Low-Temperature Solution Synthesis of Transition Metal Dichalcogenide Alloys with Tunable Optical Properties

Yifan Sun, Kazunori Fujisawa, Zhong Lin, Yu Lei, Jared S. Mondschein, Mauricio Terrones Maldonado, Raymond Edward Schaak

Research output: Contribution to journalArticle

15 Citations (Scopus)

Abstract

Nanostructures of layered transition metal dichalcogenide (TMD) alloys with tunable compositions are promising candidates for a broad scope of applications in electronics, optoelectronics, topological devices, and catalysis. Most TMD alloy nanostructures are synthesized as films on substrates using gas-phase methods at high temperatures. However, lower temperature solution routes present an attractive alternative with the potential for larger-scale, higher-yield syntheses of freestanding, higher surface area materials. Here, we report the direct solution synthesis of colloidal few-layer TMD alloys, MoxW1-xSe2 and WS2ySe2(1-y), exhibiting fully tunable metal and chalcogen compositions that span the MoSe2-WSe2 and WS2-WSe2 solid solutions, respectively. Chemical guidelines for achieving the targeted compounds are presented, along with comprehensive structural characterizations (X-ray diffraction, electron microscopy, Raman, and UV-visible spectroscopies). High-resolution microscopic imaging confirms the formation of TMD alloys and identifies a random distribution of the alloyed elements. Analysis of the tilt-angle dependency of the intensities associated with atomic-resolution annular dark field imaging line scans reveals the types of point vacancies present in the samples, thus providing atomic-level insights into the structures of colloidal TMD alloy nanostructures that were previously only accessible for substrate-confined films. The A excitonic transition of the TMD alloy nanostructures can be readily adjusted between 1.51 and 1.93 eV through metal and chalcogen alloying, correlating the compositional modulation to the realization of tunable optical properties.

Original languageEnglish (US)
Pages (from-to)11096-11105
Number of pages10
JournalJournal of the American Chemical Society
Volume139
Issue number32
DOIs
StatePublished - Aug 16 2017

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Transition metal alloys
Optical properties
Metals
Temperature
Nanostructures
Chalcogens
Imaging techniques
Substrates
Chemical analysis
Alloying
Optoelectronic devices
Electron microscopy
Catalysis
Vacancies
Solid solutions
Electronic equipment
Gases
Modulation
X-Ray Diffraction
Spectroscopy

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

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title = "Low-Temperature Solution Synthesis of Transition Metal Dichalcogenide Alloys with Tunable Optical Properties",
abstract = "Nanostructures of layered transition metal dichalcogenide (TMD) alloys with tunable compositions are promising candidates for a broad scope of applications in electronics, optoelectronics, topological devices, and catalysis. Most TMD alloy nanostructures are synthesized as films on substrates using gas-phase methods at high temperatures. However, lower temperature solution routes present an attractive alternative with the potential for larger-scale, higher-yield syntheses of freestanding, higher surface area materials. Here, we report the direct solution synthesis of colloidal few-layer TMD alloys, MoxW1-xSe2 and WS2ySe2(1-y), exhibiting fully tunable metal and chalcogen compositions that span the MoSe2-WSe2 and WS2-WSe2 solid solutions, respectively. Chemical guidelines for achieving the targeted compounds are presented, along with comprehensive structural characterizations (X-ray diffraction, electron microscopy, Raman, and UV-visible spectroscopies). High-resolution microscopic imaging confirms the formation of TMD alloys and identifies a random distribution of the alloyed elements. Analysis of the tilt-angle dependency of the intensities associated with atomic-resolution annular dark field imaging line scans reveals the types of point vacancies present in the samples, thus providing atomic-level insights into the structures of colloidal TMD alloy nanostructures that were previously only accessible for substrate-confined films. The A excitonic transition of the TMD alloy nanostructures can be readily adjusted between 1.51 and 1.93 eV through metal and chalcogen alloying, correlating the compositional modulation to the realization of tunable optical properties.",
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Low-Temperature Solution Synthesis of Transition Metal Dichalcogenide Alloys with Tunable Optical Properties. / Sun, Yifan; Fujisawa, Kazunori; Lin, Zhong; Lei, Yu; Mondschein, Jared S.; Terrones Maldonado, Mauricio; Schaak, Raymond Edward.

In: Journal of the American Chemical Society, Vol. 139, No. 32, 16.08.2017, p. 11096-11105.

Research output: Contribution to journalArticle

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AU - Fujisawa, Kazunori

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AU - Terrones Maldonado, Mauricio

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