Overview of project B02
Ab-Initio Simulation of Electronic Excitation and Relaxation
This project will be mainly concerned with the simulation of the sub-picosecond dynamics in low-dimensional systems, i.e., in molecules or two-dimensional materials, following optical excitation with a laser pulse. The methods used to simulate the dynamics comprise time-dependent density functional theory (TDDFT) combined with Ehrenfest dynamics of the atomic positions, employing a computer code based on atom-centred numerical orbitals whose capabilities have been extended by us during the last funding period. Moreover, phonons and electron-phonon coupling will be studied by static DFT.
We plan to investigate the excitation of phonons in 2D materials by inelastic electron tunnelling in collaboration with scanning tunnelling microscopy in A08 and of recently discovered chiral phonons by optical excitation with polarized light. The transfer of spin and orbital angular momentum from the electronic to the lattice system will be addressed via calculations including spin-orbit coupling and compared to time-resolved photoelectron spectroscopy (B01) and X-ray diffraction (C01). Moreover, we will provide input to model Hamiltonians treated in B03, A02 and B07 to model the order-disorder transition on the Si(100) surface investigated experimentally in A08 and C03.
A particular challenge to ab-initio modelling is the dynamics of charge transfer between a metal electrode and a 2D material, or a 2D material and a molecular layer. Using methodology developed in the last funding period, we plan to simulate the (partial) equilibration of hot electrons in gold and their electric-field enhanced tunnelling to MoS2/Au or MoSe2/Au multilayer films, a topic of interest to B01 and B06. Moreover, the GW method as well as TDDFT shall be used to study the electronic band alignment in molecular oligo-acene (e.g. anthracene) layers on MoS2 and the dynamics of electron-hole separation subsequent to optical excitation of the heterostructure. In both subprojects, experimental partners using VIS/IR pump probe and sum frequency spectroscopy (A06), as well as structural characterization of the molecular films (A08) will be crucial to verify the simulation results. Moreover, we plan to continue collaborating with C05 on TMDC thin films.
Publications
2024
Christian Brand, Alfred Hucht, Hamid Mehdipour, Giriraj Jnawali, Jonas D. Fortmann, Mohammad Tajik, Rüdiger Hild, Björn Sothmann, Peter Kratzer, Ralf Schützhold and Michael Horn-von Hoegen
Critical Behavior of the Dimerized Si(001) Surface: Continuous Order-Disorder Phase Transition in the Two-Dimensional Ising Universality Class
Phys. Rev. B 109, 134104 (2024)
DOI: 10.1103/PhysRevB.109.134104
Tao Yang, Stephan Sleziona, Erik Pollmann, Eckart Hasselbrink, Peter Kratzer, Marika Schleberger, Richard Kramer Campen and Yujin Tong
Isolating the Optical Response of a MoS2 Monolayer under Extreme Screening of a Metal Substrate
Phys. Rev. B 109, L161402 (2024)
DOI: 10.1103/PhysRevB.109.L161402
Hamid Mehdipour and Peter Kratzer
First-Principles Calculations of MoSeTe/WSeTe Bilayers: Stability, Phonons, Electronic Band Offsets, and Rashba Splitting
Phys. Rev. B 109, 085425 (2024)
DOI: 10.1103/PhysRevB.109.085425
Hamid Mehdipour, Peter Kratzer, Saeedeh S. Tafreshi and Oleg Prezhdo
Accelerated Electron-Hole Separation at the Organic-Inorganic Anthracene/Janus MoSSe Interface
J. Phys. Chem. Lett. 15, 7878 (2024)
DOI: 10.1021/acs.jpclett.4c01774
Lea Kämmerer, Gérald Kämmerer, Manuel Gruber, Jan Grunwald, Tobias Lojewski, Laurent Mercadier, Loïc Le Guyader, Robert Carley, Cammille Carinan, Natalia Gerasimova, David Hickin, Benjamin E. Van Kuiken, Giuseppe Mercurio, Martin Teichmann, Senthil Kumar Kuppusamy, Andreas Scherz, Mario Ruben, Klaus Sokolowski-Tinten, Andrea Eschenlohr, Katharina Ollefs, Carolin Schmitz-Antoniak, Felix Tuczek, Peter Kratzer, Uwe Bovensiepen and Heiko Wende
Femtosecond Spin-State Switching Dynamics of Fe(II) Complexes Condensed in Thin Films
ACS Nano 18, 34596 (2024)
DOI: 10.1021/acsnano.4c05123
2023
Christian Brand, Alfred Hucht, Giriraj Jnawali, Jonas D. Fortmann, Björn Sothmann, Hamid Mehdipour, Peter Kratzer, Ralf Schützhold and Michael Horn-von Hoegen
Dimer Coupling Energies of the Si(001) Surface
Phys. Rev. Lett. 130, 126203 (2023)
DOI: 10.1103/PhysRevLett.130.126203
Tao Yang, Erik Pollmann, Stephan Sleziona, Eckart Hasselbrink, Peter Kratzer, Marika Schleberger, Richard Kramer Campen and Yujin Tong
Interaction Between a Gold Substrate and Monolayer MoS2: An Azimuthal-Dependent Sum Frequency Generation Study
Phys. Rev. B 107, 155433 (2023)
DOI: 10.1103/physrevb.107.155433
Jennifer Schmeink, Vladislav Musytschuk, Erik Pollmann, Stephan Sleziona, Andre Maas, Peter Kratzer and Marika Schleberger
Evaluating Strain and Doping of Janus MoSSe from Phonon Mode Shifts Supported by Ab-Initio DFT Calculations
Nanoscale 15, 10834 (2023)
DOI: 10.1039/d3nr01978k
2022
Peter Kratzer, Laurenz Rettig, Irina Yu. Sklyadneva, Evgueni V. Chulkov and Uwe Bovensiepen
Relaxation of Photoexcited Hot Carriers Beyond Multitemperature Models: General Theory Description Verified by Experiments on Pb/Si(111)
Phys. Rev. Research 4, 033218 (2022)
DOI: 10.1103/PhysRevResearch.4.033218
Hamid Mehdipour and Peter Kratzer
Structural Defects in a Janus MoSSe Monolayer: A Density Functional Theory Study
Phys. Rev. B 106, 235414 (2022)
DOI: 10.1103/PhysRevB.106.235414
2021
Joscha Hekele, Yi Yao, Yosuke Kanai, Volker Blum and Peter Kratzer
All-Electron Real-Time and Imaginary-Time Time-Dependent Density Functional Theory within a Numeric Atom-Centered Basis Function Framework
J. Chem. Phys. 155, 154801 (2021)
DOI: 10.1063/5.0066753
Joscha Hekele, Matthias Linke, Thomas Keller, Jesil Jose, Marvin Hille, Eckart Hasselbrink, Sebastian Schlücker and Peter Kratzer
A Fresh Look at the Structure of Aromatic Thiols on Au Surfaces from Theory and Experiment
J. Chem. Phys. 155, 044707 (2021)
DOI: 10.1063/5.0053493
Soumyajit Sarkar and Peter Kratzer
Signatures of the Dichalcogenide-Gold Interaction in the Vibrational Spectra of MoS₂and MoSe₂on Au(111)
J. Phys. Chem. C 125, 26645 (2021)
DOI: 10.1021/acs.jpcc.1c08594
2020
Erik Pollmann, Juliana M. Morbec, Lukas Madauß, Lara Bröckers, Peter Kratzer and Marika Schleberger
Molybdenum Disulfide Nanoflakes Grown by Chemical Vapor Deposition on Graphite: Nucleation, Orientation, and Charge Transfer
J. Phys. Chem. C 124, 2689 (2020)
DOI: 10.1021/acs.jpcc.9b10120
2019
Peter Kratzer and Jörg Neugebauer
The Basics of Electronic Structure Theory for Periodic Systems
Frontiers in Chemistry 7, 106 (2019)
DOI: 10.3389/fchem.2019.00106
Maedeh Zahedifar and Peter Kratzer
Phonon-Induced Electronic Relaxation in a Strongly Correlated System: the Sn/Si(111) (√3×√3) Adlayer Revisited
Phys. Rev. B 100, 125427 (2019)
DOI: 10.1103/PhysRevB.100.125427
Takayuki Suzuki, J. Lawrence, Juliana Maria Morbec, Peter Kratzer and Giovanni Costantini
Surface Structural Phase Transition Induced by the Formation of Metal–Organic Networks on the Si(111)-√7x√3-In Surface
Nanoscale 11, 21790 (2019)
DOI: 10.1039/C9NR07074E
Peter Kratzer and Maedeh Zahedifar
Relaxation of Electrons in Quantum-Confined States in Pb/Si(111) Thin Films from Master Equation with First-Principles-Derived Rates
New J. Phys. 21, 123023 (2019)
DOI: 10.1088/1367-2630/ab5c76
2018
Eugen Speiser, Arne Baumann, Sandhya Chandola, Norbert Esser, Maedeh Zahedifar, Peter Kratzer and Christoph Tegenkamp
Surface Vibrations in the T4 and H3 Pb Phases on Si(111)
Phys. Rev. B 98, 195427 (2018)
DOI: 10.1103/PhysRevB.98.195427
2017
Juliana M. Morbec and Peter Kratzer
The Role of van der Waals Interactions in the Adsorption of Anthracene and Pentacene on the Ag(111) Surface
J. Chem. Phys. 146, 034702 (2017)
DOI: 10.1063/1.4973839
Takayuki Suzuki, J. Lawrence, M. Walker, Juliana Maria Morbec, P. Blowey, K. Yagyu, Peter Kratzer and Giovanni Costantini
Indium Coverage of the Si(111)-√7 x √3–In Surface
Phys. Rev. B 96, 035412 (2017)
DOI: 10.1103/PhysRevB.96.035412
Maedeh Zahedifar and Peter Kratzer
Coupling of Quantum Well States and Phonons in Thin Multilayer Pb Films on Si(111)
Phys. Rev. B 96, 115442 (2017)
DOI: 10.1103/PhysRevB.96.115442