Abstract

High quality stoichiometric lead sulfide (PbS) wires were synthesized by a simple chemical vapor deposition (CVD) process using pure PbS powder as the material source. Growth mechanisms were systematically investigated under various growth conditions, with three modes of growth identified: direct vapor-liquid-solid (VLS) wire growth nucleating from the substrate surface, bulk PbS crystallites by vapor-solid (VS) deposition, and subsequent VLS growth nucleating on top of the bulk deposition through spontaneously formed catalyst particles. Furthermore, we found that these growth modes can be organized in terms of different levels of supersaturation, with VS bulk deposition dominating at high supersaturation and VLS wire growth on the substrate dominating at low supersaturation. At intermediate supersaturation, the bulk VS deposition can form larger crystallites with domains of similarly oriented wires extending from the flat facets. Both predeposited catalysts and spontaneously formed Pb particles were observed as nucleation catalysts, and their interplay leads to various interesting growth scenarios such as reversely tapered growth with increasing diameter. The VLS growth mechanism was confirmed by the presence of Pb-rich caps revealed in an elaborate cross-sectional transmission electron microscopy (TEM) experiment after focused ion beam milling in a modified lift-out procedure. Temperature-dependent photoluminescence (PL) of PbS wires was performed in the mid-infrared wavelength range for the first time, demonstrating strong light emission from band edge, blue-shifted with increasing temperature. The high optical quality of PbS wires may lead to important applications in mid-infrared photonics. The substrate growth temperature as low as 400 °C allows for silicon-compatible processing for integrated optoelectronics applications.

Original languageEnglish (US)
Pages (from-to)8730-8738
Number of pages9
JournalACS Nano
Volume5
Issue number11
DOIs
StatePublished - Nov 22 2011

Fingerprint

Supersaturation
supersaturation
wire
Wire
catalysts
Catalysts
Vapors
vapors
Liquids
Crystallites
liquids
crystallites
Substrates
Infrared radiation
Integrated optoelectronics
lead sulfides
Focused ion beams
Light emission
Growth temperature
Silicon

Keywords

  • chemical vapor deposition
  • infrared photonics
  • lead sulfide
  • photoluminescence
  • supersaturation
  • vapor-liquid-solid growth

ASJC Scopus subject areas

  • Engineering(all)
  • Materials Science(all)
  • Physics and Astronomy(all)

Cite this

Influence of supersaturation and spontaneous catalyst formation on the growth of PbS wires : Toward a unified understanding of growth modes. / Nichols, Patricia L.; Sun, Minghua; Ning, Cun-Zheng.

In: ACS Nano, Vol. 5, No. 11, 22.11.2011, p. 8730-8738.

Research output: Contribution to journalArticle

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N2 - High quality stoichiometric lead sulfide (PbS) wires were synthesized by a simple chemical vapor deposition (CVD) process using pure PbS powder as the material source. Growth mechanisms were systematically investigated under various growth conditions, with three modes of growth identified: direct vapor-liquid-solid (VLS) wire growth nucleating from the substrate surface, bulk PbS crystallites by vapor-solid (VS) deposition, and subsequent VLS growth nucleating on top of the bulk deposition through spontaneously formed catalyst particles. Furthermore, we found that these growth modes can be organized in terms of different levels of supersaturation, with VS bulk deposition dominating at high supersaturation and VLS wire growth on the substrate dominating at low supersaturation. At intermediate supersaturation, the bulk VS deposition can form larger crystallites with domains of similarly oriented wires extending from the flat facets. Both predeposited catalysts and spontaneously formed Pb particles were observed as nucleation catalysts, and their interplay leads to various interesting growth scenarios such as reversely tapered growth with increasing diameter. The VLS growth mechanism was confirmed by the presence of Pb-rich caps revealed in an elaborate cross-sectional transmission electron microscopy (TEM) experiment after focused ion beam milling in a modified lift-out procedure. Temperature-dependent photoluminescence (PL) of PbS wires was performed in the mid-infrared wavelength range for the first time, demonstrating strong light emission from band edge, blue-shifted with increasing temperature. The high optical quality of PbS wires may lead to important applications in mid-infrared photonics. The substrate growth temperature as low as 400 °C allows for silicon-compatible processing for integrated optoelectronics applications.

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