Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Nonlinear electronic excitation in water under proton irradiation: a first principles study

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI: https://doi.org/10.1039/d1cp05313b · OSTI ID:1982194
ORCiD logo [1];  [1]
  1. University of North Carolina at Chapel Hill, NC (United States)
+ Show Author Affiliations

Nonlinear dynamics of electronic excitation bridge physical and physicochemical stages of water radiolysis under proton irradiation, a multi-scale physicochemical process that is fundamental to a wide range of technological and medical applications of high-energy protons. We study the spatial and temporal changes to the excited holes generated in this ionization event using first-principles theory simulation. A significant majority of holes are formed in the immediate vicinity of the irradiating proton paths, and these holes decay rapidly, while secondary excitations are simultaneously induced in regions farther away. While the hole population remains constant, the observed spatially spreading hole distribution cannot be described as concentration-dependent diffusion current. Compared to the primary excitation induced by the irradiating protons, the secondary excitation farther away is somewhat less energetic. Here, the first-principles theory simulation here provides a detailed description of how the primary excitation by proton radiation precedes the formation of cationic holes, which undergo ultrafast chemical processes in water radiolysis.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Argonne Leadership Computing Facility (ALCF)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1982194
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 9 Vol. 24; ISSN 1463-9076; ISSN PPCPFQ
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (48)

Time-Dependent Density Functional Theory Molecular Dynamics Simulations of Liquid Water Radiolysis journal October 2008
Computation of Maximally Localized Wannier Functions using a simultaneous diagonalization algorithm journal September 2003
Smoothing and Differentiation of Data by Simplified Least Squares Procedures. journal July 1964
The “Hole” Story in Ionized Water from the Perspective of Ehrenfest Dynamics journal November 2020
Ionization Energy of Liquid Water Revisited journal January 2020
The missing term in effective pair potentials journal November 1987
Absorption Spectrum of the Hydrated Electron in Water and in Aqueous Solutions journal November 1962
Single, Double, and Multiple Double Strand Breaks Induced in DNA by 3−100 eV Electrons journal April 2003
Electronic Excitation Dynamics in DNA under Proton and α-Particle Irradiation journal March 2019
Radiation from positive particles penetrating the auroral atmosphere journal September 1966
Binding energies, lifetimes and implications of bulk and interface solvated electrons in water journal March 2010
Proton beam radiation induces DNA damage and cell apoptosis in glioma stem cells through reactive oxygen species journal September 2015
Electronic Excitation Dynamics in Liquid Water under Proton Irradiation journal January 2017
Structure of the aqueous electron journal January 2019
Photoabsorption spectra in the continuum of molecules and atomic clusters journal February 2001
The electronic structure of liquid water within density-functional theory journal July 2005
Stopping of energetic light ions in elemental matter journal February 1999
Measurement of energy distributions of secondary electrons ejected from water vapor by fast electrons journal April 1977
Plane-wave pseudopotential implementation of explicit integrators for time-dependent Kohn-Sham equations in large-scale simulations journal December 2012
Retrapping and solvation dynamics after femtosecond UV excitation of the solvated electron in water journal October 1999
Temperature dependence of the hydrated electron’s excited-state relaxation. I. Simulation predictions of resonance Raman and pump-probe transient absorption spectra of cavity and non-cavity models journal August 2017
Simulating electronic excitation and dynamics with real-time propagation approach to TDDFT within plane-wave pseudopotential formulation journal September 2021
An event-by-event computer simulation of interactions of energetic charged particles and all their secondary electrons in water journal March 2000
The treatment of electronic excitations in atomistic models of radiation damage in metals journal October 2010
A multi-scale ab initio theoretical study of the production of free radicals in swift ion tracks in liquid water journal December 2006
Heavy charged particles in radiation biology and biophysics journal July 2008
First-principles calculations for the tunnel ionization rate of atoms and molecules journal May 2004
Optimally smooth norm-conserving pseudopotentials journal December 1985
Maximally localized generalized Wannier functions for composite energy bands journal November 1997
Electronic stopping power in liquid water for protons and α particles from first principles journal July 2016
Electronic stopping for protons and α particles from first-principles electron dynamics: The case of silicon carbide journal September 2016
Examining real-time time-dependent density functional theory nonequilibrium simulations for the calculation of electronic stopping power journal September 2017
Spectra of secondary electrons generated in water by energetic ions journal February 2010
Strongly Constrained and Appropriately Normed Semilocal Density Functional journal July 2015
K -Shell Core-Electron Excitations in Electronic Stopping of Protons in Water from First Principles journal August 2019
Norm-Conserving Pseudopotentials journal November 1979
Excess electrons in liquid water: First evidence of a prehydrated state with femtosecond lifetime journal April 1987
Generalized Gradient Approximation Made Simple journal October 1996
Femtosecond Solvation Dynamics of the Hydrated Electron journal February 1998
Quantum Dynamics Simulation of Electrons in Materials on High-Performance Computers journal September 2014
Insights into Current Limitations of Density Functional Theory journal August 2008
Does the Hydrated Electron Occupy a Cavity? journal July 2010
Observation of the fastest chemical processes in the radiolysis of water journal January 2020
Excited states dynamics in time-dependent density functional theory journal February 2004
The Hydrated Electron journal May 2017
Architecture of Qbox: A scalable first-principles molecular dynamics code journal January 2008
Monte Carlo Simulation of Water Radiolysis for Low-energy Charged Particles journal January 2006
Energy Distribution of Secondary Electrons I. Consistency of Experimental Data journal January 1975

Similar Records

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Chemistry
Physics