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Title: Ultrafast Charge Transfer and Hybrid Exciton Formation in 2D/0D Heterostructures

Abstract

We report that photoinduced interfacial charge transfer is at the heart of many applications, including photovoltaics, photocatalysis, and photodetection. With the emergence of a new class of semiconductors such as monolayer two-dimensional transition metal dichalcogenides (2D-TMDs), charge transfer at the 2D/2D heterojunctions attracted several efforts due to the remarkable optical and electrical properties of 2D-TMDs. Unfortunately, in 2D/2D heterojunctions, for a given combination of two materials, the relative energy band alignment and the charge transfer efficiency are locked. Due to their large variety and broad size tunability, semiconductor quantum dots (0D-QDs) interfaced with 2D-TMDs may become an attractive heterostructure for optoelectronic applications. Here, we incorporate femtosecond pump-probe spectroscopy to reveal the sub-45 fs charge transfer at a 2D/0D heterostructure composed of tungsten disulfide monolayers (2D-WS 2) and a single layer of cadmium selenide (CdSe)/zinc sulfide (ZnS) core/shell 0D-QDs. Furthermore, ultrafast dynamics and steady-state measurements suggested that following electron transfer from the 2D to the 0D, hybrid excitons (HXs), wherein the electron resides in the 0D and hole resides in the 2D-TMD monolayer, are formed with a binding energy on the order of ~140 meV, which is several times lower than that of tightly bound excitons in 2D-TMDs.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
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:
1334433
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 138; Journal Issue: 44; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 2D materials; Quantum dots; Hybrid exciton; Binding energy; Ultrafast spectroscopy; Charge transfer

Citation Formats

Boulesbaa, Abdelaziz, Wang, Kai, Mahjouri-Samani, Masoud, Tian, Mengkun, Puretzky, Alexander A., Ivanov, Ilia, Rouleau, Christopher M., Xiao, Kai, Sumpter, Bobby G., and Geohegan, David B. Ultrafast Charge Transfer and Hybrid Exciton Formation in 2D/0D Heterostructures. United States: N. p., 2016. Web. doi:10.1021/jacs.6b08883.
Boulesbaa, Abdelaziz, Wang, Kai, Mahjouri-Samani, Masoud, Tian, Mengkun, Puretzky, Alexander A., Ivanov, Ilia, Rouleau, Christopher M., Xiao, Kai, Sumpter, Bobby G., & Geohegan, David B. Ultrafast Charge Transfer and Hybrid Exciton Formation in 2D/0D Heterostructures. United States. https://doi.org/10.1021/jacs.6b08883
Boulesbaa, Abdelaziz, Wang, Kai, Mahjouri-Samani, Masoud, Tian, Mengkun, Puretzky, Alexander A., Ivanov, Ilia, Rouleau, Christopher M., Xiao, Kai, Sumpter, Bobby G., and Geohegan, David B. Tue . "Ultrafast Charge Transfer and Hybrid Exciton Formation in 2D/0D Heterostructures". United States. https://doi.org/10.1021/jacs.6b08883. https://www.osti.gov/servlets/purl/1334433.
@article{osti_1334433,
title = {Ultrafast Charge Transfer and Hybrid Exciton Formation in 2D/0D Heterostructures},
author = {Boulesbaa, Abdelaziz and Wang, Kai and Mahjouri-Samani, Masoud and Tian, Mengkun and Puretzky, Alexander A. and Ivanov, Ilia and Rouleau, Christopher M. and Xiao, Kai and Sumpter, Bobby G. and Geohegan, David B.},
abstractNote = {We report that photoinduced interfacial charge transfer is at the heart of many applications, including photovoltaics, photocatalysis, and photodetection. With the emergence of a new class of semiconductors such as monolayer two-dimensional transition metal dichalcogenides (2D-TMDs), charge transfer at the 2D/2D heterojunctions attracted several efforts due to the remarkable optical and electrical properties of 2D-TMDs. Unfortunately, in 2D/2D heterojunctions, for a given combination of two materials, the relative energy band alignment and the charge transfer efficiency are locked. Due to their large variety and broad size tunability, semiconductor quantum dots (0D-QDs) interfaced with 2D-TMDs may become an attractive heterostructure for optoelectronic applications. Here, we incorporate femtosecond pump-probe spectroscopy to reveal the sub-45 fs charge transfer at a 2D/0D heterostructure composed of tungsten disulfide monolayers (2D-WS2) and a single layer of cadmium selenide (CdSe)/zinc sulfide (ZnS) core/shell 0D-QDs. Furthermore, ultrafast dynamics and steady-state measurements suggested that following electron transfer from the 2D to the 0D, hybrid excitons (HXs), wherein the electron resides in the 0D and hole resides in the 2D-TMD monolayer, are formed with a binding energy on the order of ~140 meV, which is several times lower than that of tightly bound excitons in 2D-TMDs.},
doi = {10.1021/jacs.6b08883},
url = {https://www.osti.gov/biblio/1334433}, journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 44,
volume = 138,
place = {United States},
year = {2016},
month = {10}
}

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