Workflow Overview

This project — Nonadiabatic Molecular Dynamic in Pristine and Methylated Adamantanes —
In addition to the dynamic trajectory method, a single-optimization approach was employed.

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Static Optimization Structure

Optimize the initial crystal structure using the B3LYP functional.

• Input: Optimized CIF files,ORCA and CP2K input files with the appropriate energy_type setting( 4 different systems)

• Output: Ground state and TDDFT output files and corresponding molden files. The TDDFT output files can be further analyzed with Multiwfn to generate UV–Vis spectra in .txt format. Different spectral line shapes and degrees of peak broadening can be obtained by adjusting the full width at half maximum (FWHM).

  Related scripts and examples are available in:

  Static_Optimization_Structure/UV_Vis_spectra

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Nonadiabatic Molecular Dynamics Workflow

Step 1: Adiabatic Molecular Dynamics

• Objective:
  Obtain equilibrated adiabatic trajectories at 300 K.

• Output:
  Equilibrated ground-state molecular-dynamics trajectories for subsequent electronic-structure calculations.

• Additional Note: Restarting a CP2K MD Simulation:

  To continue a previously interrupted CP2K molecular-dynamics simulation, include the following restart settings in the input file:

  &EXT_RESTART
    RESTART_FILE_NAME adamantane_MD-1_5000.restart
    RESTART_DEFAULT T
  &END EXT_RESTART
  
  

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Step 2: TDDFT Calculations

• Input:
  TDDFT Calculations Based on a 300 K Temperature Profile.

• Output:
  For visualizing electronic entropy and UV-Vis spectra.

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Step 3: Vibronic Hamiltonian Construction

• Objective:
  Generate the time-dependent vibronic Hamiltonian using the Step 2 outputs and the selected active space.

• Active space:
  Take adamantane as an example, Orbitals 18–46, with orbital 38 as the HOMO and orbital 39 as the LUMO.

• Output:
  Time-dependent electronic energies, probability distributions and nonadiabatic couplings for the selected electronic states.

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Step 4: Nonadiabatic Molecular Dynamics

• Objective:
  Perform nonadiabatic molecular-dynamics simulations using the Step 3 Hamiltonian data with six different surface-hopping methods: FSSH, FSSH2, GFSH, IDA, IDF, and mSDM.

• Output:
  Determine the timescale using relaxation dynamics.

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