosphorene layer presenting two different structures while p...
Article
3-hydroxyflavone (3HF) is a widely studied molecule that acts as a simplified prototype of biological, more complex flavonoids. Its solvation mechanism is still under investigation. Here we report a joint experimental and simulation study of the vibrational properties of 3HF in gas phase and in simple liquids tetrachloromethane, chloroform and acet...
Article
Full-text available
Phosphorene is a new 2D material composed of a single or few atomic layers of black phosphorus. Phosphorene has both an intrinsic tunable direct bandgap and high carrier mobility values, which make it suitable for a large variety of optical and electronic devices. However, the synthesis of single‐layer phosphorene is a major challenge. The standard...
Article
Full-text available
Ions inside Fullerene molecules are model systems for the study of the electrostatic interaction across a single layer of carbon. For TbSc2N@C80 on h-BN/Ni(111) we observe with high-resolution x-ray photoelectron spectroscopy a splitting of the C 1s core level. The data may be explained quantitatively with density functional theory. The correlation...
Article
Full-text available
There are currently no experimental techniques that combine atomic resolution imaging with elemental sensitivity and chemical fingerprinting on single molecules. The advent of using molecular-modified tips in non-contact atomic force microscopy (nc-AFM) has made it possible to image (planar) molecules with atomic resolution. However, the mechanisms...
Preprint
There has been enormous interest in weak, van der Waals-type interactions due to their fundamental relevance in the field of two-dimensional materials and the so-called van der Waals heterostructures. Tackling this problem using computer simulation is extremely challenging due to the non-trivial, non-local nature of these interactions. We benchmark...
Article
The adsorption of molecules on surfaces affects the surface dipole and thus changes in the work function may be expected. The effect in change of work function is particularly strong if charge between substrate and adsorbate is involved. Here we report the deposition of a strong electron acceptor molecule, tetrafluorotetracyanoquinodimethane C$_{12...
Article
Full-text available
Interfacial supramolecular self-assembly represents a powerful tool for constructing regular and quasicrystalline materials. In particular, complex two-dimensional molecular tessellations, such as semi-regular Archimedean tilings with regular polygons, promise unique properties related to their nontrivial structures. However, their formation is cha...
Article
Although on-surface metalation protocols of tetrapyrroles with 3d metals are well established, reports on the formation of lanthanide tetrapyrrole complexes are scarce. Here, we address the synthesis of lanthanide-tetrapyrrole units in detail, refining earlier findings. Specifically, the formation of cerium tetraphenylporphyrin (Ce-TPP) was induced...
Article
Metallo-supramolecular engineering on surfaces provides a powerful strategy toward low-dimensional coordination architectures with prospects for several application fields. To date, most efforts have relied on transition metal centers, and only recently did we pioneer lanthanide-directed assembly. Coordination spheres and motifs with rare-earth ele...
Article
Full-text available
By means of scanning tunnelling microscopy (STM), complementary density functional theory (DFT) and X-ray photoelectron spectroscopy (XPS) we investigate the binding and self-assembly of a saturated molecular layer of model N-heterocyclic carbene (NHC) on the Cu(111), Ag(111), and Au(111) surfaces under ultra-high vacuum (UHV) conditions. XPS revea...
Article
Full-text available
Quantum ESPRESSO is an integrated suite of open-source computer codes for quantum simulations of materials using state-of-the art electronic-structure techniques, based on density-functional theory, density-functional perturbation theory, and many-body perturbation theory, within the plane-wave pseudo-potential and projector-augmented-wave approach...
Article
Atomically thin hexagonal boron nitride (h-BN) layers on metallic supports represent a promising platform for the selective adsorption of atoms, clusters, and molecular nanostructures. Specifically, scanning tunneling microscopy (STM) studies revealed an electronic corrugation of h-BN/Cu(111), guiding the self-assembly of molecules and their energy...
Article
Full-text available
Electron diffraction is a standard tool to investigate the atomic structure of surfaces, interfaces, and adsorbate systems. In particular, photoelectron diffraction is a promising candidate for real-time studies of structural dynamics combining the ultimate time resolution of optical pulses and the high scattering cross-sections for electrons. In v...
Article
We report on the surface-guided synthesis of an unprecedented dinuclear organocobalt complex, its self-assembly into a complex nanoarchitecture, and a single-molecule level investigation of its switching behavior. Initially, an organic layer is prepared by depositing hexakis((trimethylsilyl)ethynyl)-benzene under ultra-high vacuum conditions onto A...
Article
Extensive ab initio simulations of ice-water basal interface at seven temperatures in the range 250–400 K were performed in NVT and NPT ensembles with a collection of 389 water molecules in order to estimate the melting point of ice from direct liquid-solid two-phase coexistence. Density functional theory with the BLYP (Becke-Lee-Yang-Parr) exchang...
Article
The chemistry of aluminium or oxo-aluminium in water is still relatively unknown, although it is the basis for many chemical and industrial processes, including floc- culation in water treatment plants. Trimeric species have a predominant role in the formation of the Keggin cations, which are the basic building block of aluminium- based chemicals....
Article
The collective dynamics in liquid water is an active research topic experimentally, theoretically and via simula- tions. Here, ab initio molecular dynamics simulations are reported in heavy and ordinary water at temperature 323.15 K, or 50°C. The simulations in heavy water were performed both with and without dispersion correc- tions. We found that...
Article
The effect of electronic dispersion over a wide variety of SiO2 polymorphs (faujasite, ferrierite, α-cristobalite, α-quartz, coesite, and stishovite) is investigated using state-of-the-art density functional theory. Different functionals and dispersion correction schemes are compared, ranging from the local density approximation to fully nonlocal e...
Article
Significance Gold resources on Earth result from an exceptional concentration phenomenon yielding metal contents in ore a thousand to a million times higher than those in common rocks. We show that this process is controlled by sulfur radical ions ( S 3 − ), which strongly bind Au in aqueous solution at elevated temperatures and pressures and allow...
Article
Full-text available
The cinchona alkaloids cinchonidine and cinchonine belong to the most efficient chiral modifiers for the noble metal-catalyzed enantioselective hydrogenation of C[double bond, length as m-dash]O and C[double bond, length as m-dash]C bonds. Under reaction conditions these modifiers are coadsorbed on the noble metal surface with hydrogen. Using densi...
Article
Unlike phonons in crystals, the collective excitations in liquids cannot be treated as propagation of harmonic displacements of atoms around stable local energy minima. The viscoelasticity of liquids, reflected in transition from the adiabatic to elastic high-frequency speed of sound and in absence of the long-wavelength transverse excitations, res...
Article
The interplay between the electronic structure and reconstruction of the geometry on a surface is an intriguing and exciting investigation. One classic example that has been one of the first systems to be identified using the angularly resolved photo-emission spectroscopy and scanning tunnelling microscopy is the Herringbone reconstruction on the A...
Article
Full-text available
The proton disorder in ice has a key role in several properties such as the growth mode, thermodynamical properties, and ferroelectricity. While structural phase transitions from proton disordered to proton ordered ices have been extensively studied, much less is known about their electronic and optical properties. Here, we present ab initio many b...
Article
Full-text available
Molecular dynamics (MD) simulations have been performed on Luteolin (Lut) dissolved in various solvents (methanol, 1-propanol, 2-propanol, 1-butanol, dimethylsulfoxide, acetone and hexane) with the purpose to characterize the local structure around the hydroxyl (OH)1 and carbonyl (C = O) moieties and to correlate the findings with the experimental...
Article
The cover picture shows the rocky road of cluster stabilization. In their Full Paper on page 625 ff. K. Hahn et al. use density functional theory calculations to simulate the adsorption of small Ni clusters on a CeO2 surface to investigate the fundamental properties of the Ni/CeO2 system relevant in many catalytic applications. Deposition of Ni clu...
Article
The detail of the incorporation of carbon dioxide in silicate melts at upper mantle conditions is still badly known. To give some theoretical guidance, we have performed first-principle molecular dynamics simulations (FPMD) to quantify the speciation and the incorporation of carbon dioxide in two CO2-rich silicate melts (~ 20 wt% CO2 at 2073 K and...
Article
In this study we have used density functional theory calculations to investigate the stability, structure and catalytic properties of Ni clusters supported on CeO2. We have found Ni clusters to be stabilized with increasing cluster size up to ten atoms both as isolated clusters and adsorbed on CeO2(1 1 1). Analysis of the structural properties show...
Article
Many-body effects arise from the collective behaviour of large numbers of interacting particles, for example, electrons, and the properties of such a system cannot be understood considering only single or non-interacting particles. Despite the generality of the many-body picture, there are only a few examples of experimentally observing such effect...
Article
In this perspective we discuss how an intimate interaction of experiments with theory is able to deepen our insight into the catalytic reaction system on the molecular level. This strategy is illustrated by discussing various examples from our own research of surface chemistry and model catalysis. The particular examples were carefully chosen to ba...
Article
First-principle molecular dynamics (FPMD) calculations have been performed to evaluate the physical properties of liquid calcium carbonate (CaCO3), which are up to now poorly known. The liquid structure, the density, the atomic vibration motions, the diffusion coefficients of calcium and carbonate ions and the electrical conductivity have been eval...
Article
Full-text available
Nanotechnology, in order to become ultimately efficient, requires achieving the construction of elemental structures at the atomistic precision. One way toward this goal is using templated surfaces as support for directed synthesis. The nanomesh, a single-atom thick layer of hexagonal boron nitride on Rh(111) [Corso et al., Science 2004, 303, 217],...
Article
Full-text available
The electronic properties of high-efficiency CuInSe2 (CIS)-based solar cells are affected by the microstructural features of the absorber layer, such as point defect types and their distribution. Recently, there has been controversy over whether some of the typical point defects in CIS—VCu, VSe, InCu, CuIn—can form stable complexes in the material....
Article
Static and dynamic autocorrelations of charge density, composed of positive point ions and instantaneous distribution of electron density, are studied in liquid Li in a pressure range from ambient to 186 GPa using ab initio molecular dynamics simulations. It is shown analytically that the long-wavelength limit of the charge-charge static structure...
Article
We report a combined scanning tunneling microscopy and density functional theory study on the formation of intricate networks involving a flexible 5-fold carbonitrile–lanthanide (cerium or gadolinium) coordination. By employing linear linkers equipped with terminal carbonitrile functional groups, and by tuning the local rare-earth to molecule stoic...
Article
Catalytic activity is of pivotal relevance in enabling efficient and selective synthesis processes. Recently, covalent coupling reactions catalyzed by solid metal surfaces opened the rapidly evolving field of on-surface chemical synthesis. Tailored molecular precursors in conjunction with the catalytic activity of the metal substrate allow the synt...
Article
Full-text available
Hexagonal boron nitride (h-BN) is a prominent member in the growing family of two-dimensional materials with potential applications ranging from being an atomically smooth support for other 2D materials to templating growth of molecular layers. We have studied the structure of monolayer h-BN grown by chemical vapour deposition on Ir(111) by low-tem...
Article
Suitable templates to steer the formation of nanostructure arrays on surfaces are indispensable in nanoscience. Recently, atomically thin sp(2)-bonded layers such as graphene or boron nitride (BN) grown on metal supports have attracted considerable interest due to their potential geometric corrugation guiding the positioning of atoms, metallic clus...
Conference Paper
As our understanding of the world around us increases it becomes more challenging to make use of what we already know, and to increase our understanding still further. Computational modeling and simulation have become critical tools in addressing this challenge. The requirements of high-resolution, accurate modeling have outstripped the ability of...