skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Low temperature synthesis of hierarchical TiO2 nanostructures for high performance perovskite solar cells by pulsed laser deposition

Abstract

A promising way to advance perovskite solar cells is to improve the quality of the electron transport material e.g., titanium dioxide (TiO2) in a direction that increases electron transport and extraction. Although dense TiO2 films are easily grown in solution, efficient electron extraction suffers due to a lack of interfacial contact area with the perovskite. Conversely, mesoporous films do offer high surface-area-to-volume ratios, thereby promoting efficient electron extraction, but their morphology is relatively difficult to control via conventional solution synthesis methods. Here, a pulsed laser deposition method was used to assemble TiO2 nanoparticles into TiO2 hierarchical nanoarchitectures having the anatase crystal structure, and prototype solar cells employing these structures yielded power conversion efficiencies of ~ 14%. Our approach demonstrates a way to grow high aspect-ratio TiO2 nanostructures for improved interfacial contact between TiO2 and perovskite materials, leading to high electron-hole pair separation and electron extraction efficiencies for superior photovoltaic performance. In addition, compared to conventional solution-processed TiO2 films that require 500 °C to obtain a good crystallinity, our relatively low temperature (300 °C) TiO2 processing method may promote reduced energy-consumption during device fabrication as well as enable compatibility with various flexible polymer substrates.

Authors:
 [1];  [1];  [1];  [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1329122
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 18; Journal Issue: 39; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 14 SOLAR ENERGY

Citation Formats

Yang, Bin, Mahjouri-Samani, Masoud, Rouleau, Christopher M., Geohegan, David B., and Xiao, Kai. Low temperature synthesis of hierarchical TiO2 nanostructures for high performance perovskite solar cells by pulsed laser deposition. United States: N. p., 2016. Web. https://doi.org/10.1039/C6CP02896A.
Yang, Bin, Mahjouri-Samani, Masoud, Rouleau, Christopher M., Geohegan, David B., & Xiao, Kai. Low temperature synthesis of hierarchical TiO2 nanostructures for high performance perovskite solar cells by pulsed laser deposition. United States. https://doi.org/10.1039/C6CP02896A
Yang, Bin, Mahjouri-Samani, Masoud, Rouleau, Christopher M., Geohegan, David B., and Xiao, Kai. Fri . "Low temperature synthesis of hierarchical TiO2 nanostructures for high performance perovskite solar cells by pulsed laser deposition". United States. https://doi.org/10.1039/C6CP02896A. https://www.osti.gov/servlets/purl/1329122.
@article{osti_1329122,
title = {Low temperature synthesis of hierarchical TiO2 nanostructures for high performance perovskite solar cells by pulsed laser deposition},
author = {Yang, Bin and Mahjouri-Samani, Masoud and Rouleau, Christopher M. and Geohegan, David B. and Xiao, Kai},
abstractNote = {A promising way to advance perovskite solar cells is to improve the quality of the electron transport material e.g., titanium dioxide (TiO2) in a direction that increases electron transport and extraction. Although dense TiO2 films are easily grown in solution, efficient electron extraction suffers due to a lack of interfacial contact area with the perovskite. Conversely, mesoporous films do offer high surface-area-to-volume ratios, thereby promoting efficient electron extraction, but their morphology is relatively difficult to control via conventional solution synthesis methods. Here, a pulsed laser deposition method was used to assemble TiO2 nanoparticles into TiO2 hierarchical nanoarchitectures having the anatase crystal structure, and prototype solar cells employing these structures yielded power conversion efficiencies of ~ 14%. Our approach demonstrates a way to grow high aspect-ratio TiO2 nanostructures for improved interfacial contact between TiO2 and perovskite materials, leading to high electron-hole pair separation and electron extraction efficiencies for superior photovoltaic performance. In addition, compared to conventional solution-processed TiO2 films that require 500 °C to obtain a good crystallinity, our relatively low temperature (300 °C) TiO2 processing method may promote reduced energy-consumption during device fabrication as well as enable compatibility with various flexible polymer substrates.},
doi = {10.1039/C6CP02896A},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 39,
volume = 18,
place = {United States},
year = {2016},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Save / Share:

Works referenced in this record:

Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells
journal, May 2009

  • Kojima, Akihiro; Teshima, Kenjiro; Shirai, Yasuo
  • Journal of the American Chemical Society, Vol. 131, Issue 17, p. 6050-6051
  • DOI: 10.1021/ja809598r

Efficient planar heterojunction perovskite solar cells by vapour deposition
journal, September 2013

  • Liu, Mingzhen; Johnston, Michael B.; Snaith, Henry J.
  • Nature, Vol. 501, Issue 7467, p. 395-398
  • DOI: 10.1038/nature12509

Sequential deposition as a route to high-performance perovskite-sensitized solar cells
journal, July 2013

  • Burschka, Julian; Pellet, Norman; Moon, Soo-Jin
  • Nature, Vol. 499, Issue 7458, p. 316-319
  • DOI: 10.1038/nature12340

6.5% efficient perovskite quantum-dot-sensitized solar cell
journal, January 2011

  • Im, Jeong-Hyeok; Lee, Chang-Ryul; Lee, Jin-Wook
  • Nanoscale, Vol. 3, Issue 10, p. 4088-4093
  • DOI: 10.1039/c1nr10867k

Efficient luminescent solar cells based on tailored mixed-cation perovskites
journal, January 2016


Compositional engineering of perovskite materials for high-performance solar cells
journal, January 2015

  • Jeon, Nam Joong; Noh, Jun Hong; Yang, Woon Seok
  • Nature, Vol. 517, Issue 7535
  • DOI: 10.1038/nature14133

High-performance photovoltaic perovskite layers fabricated through intramolecular exchange
journal, May 2015


Spatial Localization of Excitons and Charge Carriers in Hybrid Perovskite Thin Films
journal, July 2015

  • Simpson, Mary Jane; Doughty, Benjamin; Yang, Bin
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 15
  • DOI: 10.1021/acs.jpclett.5b01050

Elucidation of Perovskite Film Micro-Orientations Using Two-Photon Total Internal Reflectance Fluorescence Microscopy
journal, July 2015

  • Watson, Brianna R.; Yang, Bin; Xiao, Kai
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 16
  • DOI: 10.1021/acs.jpclett.5b01474

Band filling with free charge carriers in organometal halide perovskites
journal, August 2014


Separation of Distinct Photoexcitation Species in Femtosecond Transient Absorption Microscopy
journal, February 2016


Atomistic Origins of High-Performance in Hybrid Halide Perovskite Solar Cells
journal, April 2014

  • Frost, Jarvist M.; Butler, Keith T.; Brivio, Federico
  • Nano Letters, Vol. 14, Issue 5
  • DOI: 10.1021/nl500390f

Impact of microstructure on local carrier lifetime in perovskite solar cells
journal, April 2015


Origin and elimination of photocurrent hysteresis by fullerene passivation in CH3NH3PbI3 planar heterojunction solar cells
journal, December 2014

  • Shao, Yuchuan; Xiao, Zhengguo; Bi, Cheng
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms6784

Long-Range Balanced Electron- and Hole-Transport Lengths in Organic-Inorganic CH3NH3PbI3
journal, October 2013


Perovskite Solar Cells with Near 100% Internal Quantum Efficiency Based on Large Single Crystalline Grains and Vertical Bulk Heterojunctions
journal, July 2015

  • Yang, Bin; Dyck, Ondrej; Poplawsky, Jonathan
  • Journal of the American Chemical Society, Vol. 137, Issue 29
  • DOI: 10.1021/jacs.5b03144

Extremely Slow Photoconductivity Response of CH 3 NH 3 PbI 3 Perovskites Suggesting Structural Changes under Working Conditions
journal, July 2014

  • Gottesman, Ronen; Haltzi, Eynav; Gouda, Laxman
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 15
  • DOI: 10.1021/jz501373f

Room-temperature crystallization of hybrid-perovskite thin films via solvent–solvent extraction for high-performance solar cells
journal, January 2015

  • Zhou, Yuanyuan; Yang, Mengjin; Wu, Wenwen
  • Journal of Materials Chemistry A, Vol. 3, Issue 15
  • DOI: 10.1039/C5TA00477B

Additive Enhanced Crystallization of Solution-Processed Perovskite for Highly Efficient Planar-Heterojunction Solar Cells
journal, March 2014

  • Liang, Po-Wei; Liao, Chien-Yi; Chueh, Chu-Chen
  • Advanced Materials, Vol. 26, Issue 22, p. 3748-3754
  • DOI: 10.1002/adma.201400231

High-efficiency solution-processed perovskite solar cells with millimeter-scale grains
journal, January 2015


Non-wetting surface-driven high-aspect-ratio crystalline grain growth for efficient hybrid perovskite solar cells
journal, July 2015

  • Bi, Cheng; Wang, Qi; Shao, Yuchuan
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8747

Formamidinium lead trihalide: a broadly tunable perovskite for efficient planar heterojunction solar cells
journal, January 2014

  • Eperon, Giles E.; Stranks, Samuel D.; Menelaou, Christopher
  • Energy & Environmental Science, Vol. 7, Issue 3
  • DOI: 10.1039/c3ee43822h

Lead-free solid-state organic–inorganic halide perovskite solar cells
journal, May 2014

  • Hao, Feng; Stoumpos, Constantinos C.; Cao, Duyen Hanh
  • Nature Photonics, Vol. 8, Issue 6
  • DOI: 10.1038/nphoton.2014.82

Electro-optics of perovskite solar cells
journal, December 2014

  • Lin, Qianqian; Armin, Ardalan; Nagiri, Ravi Chandra Raju
  • Nature Photonics, Vol. 9, Issue 2
  • DOI: 10.1038/nphoton.2014.284

Deciphering Halogen Competition in Organometallic Halide Perovskite Growth
journal, March 2016

  • Yang, Bin; Keum, Jong; Ovchinnikova, Olga S.
  • Journal of the American Chemical Society, Vol. 138, Issue 15
  • DOI: 10.1021/jacs.5b13254

Solvent engineering towards controlled grain growth in perovskite planar heterojunction solar cells
journal, January 2015

  • Rong, Yaoguang; Tang, Zhongjia; Zhao, Yufeng
  • Nanoscale, Vol. 7, Issue 24
  • DOI: 10.1039/C5NR02866C

Interface engineering of highly efficient perovskite solar cells
journal, July 2014


Efficiency enhancement of planar perovskite solar cells by adding zwitterion/LiF double interlayers for electron collection
journal, January 2015

  • Sun, Kuan; Chang, Jingjing; Isikgor, Furkan Halis
  • Nanoscale, Vol. 7, Issue 3
  • DOI: 10.1039/C4NR05975A

Effective hole extraction using MoO x -Al contact in perovskite CH 3 NH 3 PbI 3 solar cells
journal, May 2014

  • Zhao, Yixin; Nardes, Alexandre M.; Zhu, Kai
  • Applied Physics Letters, Vol. 104, Issue 21
  • DOI: 10.1063/1.4880899

Nickel Oxide Electrode Interlayer in CH 3 NH 3 PbI 3 Perovskite/PCBM Planar-Heterojunction Hybrid Solar Cells
journal, March 2014

  • Jeng, Jun-Yuan; Chen, Kuo-Cheng; Chiang, Tsung-Yu
  • Advanced Materials, Vol. 26, Issue 24
  • DOI: 10.1002/adma.201306217

Recent Advances in the Inverted Planar Structure of Perovskite Solar Cells
journal, December 2015


Controllable Growth of Perovskite Films by Room-Temperature Air Exposure for Efficient Planar Heterojunction Photovoltaic Cells
journal, October 2015

  • Yang, Bin; Dyck, Ondrej; Poplawsky, Jonathan
  • Angewandte Chemie International Edition, Vol. 54, Issue 49
  • DOI: 10.1002/anie.201505882

The light and shade of perovskite solar cells
journal, August 2014


Synthesis of Monodisperse Mesoporous Titania Beads with Controllable Diameter, High Surface Areas, and Variable Pore Diameters (14−23 nm)
journal, March 2010

  • Chen, Dehong; Cao, Lu; Huang, Fuzhi
  • Journal of the American Chemical Society, Vol. 132, Issue 12, p. 4438-4444
  • DOI: 10.1021/ja100040p

Synthesis of Novel Thin-Film Materials by Pulsed Laser Deposition
journal, August 1996


Gas-phase nanoparticle formation and transport during pulsed laser deposition of Y1Ba2Cu3O7−d
journal, June 1999

  • Geohegan, D. B.; Puretzky, A. A.; Rader, D. J.
  • Applied Physics Letters, Vol. 74, Issue 25
  • DOI: 10.1063/1.124180

Pulsed Laser Deposition of Photoresponsive Two-Dimensional GaSe Nanosheet Networks
journal, August 2014

  • Mahjouri-Samani, Masoud; Gresback, Ryan; Tian, Mengkun
  • Advanced Functional Materials, Vol. 24, Issue 40, p. 6365-6371
  • DOI: 10.1002/adfm.201401440

Time-resolved imaging of gas phase nanoparticle synthesis by laser ablation
journal, June 1998

  • Geohegan, David B.; Puretzky, Alex A.; Duscher, Gerd
  • Applied Physics Letters, Vol. 72, Issue 23
  • DOI: 10.1063/1.121516

Nanostructured TiO2 for energy conversion and storage
journal, January 2013

  • Weng, Zhengyang; Guo, Huan; Liu, Xiangmei
  • RSC Advances, Vol. 3, Issue 47
  • DOI: 10.1039/c3ra44031a

Hyperbranched Quasi-1D Nanostructures for Solid-State Dye-Sensitized Solar Cells
journal, October 2013

  • Passoni, Luca; Ghods, Farbod; Docampo, Pablo
  • ACS Nano, Vol. 7, Issue 11
  • DOI: 10.1021/nn403979h

Hierarchical TiO 2 Photoanode for Dye-Sensitized Solar Cells
journal, July 2010

  • Sauvage, F.; Di Fonzo, F.; Li Bassi, A.
  • Nano Letters, Vol. 10, Issue 7
  • DOI: 10.1021/nl101198b

Hyperbranched Quasi-1D TiO 2 Nanostructure for Hybrid Organic–Inorganic Solar Cells
journal, March 2015

  • Ghadirzadeh, Ali; Passoni, Luca; Grancini, Giulia
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 14
  • DOI: 10.1021/am5090429

Structure and Formation Mechanism of Black TiO 2 Nanoparticles
journal, September 2015


Raman spectrum of anatase, TiO2
journal, December 1978

  • Ohsaka, Toshiaki; Izumi, Fujio; Fujiki, Yoshinori
  • Journal of Raman Spectroscopy, Vol. 7, Issue 6
  • DOI: 10.1002/jrs.1250070606

Efficient organometal trihalide perovskite planar-heterojunction solar cells on flexible polymer substrates
journal, November 2013

  • Docampo, Pablo; Ball, James M.; Darwich, Mariam
  • Nature Communications, Vol. 4, Article No. 2761
  • DOI: 10.1038/ncomms3761

Ultra-thin and smooth transparent electrode for flexible and leakage-free organic light-emitting diodes
journal, March 2015

  • Ok, Ki-Hun; Kim, Jiwan; Park, So-Ra
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep09464

Heat mirror coatings for energy conserving windows
journal, November 1981


Ion Migration in Organometal Trihalide Perovskite and Its Impact on Photovoltaic Efficiency and Stability
journal, January 2016


Ionic transport in hybrid lead iodide perovskite solar cells
journal, June 2015

  • Eames, Christopher; Frost, Jarvist M.; Barnes, Piers R. F.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8497

Anomalous Hysteresis in Perovskite Solar Cells
journal, April 2014

  • Snaith, Henry J.; Abate, Antonio; Ball, James M.
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 9
  • DOI: 10.1021/jz500113x

Charge Accumulation and Hysteresis in Perovskite-Based Solar Cells: An Electro-Optical Analysis
journal, July 2015


    Works referencing / citing this record:

    To Be Higher and Stronger—Metal Oxide Electron Transport Materials for Perovskite Solar Cells
    journal, August 2019


    Polymeric hole-transport materials with side-chain redox-active groups for perovskite solar cells with good reproducibility
    journal, January 2018

    • Fuentes Pineda, Rosinda; Lake, Benjamin R. M.; Troughton, Joel
    • Physical Chemistry Chemical Physics, Vol. 20, Issue 40
    • DOI: 10.1039/c8cp04162h

    A one-step laser process for rapid manufacture of mesoscopic perovskite solar cells prepared under high relative humidity
    journal, January 2018

    • Chen, Qian; Mokhtar, Muhamad Z.; Ke, Jack Chun-Ren
    • Sustainable Energy & Fuels, Vol. 2, Issue 6
    • DOI: 10.1039/c8se00043c

    Pulsed photoinitiated fabrication of inkjet printed titanium dioxide/reduced graphene oxide nanocomposite thin films
    journal, May 2018