Manipulation of the dielectric properties of narrow-band gap material by an ultrashort laser pulse

Liu, Zehui; Wang, Feng; Kong, Xiao-Shuang; Zhang, Xiaoqin

doi:10.1016/j.commatsci.2020.109602

Cited by 5 publications

(2 citation statements)

References 51 publications

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“…In the last decade, these experimental advances have been accompanied by the development of first-principles methods that are able to accurately reproduce and interpret these phenomena atomistically. In particular, time-dependent (TD) density functional theory (DFT) in its real-time implementation and in conjunction with the Ehrenfest molecular dynamics scheme , is currently considered one of the most reliable and versatile approaches for describing the electron–nuclear dynamics of molecules and materials in the sub-picosecond timescale. − …”

Section: Introductionmentioning

confidence: 99%

Laser-Induced Electronic and Vibronic Dynamics in the Pyrene Molecule and Its Cation

2021

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Among polycyclic aromatic hydrocarbons, pyrene is widely used as an optical probe thanks to its peculiar ultraviolet absorption and infrared emission features. Interestingly, this molecule is also an abundant component of the interstellar medium, where it is detected via its unique spectral fingerprints. In this work, we present a comprehensive first-principles study on the electronic and vibrational response of pyrene and its cation to ultrafast, coherent pulses in resonance with their optically active excitations in the ultraviolet region. The analysis of molecular symmetries, electronic structure, and linear optical spectra is used to interpret transient absorption spectra and kinetic energy spectral densities computed for the systems excited by ultrashort laser fields. By disentangling the effects of the electronic and vibrational dynamics via ad hoc simulations with stationary and moving ions, and, in specific cases, with the aid of auxiliary model systems, we rationalize that the nuclear motion is mainly harmonic in the neutral species, while strong anharmonic oscillations emerge in the cation, driven by electronic coherence. Our results provide additional insights into the ultrafast vibronic dynamics of pyrene and related compounds and set the stage for future investigations on more complex carbon-conjugated molecules.

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Section: Introductionmentioning

confidence: 99%

Laser-Induced Electronic and Vibronic Dynamics in the Pyrene Molecule and Its Cation

2021

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“…In particular, time-dependent density-functional theory (TDDFT) 46 in its real-time implementation and in conjunction with the Ehrenfest molecular dynamics scheme 47,48 is currently considered one of the most reliable and versatile approaches for describing the electron-nuclear dynamics of molecules and materials in the sub-picosecond timescale. [49][50][51][52][53][54][55][56][57] In this work, we investigate from first principles the ultrafast electronic and vibrational dynamics of pyrene (C 16 H 10 ), a widely studied member of the PAH family, in its neutral form as well as in its positively charged configuration, which is known for its enhanced electronic and vibrational activity. 58,59 Pyrene is characterized by intense absorption and emission bands in the near ultraviolet (UV) region, and by high and long-lived fluorescence yield.…”

Section: Introductionmentioning

confidence: 99%

Laser-Induced Electronic and Vibronic Dynamics in the Pyrene Molecule and its Cation

Herperger,

Krumland,

Cocchi

2021

Preprint

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Among polycyclic aromatic hydrocarbons, pyrene is widely used as an optical probe thanks to peculiar ultraviolet absorption and infrared emission features. Interestingly, this molecule is also an abundant component of the interstellar medium, where it is detected via its unique spectral fingerprints. In this work, we present a comprehensive first-principles study on the electronic and vibrational response of pyrene and its cation to ultrafast, coherent pulses in resonance with their optically active excitations in the ultraviolet region. The analysis of molecular symmetries, electronic structure, and linear optical spectra is used to interpret transient absorption spectra and kinetic energy spectral densities computed for the systems excited by ultrashort laser fields.By disentangling the effects of the electronic and vibrational dynamics via ad hoc simulations with stationary and moving ions, and, in specific cases, with the aid of auxiliary model systems, we rationalize that the nuclear motion is mainly harmonic in the neutral species, while strong anharmonic oscillations emerge in the cation, driven by electronic coherence. Our results provide additional insight into the ultrafast vibronic dynamics of pyrene and related compounds, and set the stage for future investigations on more complex carbon-conjugated molecules.

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Ultrafast laser manufacturing: from physics to industrial applications

et al. 2021

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Manipulation of the dielectric properties of narrow-band gap material by an ultrashort laser pulse

Cited by 5 publications

References 51 publications

Laser-Induced Electronic and Vibronic Dynamics in the Pyrene Molecule and Its Cation

Laser-Induced Electronic and Vibronic Dynamics in the Pyrene Molecule and Its Cation

Laser-Induced Electronic and Vibronic Dynamics in the Pyrene Molecule and its Cation

Ultrafast laser manufacturing: from physics to industrial applications

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