Ab initio molecular dynamics simulations of femtosecond-laser-induced anti-Peierls transition in antimony

Zijlstra, Eeuwe S.; Zier, Tobias; Bauerhenne, Bernd; Krylow, Sergej; Garcia, Martín E.

doi:10.1117/12.2214668

Cited by 3 publications

(1 citation statement)

References 14 publications

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“…For the electronic system, CHIVES uses norm-conserving pseudopotentials 35 for the tightly bound core electrons and atom-centered Gaussian basis sets for the less bound valence electrons. The basis set for antimony consists of 18 basis states 36 . Our supercell contains N = 1440 atoms, which shows a good convergence in the quantities of interest and enables us to reach a high q point resolution for the structure function, see also 32 .…”

Section: Methodsmentioning

confidence: 99%

Coherent and incoherent structural dynamics in laser-excited antimony

et al. 2017

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We investigate the excitation of phonons in photoexcited antimony and demonstrate that the entire electron-lattice interactions, in particular coherent and incoherent electron-phonon coupling, can be probed simultaneously. Using femtosecond electron diffraction (FED) with high temporal resolution, we observe the coherent excitation of the fully symmetric A_1g optical phonon mode via the shift of the minimum of the atomic potential energy surface. Ab initio molecular dynamics simulations on laser excited potential energy surfaces are performed to quantify the change in lattice potential and the associated real-space amplitude of the coherent atomic oscillations. Good agreement is obtained between the parameter-free calculations and the experiment. In addition, our experimental configuration allows observing the energy transfer from electrons to phonons via incoherent electron-lattice scattering events. The electron-phonon coupling is determined as a function of electronic temperature from our DFT calculations and the data by applying different models for the energy transfer

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Section: Methodsmentioning

confidence: 99%

Coherent and incoherent structural dynamics in laser-excited antimony

et al. 2017

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Ab-Initio MD Simulations of the Excited Potential Energy Surface

Bauerhenne

2021

Materials Interaction With Femtosecond Lasers

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Real-Time Observation of a Coherent Lattice Transformation into a High-Symmetry Phase

et al. 2018

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†These authors contributed equally to this work Excursions far from their equilibrium structures can bring crystalline solids through collective transformations including transitions into new phases that may be transient or long-lived. Direct spectroscopic observation of far-from-equilibrium rearrangements provides fundamental mechanistic insight into chemical and structural transformations, and a potential route to practical applications, including ultrafast optical control over material structure and properties. However, in many cases photoinduced transitions are irreversible or only slowly reversible, or the light fluence required exceeds material damage thresholds. This precludes conventional ultrafast spectroscopy in which optical excitation and probe pulses irradiate the sample many times, each measurement providing information about the sample response at just one probe delay time following excitation, with each measurement at a high repetition rate and with the sample fully recovering its initial state in between measurements. Using a single-shot, real-time measurement method, we were able to observe the photoinduced phase transition from the semimetallic, lowsymmetry phase of crystalline bismuth into a high-symmetry phase whose existence at high electronic excitation densities was predicted based on earlier measurements at moderate excitation densities below the damage threshold. Our observations indicate that coherent lattice vibrational motion launched upon photoexcitation with an incident fluence above 10 mJ/cm 2 in bulk bismuth brings the lattice structure directly into the high-symmetry configuration for tens of picoseconds, after which carrier relaxation and diffusion restore the equilibrium lattice configuration.

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Ab initio molecular dynamics simulations of femtosecond-laser-induced anti-Peierls transition in antimony

Cited by 3 publications

References 14 publications

Coherent and incoherent structural dynamics in laser-excited antimony

Coherent and incoherent structural dynamics in laser-excited antimony

Ab-Initio MD Simulations of the Excited Potential Energy Surface

Real-Time Observation of a Coherent Lattice Transformation into a High-Symmetry Phase

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