First-Principles Approach for Assessing Cold Electron Injection Efficiency of Dye-Sensitized Solar Cell: Elucidation of Mechanism of Charge Injection and Recombination

Samanta, Pabitra Narayan; Majumdar, D.; Roszak, Szczepan; Leszczynski, Jerzy

doi:10.1021/acs.jpcc.9b10616

Title: First-Principles Approach for Assessing Cold Electron Injection Efficiency of Dye-Sensitized Solar Cell: Elucidation of Mechanism of Charge Injection and Recombination

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Abstract

The adequacy of the inclusion of spacer units in the metal-free D-π–A organic dyes pertaining to the augmentation of dye-sensitized solar cell (DSSC) efficiency has been examined through the excited-state simulations of the charge injection and recombination processes at the dye–semiconductor interface. Within the framework of the time-dependent density functional theory, the proposed computational studies focus on the precise evaluation of pivotal factors controlling the rates of photoinduced charge-transfer and energy-transfer processes, including electronic coupling, reorganization energy, and threshold energy barrier in the semiclassical Marcus formalism. The estimation of the fluorescent state appears to be the crucial step while explaining the ultrafast electron injection process and the charge recombination at the Marcus inverted region, as revealed by the obtained results. The retardation of charge recombination is facilitated by the insertion of a thiophene moiety between the π-bridge and the acceptor units. The estimated cold electron injection efficiencies deploying the Onsager–Braun theory, that rely on the computations of cold electron injection lifetime and cold electron lifetime, show a linear correlation with the experimental photovoltaic parameters of the DSSC comprising short-circuit current density, open-circuit voltage, and power conversion efficiency. The outcomes of the present investigation establish a basis for unraveling the mechanismmore »« less

Authors:

Samanta, Pabitra Narayan ^[1]; Majumdar, D. ^[1]; Roszak, Szczepan ^[2];

^[1]

Jackson State Univ., Jackson, MS (United States)
Wroclaw Univ. of Science and Technology (Poland)

Publication Date:: Fri Jan 17 00:00:00 EST 2020

Research Org.:: Jackson State Univ., Jackson, MS (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1598500

Grant/Contract Number:: SC0018322

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. C

Additional Journal Information:: Journal Volume: 124; Journal Issue: 5; Journal ID: ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 14 SOLAR ENERGY; pi-conjugation; cold electron injection; Dye-sensitized solar cell; Charge recombination

Citation Formats


                    Samanta, Pabitra Narayan, Majumdar, D., Roszak, Szczepan, and Leszczynski, Jerzy. First-Principles Approach for Assessing Cold Electron Injection Efficiency of Dye-Sensitized Solar Cell: Elucidation of Mechanism of Charge Injection and Recombination.  United States: N. p., 2020. 
Web.  doi:10.1021/acs.jpcc.9b10616.

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                    Samanta, Pabitra Narayan, Majumdar, D., Roszak, Szczepan, & Leszczynski, Jerzy. First-Principles Approach for Assessing Cold Electron Injection Efficiency of Dye-Sensitized Solar Cell: Elucidation of Mechanism of Charge Injection and Recombination.  United States.  https://doi.org/10.1021/acs.jpcc.9b10616

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                    Samanta, Pabitra Narayan, Majumdar, D., Roszak, Szczepan, and Leszczynski, Jerzy. Fri .  
"First-Principles Approach for Assessing Cold Electron Injection Efficiency of Dye-Sensitized Solar Cell: Elucidation of Mechanism of Charge Injection and Recombination".  United States.  https://doi.org/10.1021/acs.jpcc.9b10616.  https://www.osti.gov/servlets/purl/1598500.

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@article{osti_1598500,

  title        = {First-Principles Approach for Assessing Cold Electron Injection Efficiency of Dye-Sensitized Solar Cell: Elucidation of Mechanism of Charge Injection and Recombination},

  author       = {Samanta, Pabitra Narayan and Majumdar, D. and Roszak, Szczepan and Leszczynski, Jerzy},

  abstractNote = {The adequacy of the inclusion of spacer units in the metal-free D-π–A organic dyes pertaining to the augmentation of dye-sensitized solar cell (DSSC) efficiency has been examined through the excited-state simulations of the charge injection and recombination processes at the dye–semiconductor interface. Within the framework of the time-dependent density functional theory, the proposed computational studies focus on the precise evaluation of pivotal factors controlling the rates of photoinduced charge-transfer and energy-transfer processes, including electronic coupling, reorganization energy, and threshold energy barrier in the semiclassical Marcus formalism. The estimation of the fluorescent state appears to be the crucial step while explaining the ultrafast electron injection process and the charge recombination at the Marcus inverted region, as revealed by the obtained results. The retardation of charge recombination is facilitated by the insertion of a thiophene moiety between the π-bridge and the acceptor units. The estimated cold electron injection efficiencies deploying the Onsager–Braun theory, that rely on the computations of cold electron injection lifetime and cold electron lifetime, show a linear correlation with the experimental photovoltaic parameters of the DSSC comprising short-circuit current density, open-circuit voltage, and power conversion efficiency. The outcomes of the present investigation establish a basis for unraveling the mechanism of intricate dynamical processes upon photoexcitation of the sensitizers, as well as devising plausible routes for functional DSSC materials.},

  doi          = {10.1021/acs.jpcc.9b10616},

  journal      = {Journal of Physical Chemistry. C},

  number       = 5,

  volume       = 124,

  place        = {United States},

  year         = {Fri Jan 17 00:00:00 EST 2020},

  month        = {Fri Jan 17 00:00:00 EST 2020}

}

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