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Title: Band Gap Engineering and Layer-by-Layer Band Gap Mapping of Selenium-doped Molybdenum Disulfide

Abstract

Ternary two-dimensional dichalcogenide alloys exhibit compositionally modulated electronic structure and hence, control of dopant concentration within each layer of these layered compounds provides a powerful way to modify their properties. The challenge then becomes quantifying and locating the dopant atoms within each layer in order to better understand and fine-tune the desired properties. Here we report the synthesis of selenium substitutionally doped molybdenum disulfide atomic layers, with a broad range of selenium concentrations, resulting in band gap modulations of over 0.2 eV. Atomic scale chemical analysis using Z-contrast imaging provides direct maps of the dopant atom distribution in individual MoS2 layers and hence a measure of the local band gaps. Furthermore, in a bilayer structure, the dopant distribution of each layer is imaged independently. We demonstrate that each layer in the bilayer contains similar doping levels, randomly distributed, providing new insights into the growth mechanism and alloying behavior in two-dimensional dichalcogenide atomic layers. The results show that growth of uniform, ternary, two-dimensional dichalcogenide alloy films with tunable electronic properties is feasible.

Authors:
 [1];  [1];  [2];  [2];  [2];  [2];  [2];  [1]
  1. Rice University
  2. ORNL
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Shared Research Equipment Collaborative Research Center
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1120453
DOE Contract Number:  
DE-AC05-00OR22725
Resource Type:
Journal Article
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 14; Journal Issue: 2; Journal ID: ISSN 1530--6984
Country of Publication:
United States
Language:
English

Citation Formats

Gong, Yongji, Liu, Zheng, Lupini, Andrew R, Lin, Junhao, Pantelides, Sokrates T, Pennycook, Stephen J, Zhou, Wu, and Ajayan, Pullikel M. Band Gap Engineering and Layer-by-Layer Band Gap Mapping of Selenium-doped Molybdenum Disulfide. United States: N. p., 2014. Web. doi:10.1021/nl4032296.
Gong, Yongji, Liu, Zheng, Lupini, Andrew R, Lin, Junhao, Pantelides, Sokrates T, Pennycook, Stephen J, Zhou, Wu, & Ajayan, Pullikel M. Band Gap Engineering and Layer-by-Layer Band Gap Mapping of Selenium-doped Molybdenum Disulfide. United States. https://doi.org/10.1021/nl4032296
Gong, Yongji, Liu, Zheng, Lupini, Andrew R, Lin, Junhao, Pantelides, Sokrates T, Pennycook, Stephen J, Zhou, Wu, and Ajayan, Pullikel M. 2014. "Band Gap Engineering and Layer-by-Layer Band Gap Mapping of Selenium-doped Molybdenum Disulfide". United States. https://doi.org/10.1021/nl4032296.
@article{osti_1120453,
title = {Band Gap Engineering and Layer-by-Layer Band Gap Mapping of Selenium-doped Molybdenum Disulfide},
author = {Gong, Yongji and Liu, Zheng and Lupini, Andrew R and Lin, Junhao and Pantelides, Sokrates T and Pennycook, Stephen J and Zhou, Wu and Ajayan, Pullikel M},
abstractNote = {Ternary two-dimensional dichalcogenide alloys exhibit compositionally modulated electronic structure and hence, control of dopant concentration within each layer of these layered compounds provides a powerful way to modify their properties. The challenge then becomes quantifying and locating the dopant atoms within each layer in order to better understand and fine-tune the desired properties. Here we report the synthesis of selenium substitutionally doped molybdenum disulfide atomic layers, with a broad range of selenium concentrations, resulting in band gap modulations of over 0.2 eV. Atomic scale chemical analysis using Z-contrast imaging provides direct maps of the dopant atom distribution in individual MoS2 layers and hence a measure of the local band gaps. Furthermore, in a bilayer structure, the dopant distribution of each layer is imaged independently. We demonstrate that each layer in the bilayer contains similar doping levels, randomly distributed, providing new insights into the growth mechanism and alloying behavior in two-dimensional dichalcogenide atomic layers. The results show that growth of uniform, ternary, two-dimensional dichalcogenide alloy films with tunable electronic properties is feasible.},
doi = {10.1021/nl4032296},
url = {https://www.osti.gov/biblio/1120453}, journal = {Nano Letters},
issn = {1530--6984},
number = 2,
volume = 14,
place = {United States},
year = {Wed Jan 01 00:00:00 EST 2014},
month = {Wed Jan 01 00:00:00 EST 2014}
}