Title: Rational Design of Dithienopicenocarbazole-Based Dyes and a Prediction of Their Energy-Conversion Efficiency Characteristics for Dye-Sensitized Solar Cells

Abstract

Here, a series of metal-free organic donor-acceptor (D-A) derivatives (ME01-ME06) of the known dye C281 were designed using first principles calculations in order to evaluate their potential for applications in dye-sensitized solar cells (DSSCs). Their physical and electronic properties were calculated using density functional theory (DFT) and time-dependent density functional theory (TD-DFT). These include molecular properties that are required to assess the feasibility of a dye to function in DSSCs: UV/vis absorption spectra, light-harvesting efficiency (LHE), and driving forces of electron injection (ΔG_inj). ME01, ME02, and ME04 are predicted to exhibit broad absorption optical spectra that cover the entire visible range, rendering these three dyes promising DSSC prospects. Device-relevant calculations on these three short-listed dyes and the parent dye C281 were then performed, whereupon the dye molecules were adsorbed onto anatase TiO₂ surfaces to form the DSSC working electrode. Associated DSSC device characteristics of this dye…TiO₂ interfacial structure were determined. These include the light-harvesting efficiency, the number of injected electrons, the electron-injection lifetime, and the quantum energy alignment of the adsorbed dye molecule to that of its device components. In turn, these calculated parameters enabled the derivation of the DSSC device performance parameters: short-circuit current density, J_SC, incident photon-to-electron conversionmore » efficiency, IPCE, and open-circuit voltage, V_OC. Thus, we demonstrate a systematic ab initio approach to screen rationally designed D-A dyes with respect to their potential applicability in high-performance DSSC devices.« less

Authors:

Yang, Zhenqing  ^[1];

• Search DOE PAGES for author "Yang, Zhenqing"
• Search DOE PAGES for ORCID "0000-0001-7453-2761"

Liu, Chunmeng ^[2]; Li, Kuan ^[2]; Cole, Jacqueline M.  ^[3];

• Search DOE PAGES for author "Cole, Jacqueline M."
• Search DOE PAGES for ORCID "0000-0002-1552-8743"

Shao, Changjin ^[2]; Cao, Dapeng  ^[4]

• Search DOE PAGES for author "Cao, Dapeng"
• Search DOE PAGES for ORCID "0000-0002-6981-7794"

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+ Show Author Affiliations

1. China Univ. of Petroleum, Beijing (People's Republic of China); Univ. of Cambridge, Cambridge (United Kingdom)
2. China Univ. of Petroleum, Beijing (People's Republic of China)
3. Univ. of Cambridge, Cambridge (United Kingdom); Rutherford Appleton Lab., Oxfordshire (United Kingdom); Argonne National Lab. (ANL), Argonne, IL (United States)
4. Beijing Univ. of Chemical Technology, Beijing (People's Republic of China)

Publication Date:

Tue Mar 13 00:00:00 EDT 2018

Research Org.:

Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1491748

Grant/Contract Number:  

AC02-06CH11357

Resource Type:

Accepted Manuscript

Journal Name:

ACS Applied Energy Materials

Additional Journal Information:

Journal Volume: 1; Journal Issue: 4; Journal ID: ISSN 2574-0962

Publisher:

American Chemical Society (ACS)

Country of Publication:

United States

Language:

English

Subject:

14 SOLAR ENERGY; DFT/TD-DFT; Metal-free organic dyes; absorption spectrum; donor-acceptor (D-A); dye-sensitized solar cells