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Ion Mobility-Mass Spectrometry Techniques for Determining the Structure and Mechanisms of Metal Ion Recognition and Redox Activity of Metal Binding Oligopeptides
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First-Principles Nonequilibrium Green's Function Approach to Ultrafast Charge Migration in Glycine.

E Perfetto1, D Sangalli1, M Palummo2

  • 1CNR-ISM, Division of Ultrafast Processes in Materials (FLASHit) , Area della Ricerca di Roma 1 , Via Salaria Km 29.3 , I-00016 Monterotondo Scalo , Italy.

Journal of Chemical Theory and Computation
|July 18, 2019
PubMed
Summary
This summary is machine-generated.

We studied ultrafast charge migration in glycine molecules using a novel nonequilibrium Green

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Area of Science:

  • Computational Chemistry
  • Quantum Dynamics
  • Molecular Physics

Background:

  • Ultrafast charge migration is a fundamental process in molecular systems following photoexcitation.
  • Understanding electron dynamics in molecules like glycine is crucial for fields such as attosecond science and photochemistry.

Purpose of the Study:

  • To investigate the photoinduced ultrafast charge migration in the glycine molecule.
  • To simulate the laser-induced photoionization process and analyze electron dynamics post-pulse.
  • To disentangle polarization and correlation effects on electronic motion.

Main Methods:

  • Utilized a recently proposed nonequilibrium Green's functions (NEGF) approach.
  • Simulated sudden electron removal from valence shells.
  • Explicitly modeled laser-induced photoionization and subsequent system evolution.

Main Results:

  • Achieved satisfactory agreement with available data for electron removal dynamics.
  • Identified and assigned main frequencies to specific elements of the reduced one-particle density matrix.
  • Demonstrated that electronic correlations renormalize frequencies, redistribute spectral weights, and create new spectral features.

Conclusions:

  • The NEGF approach provides a robust framework for studying ultrafast charge migration.
  • Electronic correlations play a significant role in shaping electron dynamics and spectral properties.
  • Detailed insights into glycine's photoinduced electron behavior were obtained.