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

Title: Ultrafast Exciton Dissociation at the 2D-WS2 Monolayer/Perovskite Interface

Abstract

For an excitonic photovoltaic (PV) device to perform efficiently, photogenerated excitons in the charge donor need to be dissociated through charge transfer (CT) to the acceptor rapidly after their photogeneration and remain separated for a longer time to allow the collection of charges. To improve the efficiency of these steps, several combinations of materials have been examined. Due to their excellent optical properties, two-dimensional transition-metal dichalcogenides (2D-TMDs) have recently been explored. Another promising class of materials to platform efficient PVs is organic–inorganic perovskites. Here, we report on the ultrafast exciton dissociation through electron transfer from a 2D tungsten disulfide (WS2) monolayer to a thin layer of methylammonium lead iodide (CH3NH3PbI3) perovskites. Photoluminescence measurements showed that when the 2D-WS2 monolayer was covered with perovskites, its emission completely quenched, suggesting that the CT process is highly efficient. Despite that pump–probe spectroscopy measurements were carried out with a ~45 fs temporal resolution, the CT dynamics were not captured. A comparison of the ultrafast dynamics of the two band-edge excitons of the charge donor (2D-WS2) suggested that electron transfer is the dominant pathway of CT. Furthermore, these pump–probe measurements indicated that a small fraction of transferred electrons remained in the perovskites up to almostmore » 2 ns. These findings may open a new horizon for understanding the dissociation of photogenerated excitons in 2D-TMDs through hybridization with another class of nanomaterials.« less

Authors:
 [1];  [1];  [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. California State Univ., Northridge, CA (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1607233
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 50; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; excitons; charge transfer; monolayers; hole transfer; perovskites

Citation Formats

Bauer, Joshua, Quintanar, Leo Scott, Wang, Kai, Puretzky, Alexander, Xiao, Kai, Geohegan, David, and Boulesbaa, Abdelaziz. Ultrafast Exciton Dissociation at the 2D-WS2 Monolayer/Perovskite Interface. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.8b08183.
Bauer, Joshua, Quintanar, Leo Scott, Wang, Kai, Puretzky, Alexander, Xiao, Kai, Geohegan, David, & Boulesbaa, Abdelaziz. Ultrafast Exciton Dissociation at the 2D-WS2 Monolayer/Perovskite Interface. United States. https://doi.org/10.1021/acs.jpcc.8b08183
Bauer, Joshua, Quintanar, Leo Scott, Wang, Kai, Puretzky, Alexander, Xiao, Kai, Geohegan, David, and Boulesbaa, Abdelaziz. 2018. "Ultrafast Exciton Dissociation at the 2D-WS2 Monolayer/Perovskite Interface". United States. https://doi.org/10.1021/acs.jpcc.8b08183. https://www.osti.gov/servlets/purl/1607233.
@article{osti_1607233,
title = {Ultrafast Exciton Dissociation at the 2D-WS2 Monolayer/Perovskite Interface},
author = {Bauer, Joshua and Quintanar, Leo Scott and Wang, Kai and Puretzky, Alexander and Xiao, Kai and Geohegan, David and Boulesbaa, Abdelaziz},
abstractNote = {For an excitonic photovoltaic (PV) device to perform efficiently, photogenerated excitons in the charge donor need to be dissociated through charge transfer (CT) to the acceptor rapidly after their photogeneration and remain separated for a longer time to allow the collection of charges. To improve the efficiency of these steps, several combinations of materials have been examined. Due to their excellent optical properties, two-dimensional transition-metal dichalcogenides (2D-TMDs) have recently been explored. Another promising class of materials to platform efficient PVs is organic–inorganic perovskites. Here, we report on the ultrafast exciton dissociation through electron transfer from a 2D tungsten disulfide (WS2) monolayer to a thin layer of methylammonium lead iodide (CH3NH3PbI3) perovskites. Photoluminescence measurements showed that when the 2D-WS2 monolayer was covered with perovskites, its emission completely quenched, suggesting that the CT process is highly efficient. Despite that pump–probe spectroscopy measurements were carried out with a ~45 fs temporal resolution, the CT dynamics were not captured. A comparison of the ultrafast dynamics of the two band-edge excitons of the charge donor (2D-WS2) suggested that electron transfer is the dominant pathway of CT. Furthermore, these pump–probe measurements indicated that a small fraction of transferred electrons remained in the perovskites up to almost 2 ns. These findings may open a new horizon for understanding the dissociation of photogenerated excitons in 2D-TMDs through hybridization with another class of nanomaterials.},
doi = {10.1021/acs.jpcc.8b08183},
url = {https://www.osti.gov/biblio/1607233}, journal = {Journal of Physical Chemistry. C},
issn = {1932-7447},
number = 50,
volume = 122,
place = {United States},
year = {Thu Nov 29 00:00:00 EST 2018},
month = {Thu Nov 29 00:00:00 EST 2018}
}

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

Citation Metrics:
Cited by: 15 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

A low-cost, high-efficiency solar cell based on dye-sensitized colloidal TiO2 films
journal, October 1991


Dye-Sensitized Solar Cells
journal, November 2010


Direct measurement of the exciton binding energy and effective masses for charge carriers in organic–inorganic tri-halide perovskites
journal, June 2015


Monolayer MoS2 Heterojunction Solar Cells
journal, July 2014


Photovoltaic Heterojunctions of Fullerenes with MoS 2 and WS 2 Monolayers
journal, March 2014


Extraordinary Sunlight Absorption and One Nanometer Thick Photovoltaics Using Two-Dimensional Monolayer Materials
journal, July 2013


Spatiotemporal dynamics of excitons in monolayer and bulk WS 2
journal, January 2015


Ultrafast Dynamics of Metal Plasmons Induced by 2D Semiconductor Excitons in Hybrid Nanostructure Arrays
journal, November 2016


Photoluminescence of monolayer MoS 2 on LaAlO 3 and SrTiO 3 substrates
journal, January 2014


Tightly Bound Excitons in Monolayer WSe 2
journal, July 2014


Binding energies and structures of two-dimensional excitonic complexes in transition metal dichalcogenides
journal, March 2016


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


Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites
journal, October 2012


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


The emergence of perovskite solar cells
journal, July 2014


High Efficiency Solid-State Sensitized Solar Cell-Based on Submicrometer Rutile TiO2 Nanorod and CH3NH3PbI3 Perovskite Sensitizer
journal, May 2013


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


Recent advances in perovskite solar cells: efficiency, stability and lead-free perovskite
journal, January 2017


Hybrid Bilayer WSe 2 -CH 3 NH 3 PbI 3 Organolead Halide Perovskite as a High-Performance Photodetector
journal, September 2016


van der Waals Heterojunction Devices Based on Organohalide Perovskites and Two-Dimensional Materials
journal, December 2015


Ultrasmooth organic–inorganic perovskite thin-film formation and crystallization for efficient planar heterojunction solar cells
journal, January 2015


Pinhole-free perovskite films for efficient solar modules
journal, January 2016


Chlorine Incorporation for Enhanced Performance of Planar Perovskite Solar Cell Based on Lead Acetate Precursor
journal, October 2015


Ultrafast Charge Transfer and Hybrid Exciton Formation in 2D/0D Heterostructures
journal, October 2016


Observation of two distinct negative trions in tungsten disulfide monolayers
journal, September 2015


Exciton valley relaxation in a single layer of WS 2 measured by ultrafast spectroscopy
journal, July 2014


Large spin splitting in the conduction band of transition metal dichalcogenide monolayers
journal, December 2013


Band offsets and heterostructures of two-dimensional semiconductors
journal, January 2013


Ultrafast charge transfer in atomically thin MoS2/WS2 heterostructures
journal, August 2014


Ultrafast formation of interlayer hot excitons in atomically thin MoS2/WS2 heterostructures
journal, August 2016


Type-I van der Waals heterostructure formed by MoS 2 and ReS 2 monolayers
journal, January 2017


The effect of the substrate on the Raman and photoluminescence emission of single-layer MoS2
journal, April 2014


Exciton Dynamics in Suspended Monolayer and Few-Layer MoS 2 2D Crystals
journal, January 2013


Ultrafast Dynamics of Defect-Assisted Electron–Hole Recombination in Monolayer MoS 2
journal, December 2014


Exciton dynamics in monolayer transition metal dichalcogenides
journal, January 2016


Transient Absorption Microscopy of Monolayer and Bulk WSe 2
journal, February 2014


Influence of hydration water on CH_3NH_3PbI_3 perovskite films prepared through one-step procedure
journal, January 2016


Highly mobile charge-transfer excitons in two-dimensional WS 2 /tetracene heterostructures
journal, January 2018


Works referencing / citing this record:

Spintronics of Hybrid Organic–Inorganic Perovskites: Miraculous Basis of Integrated Optoelectronic Devices
journal, June 2019