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No. of Publications: 66

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Direct Experimental Evidence for Substrate Adatom Incorporation into a Molecular Overlayer

Direct Experimental Evidence for Substrate Adatom Incorporation into a Molecular Overlayer

P. J. Mouslez, L. A. Rochford, P. T. P. Ryan, P. Blowey, J. Lawrence, D. A. Duncan, H. Hussain, B. Sohail, T.-L. Lee, G. R. Bell, G. Costantini, R. J. Maurer, C. Nicklin, D. P. Woodruff, J. Phys. Chem. C 126, 7346 - 7355 (2022)

"We present the results of a detailed structural study of the Au(111)-F4TCNQ system, combining surface characterization by STM, low-energy electron diffraction, and soft X-ray photoelectron spectroscopy with quantitative experimental structural information from normal incidence X-ray standing wave (NIXSW) and SXRD, together with dispersion-corrected density functional theory (DFT) calculations. SXRD measurements provide unequivocal evidence for the presence and location of Au adatoms, while the DFT calculations show this reconstruction to be strongly energetically favored"


Design Principles for Metastable Standing Molecules

Design Principles for Metastable Standing Molecules

H. H. Arefi, D.Corken, F. S.Tautz, R. J. Maurer, C. Wagner, J. Phys. Chem. C 126, 6880-6891 (2022)

"Here, we use density functional theory to study 3,4,9,10-perylene-tetracarboxylic dianhydride (PTCDA) standing on the Ag(111) surface as well as on the tip of a scanning probe microscope. We cast our results into a simple set of design principles for such metastable structures, the validity of which we subsequently demonstrate in two computational case studies. Our work proves the capabilities of computational nanostructure design in the field of metastable molecular structures and offers the intuition needed to fabricate new devices without tedious trial and error."


Thermodynamic Driving Forces for Substrate Atom Extraction by Adsorption of Strong Electron Acceptor Molecules

Thermodynamic Driving Forces for Substrate Atom Extraction by Adsorption of Strong Electron Acceptor Molecules

P. Ryan, P. J. Blowey, B. S. Sohail, L. A. Rochford, D. A. Duncan, T.-L. Lee, P. Starrs, G. Costantini, R. J. Maurer, J. Phys. Chem. C 126, 6082-6090 (2022)

"A quantitative structural investigation is reported, aimed at resolving the issue of whether substrate adatoms are incorporated into the monolayers formed by strong molecular electron acceptors deposited onto metallic electrodes. A combination of X-ray standing waves, STM, and DFT show that there is an energetic driving force for adatom incorporation into adsorbate structures of the strong acceptor F4TCNQ on Ag(100) but not for the weaker acceptor TCNQ."


Effect of electron donating/withdrawing groups on molecular photoswitching of functionalized hemithioindigo derivatives: a computational multireference study

Effect of electron donating/withdrawing groups on molecular photoswitching of functionalized hemithioindigo derivatives: a computational multireference study

M. Lea, V. Stavros, R. J. Maurer, ChemPhotoChem, DOI: 10.1002/cptc.202100290 (2022)

"The mechanism of photoswitching for hemithioindigo cannot be described by pure dihedral rotation around the central carbon-carbon bond. A complementary motion, often pyramidalization, is required to facilitate radiationless internal conversion. This computational study, explores how the inclusion of electron-withdrawing and electron-donating substituents alters the excited state potential energy surfaces and the mechanism of photoisomerization. The predicted changes in energy landscapes reflect the acceleration or slowing of the photoisomerization process for different derivatives that is also observed in experiment."


Roadmap on Machine Learning in Electronic Structure

Roadmap on Machine Learning in Electronic Structure

Kulik et al., IOP Electronic Structure DOI: 10.1088/2516-1075/ac572f (2022)

"A perspective roadmap that covers the present role and future perspective of machine learning in materials property prediction, the construction of accurate force fields, the solution of the many-body problem, and big data challenges."


Coexistence of carbonyl and ether groups on oxygen-terminated (110)-oriented diamond surfaces

Coexistence of carbonyl and ether groups on oxygen-terminated (110)-oriented diamond surfaces

Shayanthan Chaudhuri, Samuel J. Hall, Benedikt P. Klein, Marc Walker, Andrew J. Logsdail, Julie V. Macpherson, Reinhard J. Maurer, Communications Materials 3, 6 (2022)

"Here, we determine the oxygenation state of the (110) surface using a combination of density functional theory calculations and X-ray photoelectron spectroscopy experiments. We report the fabrication of the highest-quality (100)-oriented diamond crystal surface to date. We further propose a mechanism for the formation of the hybrid carbonyl-ether phase and rationalize its high stability. "


Core Electron Binding Energies in Solids from Periodic All-Electron Δ-Self-Consistent-Field Calculations

Core Electron Binding Energies in Solids from Periodic All-Electron Delta-Self-Consistent-Field Calculations

J. Matthias Kahk, Georg S. Michelitsch, Reinhard J. Maurer, Karsten Reuter, Johannes Lischner, J. Phys. Chem. Lett. 12, 9353-9359 (2021)

"We present an approach to calculate accurate core electron binding energies of a variety of materials based on Delta-self-consistent-field calculations that are referenced to the valence band maximum. We further show that the resulting simulations provide excellent agreement with experimental X-ray photoemission spectroscopy data."


Adiabatic versus non-adiabatic electron transfer at 2D electrode materials

Adiabatic versus non-adiabatic electron transfer at 2D electrode materials

Dan-Qing Liu, Minkyung Kang, David Perry, Chang-Hui Chen, Geoff West, Xue Xia, Shayantan Chaudhuri, Zachary P. L. Laker, Neil R. Wilson, Gabriel N. Meloni, Marko M. Melander, Reinhard J. Maurer, Patrick R. Unwin, Nature Communications 12, 7110 (2021)

"Using scanning electrochemical cell microscopy, and co-located structural microscopy, the classical hexaamineruthenium (III/II) couple is measured on a graphene-metal electrode. Using model Hamiltonian and constant potential density functional theory, we can rationalize the fact that monolayer graphene shows faster kinetics than bilayer graphene and we are able to identify the electron transfer as dominantly adiabatic."

Nature Portfolio Blogpost

The stabilization potential of a standing molecule

The stabilization potential of a standing molecule

Marvin Knol, Hadi H. Arefi, Daniel Corken, James Gardner, F. Stefan Tautz, Reinhard J. Maurer, and Christian Wagner, Science Advances 7, eabj9751 (2021)

"Here, we combine scanning probe experiments with ab initio potential energy calculations to investigate the thermal stability of a prototypical standing molecule. We reveal its generic stabilization mechanism, a fine balance between covalent and van der Waals interactions including the latter's long-range screening by many-body effects, and find a remarkable agreement between measured and calculated stabilizing potentials."

Warwick University Press Release
Warwthermal stability of a prototypical standing molecule. We reveal its generic stabilization mechanism, a fine balance
between covalent and van der Waals interactions including the latter’s long-range screening by many-body fects, and find a remarkable agreement between measured and calculated stabilizing potentials.."

Perspective on integrating machine learning into computational chemistry and materials science

Perspective on integrating machine learning into computational chemistry and materials science

Julia Westermayr, Michael Gastegger, Kristof T. Schütt, Reinhard J. Maurer, J. Chem. Phys. 154, 230903 (2021)

"As ML is becoming pervasive in electronic structure theory and molecular simulation, we provide an overview of how atomistic computational modeling is being transformed by the incorporation of ML approaches. From the perspective of the practitioner in the field, we assess how common workflows to predict structure, dynamics, and spectroscopy are affected by ML."

Topology Effects in Molecular Organic Electronic Materials: Pyrene and Azupyrene

Topology Effects in Molecular Organic Electronics Materials: Pyrene and Azupyrene

Benedikt P. Klein, Lukas Ruppenthal, Samuel J. Hall, Lars E Sattler, Sebastian M. Weber, Jan Herritsch, Andrea Jaegermann, Reinhard J. Maurer, Gerhard Hilt, and Michael Gottfried, ChemPhysChem 22, 1-10 (2021)

"Using photoelectron spectroscopy, near edge X-ray absoption fine structure spectroscopy, and density functional theory, we characterize the electronic and optical properties of pyrene and azupyrene thin films. The differences between the properties of the two compounds can be understood in terms of their different bonding topology."

First-principles calculations of hybrid inorganic-organic interfaces: From state-of-the-art to best practice

First-principles calculations of hybrid inorganic-organic interfaces: From state-of-the-art to best practice

Oliver T. Hofmann, Egbert Zojer, Lukas Hörmann, Andreas Jeindl, and R. J. Maurer, Phys. Chem. Chem. Phys. 23, 8132-8180 (2021)

"In this review, we discuss how to choose appropriate atomistic representations for the simulation of hybrid inorganic-organic interfaces. We provide tips and tricks on how to efficiently converge the self-consistent field cycle and to obtain accurate geometries. We particularly focus on potentially unexpected pitfalls and the errors they incur. As a summary, we provide a list of best practice rules for interface simulations that should especially serve as a useful starting point for less experienced users and newcomers to the field."

The Nuts and Bolts of Ab-Initio Core-Hole Simulations for K-shell X-Ray Photoemission and Absorption Spectra

The Nuts and Bolts of Ab-Initio Core-Hole Simulations for K-shell X-Ray Photoemission and Absorption Spectra

B. Klein, S. J. Hall, R. J. Maurer, J. Phys. Condens. Matter 33, 154005 (2020)

"We present the numerical and technical details of our variants of the DeltaSCF and transition potential method (coined DeltaIP-TP) to simulate XPS and NEXAFS transitions. Using exemplary molecules in gas-phase, in bulk crystals, and at metal-organic interfaces, we systematically assess how practical simulation choices affect the stability and accuracy of simulations. We particularly focus on the choice of aperiodic or periodic description of systems and how spurious charge effects in periodic calculations affect the simulation outcomes. For the benefit of practitioners in the field, we discuss sensible default choices, limitations of the methods, and future prospects."

Determining the effect of hot electron dissipation on molecular scattering experiments at metal surfaces

Determining the effect of hot electron dissipation on molecular scattering experiments at metal surfaces

C. L. Box, Y. Zhang, R. Yin, B. Jiang, R. J. Maurer, JACS Au 1, 164-173 (2020)

"Vibrational state-to-state scattering of NO on Au(111) provides a testing ground for developing various nonadiabatic theories, including electronic friction theory. This system is often cited as the prime example for the breakdown of electronic friction theory, a very efficient model accounting for dissipative forces on metal-adsorbed molecules due to the creation of electron-hole-pair excitations in the metal. Here we present a comprehensive quantitative analysis of the performance of molecular dynamics with electronic friction (MDEF) in describing vibrational state-to-state scattering of NO on Au(111) and connect directly to fundamental approximations. Our analysis provides a firm baseline for the future development of nonadiabatic dynamics methods to tackle problems in surface chemistry and photocatalysis."

A deep neural network for molecular wave functions in quasi-atomic minimal basis representation

A deep neural network for molecular wave functions in quasi-atomic minimal basis representation

M. Gastegger, A. McSloy, M. Luya, K. T. Schütt, R. J. Maurer, J. Chem. Phys 153, 044123 (2020)

"We present an adaptation of the recently proposed SchNet for Orbitals (SchNOrb) deep convolutional neural network model [Nature Commun. 10, 5024 (2019)] for electronic wave functions in an optimised quasi-atomic minimal basis representation. For five organic molecules ranging from 5 to 13 heavy atoms, the model accurately predicts molecular orbital energies and wavefunctions and provides access to derived properties for chemical bonding analysis. Particularly for larger molecules, the model outperforms the original atomic-orbital-based SchNOrb method in terms of accuracy and scaling. "

Alkali Doping Leads to Charge-Transfer Salt Formation in a Two-Dimensional Metal-Organic Framework

Alkali Doping Leads to Charge-Transfer Salt Formation in a Two-Dimensional Metal-Organic Framework

P. J. Blowey, B. Sohail, L. A. Rochford, T. Lafosse, D. A. Duncan, P. T. P. Ryan, D. A. Warr, T.-L. Lee, G. Costantini, R. J. Maurer, and D. P. Woodruff, ACS Nano 14, 7475-7483 (2020)

"We show that the insertion of alkali atoms can significantly change the structure and electronic properties of a metal-organic interface. Coadsorption of tetracyanoquinodimethane (TCNQ) and potassium on a Ag(111) surface leads to the formation of a two-dimensional charge transfer salt, with properties quite different to those of the two-dimensional Ag adatom TCNQ metal-organic framework formed in the absence of K doping. We establish a highly accurate structural model by combination of quantitative XSW, STM, and DFT calculations. Full agreement between the experimental data and the computational prediction of the structure is only achieved by inclusion of a charge-transfer-scaled dispersion correction in the DFT, which correctly accounts for the effects of strong charge transfer on the atomic polarizability of potassium. "

Enhanced Bonding of Pentagon–Heptagon Defects in Graphene to Metal Surfaces: Insights from the Adsorption of Azulene and Naphthalene to Pt(111)

Enhanced Bonding of Pentagon–Heptagon Defects in Graphene to Metal Surfaces: Insights from the Adsorption of Azulene and Naphthalene to Pt(111)

Benedikt P. Klein, S. Elizabeth Harman, Lukas Ruppenthal, Griffin M. Ruehl, Samuel J. Hall, Spencer J. Carey, Jan Herritsch, Martin Schmid, Reinhard J. Maurer, Ralf Tonner, Charles T. Campbell, and J. Michael Gottfried, Chem. Mater. 32, 1041-1053 (2020)

"We show here that the interface properties may be controlled by topological defects, such as the pentagon–heptagon (5–7) pairs, because of their strongly enhanced bonding to the metal. To measure the bond energy and other key properties not accessible for the embedded defects, we use azulene as a molecular model for the 5–7 defect. Comparison to its isomer naphthalene, which represents the regular graphene structure, reveals that azulene interacts more strongly with a Pt(111) surface. Using a combination of single-crystal adsorption calorimetry, x-ray photoelectron and photoabsorption spectroscopies (XPS/NEXAFS), and Density Functional Theory, we fully characterize the adsorption strength, the surface structure and surface chemistry of 5-7 defect systems on Pt(111). Our model study shows that the topology of the π-electron system strongly affects its bonding to a transition metal and thus can be utilized to tailor interface properties."

Unifying machine learning and quantum chemistry with a deep neural network for molecular wavefunctions

Unifying machine learning and quantum chemistry with a deep neural network for molecular wavefunctions

Kristof T. Schütt, Michael Gastgger, Alexandre Tkatchenko, Klaus-Robert Müller, Reinhard J. Maurer, Nature Commun. 10, 5024 (2019)

"Here we present a deep machine learning framework for the prediction of the quantum mechanical wavefunction in a local basis of atomic orbitals from which all other ground-state properties can be derived. This approach retains full access to the electronic structure via the wavefunction at force-field-like efficiency and captures quantum mechanics in an analytically differentiable representation. On several examples, we demonstrate that this opens promising avenues to perform inverse design of molecular structures for targeting electronic property optimisation and a clear path towards increased synergy of machine learning and quantum chemistry."

Molecule–Metal Bond of Alternant versus Nonalternant Aromatic Systems on Coinage Metal Surfaces: Naphthalene versus Azulene on Ag(111) and Cu(111)

Molecule–Metal Bond of Alternant versus Nonalternant Aromatic Systems on Coinage Metal Surfaces: Naphthalene versus Azulene on Ag(111) and Cu(111)

    Benedikt P. Klein, Juliana M. Morbec, Markus Franke, Katharina K. Greulich, Malte Sachs, Shayan Parhizkar, Francois C. Boquet, Martin Schmidt, Samuel J. Hall, Reinhard J. Maurer, Bernd Meyer, Ralf Tonner, Christian Kumpf, Peter Kratzer, and J. Michael Gottfried, J. Phys. Chem. C just accepted, DOI: 10.1021/acs.jpcc.9b08824 (2019)

    "The coverage-dependent interaction of Azulene and Naphthalene with Ag(111) and Cu(111) surfaces was studied with the normal-incidence X-ray standing wave (NIXSW) technique, near-edge X-ray absorption fine structure (NEXAFS) spectroscopy, UV and X-ray photoelectron spectroscopies (UPS and XPS), and density functional theory (DFT). We analyse the interaction strength and charge-transfer at the molecule-metal interface by comparing simulated and measured NEXAFS spectra."

    Performance of van der Waals DFT approaches for helium diffraction on metal surfaces

    Performance of van der Waals DFT approaches for helium diffraction on metal surfaces

    Marcos del Cueto, Reinhard Maurer, Amjad Al Taleb, Daniel Farias, Fernando Martin and Cristina Diaz, J. Phys.: Condens. Matter 31, 135901 (2019).

    "The ability of the different approaches proposed to date to include the effects of van der Waals (vdW) dispersion forces in density functional theory (DFT) is currently under debate. Here, we used the diffraction of He on a Ru(0001) surface as a challenging benchmark system to analyze the suitability of several representative approaches, from the ones correcting the exchange-correlation generalized gradient approximation (GGA) functional, to the ones correcting the DFT energies through pairwise-based methods. To perform our analysis, we have built seven continuous potential energy surfaces (PESs) and carried out quantum dynamics simulations using a multi-configuration time-dependent Hartree (MCTDH) method. Our analysis reveals that standard DFT within the PBE-GGA framework, although it overestimates diffraction probabilities, yields the best results in comparison with available experimental measurements."
    Wed 16 Jan 2019, 20:08 | Tags: Density Functional Theory, dispersion interactions

    Adhesion, forces and the stability of interfaces

    Adhesion, forces and the stability of interfaces

    Robin Guttmann, Johannes Hoja, Christoph Lechner, Reinhard J. Maurer, and Alexander F. Sax, Beilstein J. Org. Chem., 15, 106–129. (2019)

    "Weak molecular interactions (WMI) are responsible for processes such as physisorption; they are essential for the structure and stability of interfaces, and for bulk properties of liquids and molecular crystals. For a long time, dispersion was largely ignored in chemistry, attractive intermolecular interactions were nearly exclusively attributed to electrostatic interactions. We discuss the importance of dispersion interactions for the stabilization in systems that are traditionally explained in terms of the “special interactions” mentioned above."

    https://www.beilstein-journals.org/s/eDT9bbVnb5


    Hot-electron effects during reactive scattering of H2 from Ag(111): assessing the sensitivity to initial conditions, coupling magnitude, and electronic temperature

    Hot-electron effects during reactive scattering of H2 from Ag(111): assessing the sensitivity to initial conditions, coupling magnitude, and electronic temperature

    Yaolong Zhang, Reinhard J. Maurer, Hua Guo and Bin Jiang, Faraday Discuss. 214, 105-121 (2019)

    "Using molecular dynamics simulations with electronic friction, we systematically study the effect of hot electrons on measurable state-to-state scattering probabilities of molecular hydrogen from a (111) surface of silver. We find that dynamic scattering results and the ensuing energy loss are highly sensitive to the magnitude of electronic friction."



    Hot-electron effects during reactive scattering of H2 from Ag(111): the interplay between mode-specific electronic friction and the potential energy landscape

    Hot-electron effects during reactive scattering of H2 from Ag(111): the interplay between mode-specific electronic friction and the potential energy landscape

    Y.Zhang, R.J.Maurer, H.Guo, B.Jiang, Chem. Sci. 10, 1089-1097 (2019)

    "The breakdown of the Born-Oppenheimer approximation gives rise to nonadiabatic effects in gas-surface reactions at metal surfaces. However, for a given reaction, it remains unclear which factors quantitatively determine whether these effects measurably contribute to surface reactivity in catalysis and photo/electrochemistry. Here, we systematically investigate hot electron effects during H2 scattering from Ag(111) using electronic friction theory."


    The Structure of VOPc on Cu(111): Does V═O Point Up, or Down, or Both?

    The Structure of VOPc on Cu(111): Does V═O Point Up, or Down, or Both?

    P.J.Blowey. R.J.Maurer, L.A.Rochford, D.A.Duncan, J.-H.Kang, D.A.Warr, A.J.Ramadan, T.-L.Lee, P.K.Thakur, G.Constantini, K.Reuter and D.P.Woodruff The Journal of Physical Chemistry C 123, 8101-8111, (2019)

    "The local structure of the nonplanar phthalocyanine, vanadyl phthalocyanine (VOPc), adsorbed on Cu(111) at a coverage of approximately one-half of a saturated molecular layer, has been investigated by a combination of normal-incidence X-ray standing waves (NIXSW), scanned-energy mode photoelectron diffraction (PhD), and density-functional theory (DFT), complemented by scanning tunnelling microscopy (STM)."


    Computational design of metal-supported molecular switches: Transient ion formation during light- and electron-induced isomerisation of azobenzene

    Computational design of metal-supported molecular switches: Transient ion formation during light- and electron-induced isomerisation of azobenzene

    R. J. Maurer and K. Reuter, J. Phys. Condens Matter, DOI:10.1088/1361-648X/aaf0e1 (2018), Invited Article

    "Using DFT and linear expansion Delta-Self-Consistent DFT excited-state calculations, we systematically analyse important design parameters that define successful light-induced molecular switching of azobenzene."


    Tracking Metal Electrodeposition Dynamics from Nucleation and Growth of a Single Atom to Crystalline Nanoparticle

    Tracking Metal Electrodeposition Dynamics from Nucleation and Growth of a Single Atom to Crystalline Nanoparticle

    H. E. M. Hussein, R. J. Maurer, H. Amari, J. J. P. Peters, L. Meng, R. Beanland, M. E. Newton, J. V. Macpherson, ACS Nano 12, pp. 7388-7396 (2018)

    "Identical Location Scanning Transmission Electron Microscopy and Density Functional Theory calculations give the first account of electrochemically-driven gold deposition with single-atom resolution."


    Electron-Hole-Pair-Induced Vibrational Energy Relaxation of Rhenium Catalysts on Gold Surfaces

    Electron-Hole-Pair-Induced Vibrational Energy Relaxation of Rhenium Catalysts on Gold Surfaces

    Aimin Ge, Benjamin Rudshteyn, Jingyi Zhu, Reinhard J. Maurer, VIctor S. Batista, and Tianquan Lian, J. Phys. Chem. Lett. 9, 406-412 (2018)

    "Using a combination of time-resolved vibrational spectroscopy and Density Functional Theory, we study the vibrational relaxation mechanisms of a metal-adsorbed reduction catalyst."


    Ab-initio tensorial electronic friction for molecules on metal surfaces: nonadiabatic vibrational relaxation

    Ab-initio tensorial electronic friction for molecules on metal surfaces: nonadiabatic vibrational relaxation

    Reinhard J. Maurer, Mikhail Askerka, Victor S. Batista, John C. Tully, Phys. Rev. B. 94, 115432 (2016)

    We present our efficient and robust ab-initio implementation of tensorial electronic friction and apply it to calculate vibrational lifetimes.


    Switching of an Azobenzene-Tripod Molecule on Ag(111)

    Switching of an Azobenzene-Tripod Molecule on Ag(111)

    Katharina Scheil, Thiruvancheril G. Gopakumar, Julia Bahrenburg, Friedrich Temps, Reinhard J. Maurer, Karsten Reuter, Richard Berndt, J. Phys. Chem. Lett. 7, 2080-2084 (2016)

    We observe and interpret the mechanism of multistate switching of an Azobenzene Tripod on Ag(111) using STM, STS and Density Functional Theory.


    Adsorption structures and energetics of molecules on metal surfaces: Bridging experiment and theory

    Adsorption structures and energetics of molecules on metal surfaces: Bridging experiment and theory

    Reinhard J. Maurer, Victor G. Ruiz, Javier Camarillo-Cisneros, Wei Liu, Nicola Ferri, Karsten Reuter, Alexandre Tkatchenko, Prog. Surf. Sci. 91, 72-100 (2016)

    By reviewing experiment and calculation data for structures and energies, we compose a benchmark database for molecules on metal surfaces.


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