Analyzing Excitation-Energy Transfer Based on the Time-Dependent Density Functional Theory in Real Time

Schelter, Ingo; Kümmel, Stephan

doi:10.1021/acs.jctc.2c00600

Cited by 7 publications

(2 citation statements)

References 91 publications

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“…On the other hand, when the initial temperature is under the T g , the maximum σ zz seems independent of the temperature. The temperature independence and dependence are attributed to the changes mass density at different temperature, as the density can affect the energy transfer efficiency . As previously discussed in this paper, when the temperature is under T g , it has little effect on the density but changes the density significantly when it is above the T g .…”

Section: Resultssupporting

confidence: 54%

Impact Velocity and Temperature Effects on the Shock Wave Propagation and Spallation of Hydroxyl-Terminated Polybutadiene: A Molecular Dynamics Study

Liu,

He,

Xian

et al. 2023

ACS Appl. Polym. Mater.

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Hydroxyl-terminated polybutadiene (HTPB) is frequently employed as a key component of propellant binder in missiles or solid rockets. Understanding its shock response can help us to deepen our understanding of the shock response in its composites. Considering that missiles or solid rockets often need to operate in various temperature environments, investigating the shock wave propagation within the HTPB and its spallation behaviors under different temperatures and impact velocities is critical for understanding its failure modes. By employing large-scale molecular dynamics simulations, we provide a thorough analysis of the shock propagation and spallation strength of the HTPB under different initial temperatures and impact velocities. The quantification of the spallation strength is done by indirect methods based on the acoustic and modified acoustic assumptions and by the direct method that analyzes atomic stress in the spallation region. Our simulation results reveal that the spallation strength is associated with the impact velocity acting on the materials as well as the initial temperature. When the initial temperature is below the glass transition temperature, the spallation strength exhibits a monotonic decrease with increasing impact velocity. In contrast, such monotonicity is not observed above the glass transition temperature. Our findings furnish insights at the molecular level regarding the spallation processes in HTPB under varying impact loadings and temperature conditions, thereby facilitating the design of HTPB materials with enhanced resistance to impact loading.

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Section: Resultssupporting

confidence: 54%

Impact Velocity and Temperature Effects on the Shock Wave Propagation and Spallation of Hydroxyl-Terminated Polybutadiene: A Molecular Dynamics Study

Liu,

He,

Xian

et al. 2023

ACS Appl. Polym. Mater.

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“…Real-time TDDFT has been used to study electron (and nuclear) dynamics in a myriad of cases: multinucleon transfer reactions through molecular and atomic collisions, 1,2 molecules in oscillating electromagnetic fields of varying strengths, [3][4][5][6][7] high-harmonic generation, 8,9 resonant excitation dynamics (e.g. charge transfer, [10][11][12][13][14] excitation-energy transfer, 15 strong-field ionization, 16 core excitations, [17][18][19] plasmonic excitations 20 ), perturbations in organic, 21 biomolecules, 22 chiral molecules, 23,24 metallic [25][26][27] systems, periodic 28,29 systems, semiconductor materials, 30 optical cavities, 31 electronic stopping 32 etc. Runge and Gross 33 proved that there exists a one-to-one mapping between the time-dependent density of a system and the external potential, justifying the use of TDDFT to simulate time-dependent electronic phenomena.…”

Section: Introductionmentioning

confidence: 99%

Size-dependent errors in real-time electron density propagation

Ranka

Isborn

2023

The Journal of Chemical Physics

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Real-time (RT) electron density propagation with time-dependent density functional theory (TDDFT) or Hartree–Fock (TDHF) is one of the most popular methods to model the charge transfer in molecules and materials. However, both RT-TDHF and RT-TDDFT within the adiabatic approximation are known to produce inaccurate evolution of the electron density away from the ground state in model systems, leading to large errors in charge transfer and erroneous shifting of peaks in absorption spectra. Given the poor performance of these methods with small model systems and the widespread use of the methods with larger molecular and material systems, here we bridge the gap in our understanding of these methods and examine the size-dependence of errors in RT density propagation. We analyze the performance of RT density propagation for systems of increasing size during the application of a continuous resonant field to induce Rabi-like oscillations, during charge-transfer dynamics, and for peak shifting in simulated absorption spectra. We find that the errors in the electron dynamics are indeed size dependent for these phenomena, with the largest system producing the results most aligned with those expected from linear response theory. The results suggest that although the RT-TDHF and RT-TDDFT methods may produce severe errors for model systems, the errors in charge transfer and resonantly driven electron dynamics may be much less significant for more realistic, large-scale molecules and materials.

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QRCODE: Massively parallelized real-time time-dependent density functional theory for periodic systems

Choi,

Okyay,

Dieguez

et al. 2024

Computer Physics Communications

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Analyzing Excitation-Energy Transfer Based on the Time-Dependent Density Functional Theory in Real Time

Cited by 7 publications

References 91 publications

Impact Velocity and Temperature Effects on the Shock Wave Propagation and Spallation of Hydroxyl-Terminated Polybutadiene: A Molecular Dynamics Study

Impact Velocity and Temperature Effects on the Shock Wave Propagation and Spallation of Hydroxyl-Terminated Polybutadiene: A Molecular Dynamics Study

Size-dependent errors in real-time electron density propagation

QRCODE: Massively parallelized real-time time-dependent density functional theory for periodic systems

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