Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy

Khalili, Khadijeh; Inhester, Ludger; Arnold, Caroline; Welsch, Ralph; Andreasen, Jens Wenzel; Santra, Robin

doi:10.1063/1.5097653

Title: Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy

Abstract

Theoretical and experimental methodologies that can characterize electronic and nuclear dynamics, and the coupling between the two, are needed to understand photoinduced charge transfer in molecular building blocks used in organic photovoltaics. Ongoing developments in ultrafast pump-probe techniques such as time-resolved X-ray absorption spectroscopy, using an X-ray free electron laser in combination with an ultraviolet femtosecond laser, present desirable probes of coupled electronic and nuclear dynamics. In this work, we investigate the charge transfer dynamics of a donor-acceptor pair, which is widely used as a building block in low bandgap block copolymers for organic photovoltaics. We simulate the dynamics of the benzothiadiazole-thiophene molecule upon photoionization with a vacuum ultraviolet (VUV) pulse and study the potential of probing the subsequent charge dynamics using time-resolved X-ray absorption spectroscopy. The photoinduced dynamics are calculated using on-the-fly nonadiabatic molecular dynamics simulations based on Tully's Fewest Switches Surface Hopping approach. We calculate the X-ray absorption spectrum as a function of time after ionization at the Hartree-Fock level. The changes in the time-resolved X-ray absorption spectrum at the sulfur K-edge reveal the ultrafast charge carrier dynamics in the molecule occurring on a femtosecond time scale. These theoretical findings anticipate that ultrafast time-resolved X-ray absorption spectroscopy usingmore »« less

Authors:

^[1];

^[2];

^[3]; Welsch, Ralph ^[2];

^[1];

^[3]

Technical Univ. of Denmark, Roskilde (Denmark)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); The Hamburg Centre for Ultrafast Imaging, Hamburg (Germany)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); The Hamburg Centre for Ultrafast Imaging, Hamburg (Germany); Univ. of Hamburg (Germany)

Publication Date:: 2019-07-23

Research Org.:: Kansas State Univ., Manhattan, KS (United States)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1613239

Alternate Identifier(s):: OSTI ID: 1544455

Grant/Contract Number:: SC0019451

Resource Type:: Accepted Manuscript

Journal Name:: Structural Dynamics

Additional Journal Information:: Journal Volume: 6; Journal Issue: 4; Journal ID: ISSN 2329-7778

Publisher:: American Crystallographic Association/AIP

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Chemistry; Physics

Citation Formats


                    Khalili, Khadijeh, Inhester, Ludger, Arnold, Caroline, Welsch, Ralph, Andreasen, Jens Wenzel, and Santra, Robin. Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy.  United States: N. p., 2019. 
Web.  doi:10.1063/1.5097653.

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                    Khalili, Khadijeh, Inhester, Ludger, Arnold, Caroline, Welsch, Ralph, Andreasen, Jens Wenzel, & Santra, Robin. Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy.  United States.  https://doi.org/10.1063/1.5097653

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                    Khalili, Khadijeh, Inhester, Ludger, Arnold, Caroline, Welsch, Ralph, Andreasen, Jens Wenzel, and Santra, Robin. Tue .  
"Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy".  United States.  https://doi.org/10.1063/1.5097653.  https://www.osti.gov/servlets/purl/1613239.

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@article{osti_1613239,

  title        = {Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy},

  author       = {Khalili, Khadijeh and Inhester, Ludger and Arnold, Caroline and Welsch, Ralph and Andreasen, Jens Wenzel and Santra, Robin},

  abstractNote = {Theoretical and experimental methodologies that can characterize electronic and nuclear dynamics, and the coupling between the two, are needed to understand photoinduced charge transfer in molecular building blocks used in organic photovoltaics. Ongoing developments in ultrafast pump-probe techniques such as time-resolved X-ray absorption spectroscopy, using an X-ray free electron laser in combination with an ultraviolet femtosecond laser, present desirable probes of coupled electronic and nuclear dynamics. In this work, we investigate the charge transfer dynamics of a donor-acceptor pair, which is widely used as a building block in low bandgap block copolymers for organic photovoltaics. We simulate the dynamics of the benzothiadiazole-thiophene molecule upon photoionization with a vacuum ultraviolet (VUV) pulse and study the potential of probing the subsequent charge dynamics using time-resolved X-ray absorption spectroscopy. The photoinduced dynamics are calculated using on-the-fly nonadiabatic molecular dynamics simulations based on Tully's Fewest Switches Surface Hopping approach. We calculate the X-ray absorption spectrum as a function of time after ionization at the Hartree-Fock level. The changes in the time-resolved X-ray absorption spectrum at the sulfur K-edge reveal the ultrafast charge carrier dynamics in the molecule occurring on a femtosecond time scale. These theoretical findings anticipate that ultrafast time-resolved X-ray absorption spectroscopy using an X-ray probe in combination with a VUV pump offers a new approach to investigate the detailed dynamics of organic photovoltaic materials.},

  doi          = {10.1063/1.5097653},

  journal      = {Structural Dynamics},

  number       = 4,

  volume       = 6,

  place        = {United States},

  year         = {2019},

  month        = {7}

}

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Title: Hole dynamics in a photovoltaic donor-acceptor couple revealed by simulated time-resolved X-ray absorption spectroscopy

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Beyond structure: ultrafast X-ray absorption spectroscopy as a probe of non-adiabatic wavepacket dynamics journal, January 2016

Probing ultrafast ππ*/nπ* internal conversion in organic chromophores via K-edge resonant absorption journal, June 2017

Excited state X-ray absorption spectroscopy: Probing both electronic and structural dynamics journal, October 2016

Control of Local Ionization and Charge Transfer in the Bifunctional Molecule 2-Phenylethyl- N , N -dimethylamine Using Rydberg Fingerprint Spectroscopy journal, March 2005

Low band gap polymers for organic photovoltaics journal, July 2007

Nonadiabatic Molecular Dynamics Based on Trajectories journal, December 2013

Polymer Solar Cells journal, January 1991

Efficiency of bulk-heterojunction organic solar cells journal, December 2013

Molecular Structural Dynamics Probed by Ultrafast X-Ray Absorption Spectroscopy journal, March 2010

Butterfly Deformation Modes in a Photoexcited Pyrazolate-Bridged Pt Complex Measured by Time-Resolved X-Ray Scattering in Solution journal, September 2016

Femtosecond Time-Resolved Photoelectron Spectroscopy journal, April 2004

State-resolved attosecond reversible and irreversible dynamics in strong optical fields journal, February 2017

Coupled perturbed Hartree—Fock equations. An alternative derivation and generalization to non-orthogonal orbitals journal, March 1994

Conjugated Polymer-Based Organic Solar Cells journal, July 2007

Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction journal, April 2017

Polymer Photovoltaic Cells: Enhanced Efficiencies via a Network of Internal Donor-Acceptor Heterojunctions journal, December 1995

Polymer solar cells: Recent development and possible routes for improvement in the performance journal, February 2010

Polymer solar cells journal, February 2012

Charge transfer relaxation in donor–acceptor type conjugated materials journal, January 2013

Derivative studies in hartree-fock and møller-plesset theories journal, March 1979

Concepts in x-ray physics journal, December 2008

Ultrafast Dynamics of Photoionized Acetylene text, January 2011

Orbital-specific mapping of the ligand exchange dynamics of $Fe(CO)_{5}$ in solution text, January 2015

Force Constants and Dipole‐Moment Derivatives of Molecules from Perturbed Hartree–Fock Calculations. I journal, August 1968

Orbital-specific mapping of the ligand exchange dynamics of Fe(CO)5 in solution journal, April 2015

Synthesis and characterization of a thiophene-benzothiadiazole copolymer journal, May 2009

Recent experimental and theoretical developments in time-resolved X-ray spectroscopies journal, October 2014

Molecular dynamics with electronic transitions journal, July 1990

Concepts in x-ray physics journal, July 2009

Femtosecond time-resolved X-ray absorption spectroscopy of anatase TiO2 nanoparticles using XFEL journal, June 2017

Probing wavepacket dynamics using ultrafast x-ray spectroscopy journal, September 2015

Core-level transient absorption spectroscopy as a probe of electron hole relaxation in photoionized H + (H 2 O) n journal, January 2014

Femtosecond Time-Resolved Photoelectron Spectroscopy journal, June 2004

Organic Solar Cells journal, January 1983

Time-resolved X-ray absorption spectroscopy with a water-window high-harmonic source conference, June 2017

Efficient electronic structure calculation for molecular ionization dynamics at high x-ray intensity text, January 2015

Ultrafast X-ray spectroscopy of conical intersections text, January 2018

Simulation of time-resolved x-ray absorption spectroscopy of ultrafast dynamics in particle-hole-excited 4‐(2-thienyl)-2,1,3-benzothiadiazole journal, July 2020

Simulation of time-resolved x-ray absorption spectroscopy of ultrafast dynamics in particle-hole-excited 4‐(2-thienyl)-2,1,3-benzothiadiazole text, January 2020

Femtosecond X-ray Absorption Spectroscopy at a Hard X-ray Free Electron Laser: Application to Spin Crossover Dynamics
journal, January 2013

Matrix Organization and Merit Factor Evaluation as a Method to Address the Challenge of Finding a Polymer Material for Roll Coated Polymer Solar Cells
journal, February 2015

Photoinduced Charge Generation and Recombination Dynamics in Model Donor/Acceptor Pairs for Organic Solar Cell Applications: A Full Quantum-Chemical Treatment
journal, April 2005

X-ray free-electron lasers
journal, November 2010

Concepts in x-ray physics
text, January 2009

Achieving few-femtosecond time-sorting at hard X-ray free-electron lasers
journal, February 2013

Impulsive UV-pump/X-ray probe study of vibrational dynamics in glycine
journal, October 2018

Coherent structural trapping through wave packet dispersion during photoinduced spin state switching
journal, May 2017

Conformational and electronic properties of small benzothiadiazole-cored oligomers with aryl flanking units: Thiophene versus Furan
journal, January 2017

Infrared-laser-pulse-enhanced ultrafast fragmentation of ${N_{2}}^{2 +}$ following Auger decay: Mixed quantum-classical simulations
journal, December 2018

Time-resolved x-ray absorption spectroscopy with a water window high-harmonic source
journal, January 2017

Ultrafast Dynamics of Photoionized Acetylene
journal, December 2011

Ultrafast X-Ray Spectroscopy of Conical Intersections
journal, June 2018

Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses
journal, March 2015

High resolution 1s core hole X-ray spectroscopy in 3d transition metal complexes—electronic and structural information
journal, January 2005

A computer simulation method for the calculation of equilibrium constants for the formation of physical clusters of molecules: Application to small water clusters
journal, January 1982

Challenges in XUV Photochemistry Simulations: A Case Study on Ultrafast Fragmentation Dynamics of the Benzene Radical Cation
journal, January 2018

Models of charge pair generation in organic solar cells
journal, January 2015

Conjugated Polymer-Based Organic Solar Cells
journal, April 2007

Mixed quantum–classical dynamics
journal, January 1998

Ultrafast strong-field dissociative ionization dynamics of CH2Br2 probed by femtosecond soft x-ray transient absorption spectroscopy
journal, May 2008

Infrared-laser-pulse-enhanced ultrafast fragmentation of $N_2^{2+}$ following Auger decay: Mixed quantum-classical simulations
text, January 2018

Solvent control of charge transfer excited state relaxation pathways in [Fe(2,2′-bipyridine)(CN) ₄ ] ²⁻
journal, January 2018

Beyond structure: ultrafast X-ray absorption spectroscopy as a probe of non-adiabatic wavepacket dynamics
journal, January 2016

Probing ultrafast ππ/nπ internal conversion in organic chromophores via K-edge resonant absorption
journal, June 2017

Excited state X-ray absorption spectroscopy: Probing both electronic and structural dynamics
journal, October 2016

Control of Local Ionization and Charge Transfer in the Bifunctional Molecule 2-Phenylethyl- N , N -dimethylamine Using Rydberg Fingerprint Spectroscopy
journal, March 2005

Low band gap polymers for organic photovoltaics
journal, July 2007

Nonadiabatic Molecular Dynamics Based on Trajectories
journal, December 2013

Polymer Solar Cells
journal, January 1991

Efficiency of bulk-heterojunction organic solar cells
journal, December 2013

Molecular Structural Dynamics Probed by Ultrafast X-Ray Absorption Spectroscopy
journal, March 2010

Butterfly Deformation Modes in a Photoexcited Pyrazolate-Bridged Pt Complex Measured by Time-Resolved X-Ray Scattering in Solution
journal, September 2016

Femtosecond Time-Resolved Photoelectron Spectroscopy
journal, April 2004

State-resolved attosecond reversible and irreversible dynamics in strong optical fields
journal, February 2017

Coupled perturbed Hartree—Fock equations. An alternative derivation and generalization to non-orthogonal orbitals
journal, March 1994

Conjugated Polymer-Based Organic Solar Cells
journal, July 2007

Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction
journal, April 2017

Polymer Photovoltaic Cells: Enhanced Efficiencies via a Network of Internal Donor-Acceptor Heterojunctions
journal, December 1995

Polymer solar cells: Recent development and possible routes for improvement in the performance
journal, February 2010

Polymer solar cells
journal, February 2012

Charge transfer relaxation in donor–acceptor type conjugated materials
journal, January 2013

Derivative studies in hartree-fock and møller-plesset theories
journal, March 1979

Concepts in x-ray physics
journal, December 2008

Ultrafast Dynamics of Photoionized Acetylene
text, January 2011

Orbital-specific mapping of the ligand exchange dynamics of $Fe(CO)_{5}$ in solution
text, January 2015

Force Constants and Dipole‐Moment Derivatives of Molecules from Perturbed Hartree–Fock Calculations. I
journal, August 1968

Orbital-specific mapping of the ligand exchange dynamics of Fe(CO)5 in solution
journal, April 2015

Synthesis and characterization of a thiophene-benzothiadiazole copolymer
journal, May 2009

Recent experimental and theoretical developments in time-resolved X-ray spectroscopies
journal, October 2014

Molecular dynamics with electronic transitions
journal, July 1990

Concepts in x-ray physics
journal, July 2009

Femtosecond time-resolved X-ray absorption spectroscopy of anatase TiO2 nanoparticles using XFEL
journal, June 2017

Probing wavepacket dynamics using ultrafast x-ray spectroscopy
journal, September 2015

Core-level transient absorption spectroscopy as a probe of electron hole relaxation in photoionized H ⁺ (H ₂ O) _n
journal, January 2014

Femtosecond Time-Resolved Photoelectron Spectroscopy
journal, June 2004

Organic Solar Cells
journal, January 1983

Time-resolved X-ray absorption spectroscopy with a water-window high-harmonic source
conference, June 2017

Efficient electronic structure calculation for molecular ionization dynamics at high x-ray intensity
text, January 2015

Ultrafast X-ray spectroscopy of conical intersections
text, January 2018

Simulation of time-resolved x-ray absorption spectroscopy of ultrafast dynamics in particle-hole-excited 4‐(2-thienyl)-2,1,3-benzothiadiazole
journal, July 2020

Simulation of time-resolved x-ray absorption spectroscopy of ultrafast dynamics in particle-hole-excited 4‐(2-thienyl)-2,1,3-benzothiadiazole
text, January 2020