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

Title: Transition-Metal Substitution Doping in Synthetic Atomically Thin Semiconductors

Abstract

Semiconductor impurity doping has enabled an entire generation of technology. The emergence of alternative semiconductor material systems, such as transition metal dichalcogenides (TMDCs), requires the development of scalable doping strategies. We report an unprecedented one-pot synthesis for transition-metal substitution in large-area, synthetic monolayer TMDCs. Electron microscopy, optical and electronic transport characterization and ab initio calculations indicate that our doping strategy preserves the attractive qualities of TMDC monolayers, including semiconducting transport and strong direct-gap luminescence. These results are expected to encourage exploration of transition-metal substitution in two-dimensional systems, potentially enabling next-generation optoelectronic technology in the atomically-thin regime.

Authors:
 [1];  [2];  [3];  [4];  [1];  [1];  [1];  [5];  [4];  [6];  [6];  [2];  [7]
  1. Rensselaer Polytechnic Inst., Troy, NY (United States). Dept. of Materials Science and Engineering
  2. Columbia Univ., New York, NY (United States). Dept. of Mechanical Engineering
  3. Rensselaer Polytechnic Inst., Troy, NY (United States). Dept. of Physics, Applied Physics and Astronomy; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  5. Rensselaer Polytechnic Inst., Troy, NY (United States). Dept. of Mechanical, Aerospace and Nuclear Engineering
  6. Rensselaer Polytechnic Inst., Troy, NY (United States). Dept. of Physics, Applied Physics and Astronomy
  7. Rensselaer Polytechnic Inst., Troy, NY (United States). Dept. of Materials Science and Engineering ; Rensselaer Polytechnic Inst., Troy, NY (United States). Dept. of Mechanical, Aerospace and Nuclear Engineering
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF); US Department of the Navy, Office of Naval Research (ONR)
OSTI Identifier:
1334421
Grant/Contract Number:
AC05-00OR22725; 1435783; 1510828; 1608171; DMR-1420634
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 28; Journal Issue: 44; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; band structure; chemical vapor deposition; electronic properties; monolayer transition-metal dichalcogenides; transition-metal doping

Citation Formats

Gao, Jian, Kim, Young Duck, Liang, Liangbo, Idrobo, Juan Carlos, Chow, Phil, Tan, Jiawei, Li, Baichang, Li, Lu, Sumpter, Bobby G., Lu, Toh-Ming, Meunier, Vincent, Hone, James, and Koratkar, Nikhil. Transition-Metal Substitution Doping in Synthetic Atomically Thin Semiconductors. United States: N. p., 2016. Web. doi:10.1002/adma.201601104.
Gao, Jian, Kim, Young Duck, Liang, Liangbo, Idrobo, Juan Carlos, Chow, Phil, Tan, Jiawei, Li, Baichang, Li, Lu, Sumpter, Bobby G., Lu, Toh-Ming, Meunier, Vincent, Hone, James, & Koratkar, Nikhil. Transition-Metal Substitution Doping in Synthetic Atomically Thin Semiconductors. United States. doi:10.1002/adma.201601104.
Gao, Jian, Kim, Young Duck, Liang, Liangbo, Idrobo, Juan Carlos, Chow, Phil, Tan, Jiawei, Li, Baichang, Li, Lu, Sumpter, Bobby G., Lu, Toh-Ming, Meunier, Vincent, Hone, James, and Koratkar, Nikhil. 2016. "Transition-Metal Substitution Doping in Synthetic Atomically Thin Semiconductors". United States. doi:10.1002/adma.201601104. https://www.osti.gov/servlets/purl/1334421.
@article{osti_1334421,
title = {Transition-Metal Substitution Doping in Synthetic Atomically Thin Semiconductors},
author = {Gao, Jian and Kim, Young Duck and Liang, Liangbo and Idrobo, Juan Carlos and Chow, Phil and Tan, Jiawei and Li, Baichang and Li, Lu and Sumpter, Bobby G. and Lu, Toh-Ming and Meunier, Vincent and Hone, James and Koratkar, Nikhil},
abstractNote = {Semiconductor impurity doping has enabled an entire generation of technology. The emergence of alternative semiconductor material systems, such as transition metal dichalcogenides (TMDCs), requires the development of scalable doping strategies. We report an unprecedented one-pot synthesis for transition-metal substitution in large-area, synthetic monolayer TMDCs. Electron microscopy, optical and electronic transport characterization and ab initio calculations indicate that our doping strategy preserves the attractive qualities of TMDC monolayers, including semiconducting transport and strong direct-gap luminescence. These results are expected to encourage exploration of transition-metal substitution in two-dimensional systems, potentially enabling next-generation optoelectronic technology in the atomically-thin regime.},
doi = {10.1002/adma.201601104},
journal = {Advanced Materials},
number = 44,
volume = 28,
place = {United States},
year = 2016,
month = 9
}

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

Citation Metrics:
Cited by: 2works
Citation information provided by
Web of Science

Save / Share:
  • Two-dimensional layered materials have attracted considerable attention since the discovery of graphene. Here we demonstrate that the layered Bi{sub 2}Sr{sub 2}Co{sub 2}O{sub 8} (BSCO) can be mechanically exfoliated into single- or few-layer nanosheets. The BSCO nanosheets with four or more layers display bulk metallic characteristics, while the nanosheets with three or fewer layers have a layer-number-dependent semiconducting characteristics. Charge transport in bilayer or trilayer BSCO nanosheets exhibits Mott 2D variable-range-hopping (VRH) conduction throughout 2 K–300 K, while the charge transport in monolayers follows the Mott-VRH law above a crossover temperature of 75 K, and is governed by Efros and Shklovskii-VRHmore » laws below 75 K. Disorder potentials and Coulomb charging both contribute to the transport gap of these nanodevices. Our study reveals a distinct layer number-dependent metal-to-semiconductor transition in a new class of 2D materials, and is of great significance for both fundamental investigations and practical devices.« less
  • Transition metal dichalcogenide semiconductors represent elementary components of layered heterostructures for emergent technologies beyond conventional opto-electronics. In their monolayer form they host electrons with quantized circular motion and associated valley polarization and valley coherence as key elements of opto-valleytronic functionality. Here, we introduce two-dimensional polarimetry as means of direct imaging of the valley pseudospin degree of freedom in monolayer transition metal dichalcogenides. Using MoS 2 as a representative material with valley-selective optical transitions, we establish quantitative image analysis for polarimetric maps of extended crystals, and identify valley polarization and valley coherence as sensitive probes of crystalline disorder. Moreover, we findmore » site-dependent thermal and non-thermal regimes of valley-polarized excitons in perpendicular magnetic fields. Finally, we demonstrate the potential of widefield polarimetry for rapid inspection of opto-valleytronic devices based on atomically thin semiconductors and heterostructures.« less
  • The research on emerging layered two-dimensional (2D) semiconductors, such as molybdenum disulfide (MoS 2), reveals unique optical properties generating significant interest. Experimentally, these materials were observed to host extremely strong light-matter interactions as a result of the enhanced excitonic effect in two dimensions. Thus, understanding and manipulating the excitons are crucial to unlocking the potential of 2D materials for future photonic and optoelectronic devices. Here in this review, we unravel the physical origin of the strong excitonic effect and unique optical selection rules in 2D semiconductors. In addition, control of these excitons by optical, electrical, as well as mechanical meansmore » is examined. Finally, the resultant devices such as excitonic light emitting diodes, lasers, optical modulators, and coupling in an optical cavity are overviewed, demonstrating how excitons can shape future 2D optoelectronics.« less