Synthesis and fundamental studies of (H3Ge)xSiH 4-x molecules: Precursors to semiconductor hetero- and nanostructures on Si

Cole J. Ritter, Changwu Hu, Andrew Chizmeshya, John Tolle, Douglas Klewer, Ignatius S T Tsong, John Kouvetakis

Research output: Contribution to journalArticle

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Abstract

The synthesis of the entire silyl-germyl sequence of molecules (H 3Ge)xSiH4-x (x = 1-4) has been demonstrated. These include the previously unknown (H3Ge)2SiH 2, (H3Ge)3SiH, and (H3Ge) 4Si species as well as the H3GeSiH3 analogue which is obtained in practical high-purity yields as a viable alternative to disilane and digermane for semiconductor applications. The molecules are characterized by FTIR, multinuclear NMR, mass spectrometry, and Rutherford backscattering. The structural, thermochemical, and vibrational properties are studied using density functional theory. A detailed comparison of the experimental and theoretical data is used to corroborate the synthesis of specific molecular structures. The (H3Ge)xSiH 4-x family of compounds described here is not only of intrinsic molecular interest but also provides a unique route to a new class of Si-based semiconductors including epitaxial layers and coherent islands (quantum dots), with Ge-rich stoichiometries SiGe, SiGe2, SiGe3, and SiGe4 reflecting the Si/Ge content of the corresponding precursor. The layers grow directly on Si(100) at unprecedented low temperatures of 300-450 °C and display homogeneous compositional and strain profiles, low threading defect densities, and atomically planar surfaces circumventing entirely the need for conventional graded compositions or lift-off technologies. The activation energies of all Si-Ge hydride reactions on Si(100) (Ea ≈ 1.5-2.0 eV) indicate high reactivity profiles with respect to H2 desorption, consistent with the low growth temperatures of the films. The quantum dots are obtained exclusively at higher temperatures (T > 500 °C) and represent a new family of Ge-rich compositions with narrow size distribution, defect-free microstructures, and homogeneous, precisely tuned elemental content at the atomic level.

Original languageEnglish (US)
Pages (from-to)9855-9864
Number of pages10
JournalJournal of the American Chemical Society
Volume127
Issue number27
DOIs
StatePublished - Jul 13 2005

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Semiconductors
Nanostructures
Semiconductor quantum dots
Heterojunctions
Quantum Dots
Semiconductor materials
Molecules
Temperature
Defect density
Epitaxial layers
Rutherford backscattering spectroscopy
Growth temperature
Chemical analysis
Hydrides
Stoichiometry
Molecular structure
Biomolecular Nuclear Magnetic Resonance
Density functional theory
Mass spectrometry
Desorption

ASJC Scopus subject areas

  • Chemistry(all)

Cite this

Synthesis and fundamental studies of (H3Ge)xSiH 4-x molecules : Precursors to semiconductor hetero- and nanostructures on Si. / Ritter, Cole J.; Hu, Changwu; Chizmeshya, Andrew; Tolle, John; Klewer, Douglas; Tsong, Ignatius S T; Kouvetakis, John.

In: Journal of the American Chemical Society, Vol. 127, No. 27, 13.07.2005, p. 9855-9864.

Research output: Contribution to journalArticle

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abstract = "The synthesis of the entire silyl-germyl sequence of molecules (H 3Ge)xSiH4-x (x = 1-4) has been demonstrated. These include the previously unknown (H3Ge)2SiH 2, (H3Ge)3SiH, and (H3Ge) 4Si species as well as the H3GeSiH3 analogue which is obtained in practical high-purity yields as a viable alternative to disilane and digermane for semiconductor applications. The molecules are characterized by FTIR, multinuclear NMR, mass spectrometry, and Rutherford backscattering. The structural, thermochemical, and vibrational properties are studied using density functional theory. A detailed comparison of the experimental and theoretical data is used to corroborate the synthesis of specific molecular structures. The (H3Ge)xSiH 4-x family of compounds described here is not only of intrinsic molecular interest but also provides a unique route to a new class of Si-based semiconductors including epitaxial layers and coherent islands (quantum dots), with Ge-rich stoichiometries SiGe, SiGe2, SiGe3, and SiGe4 reflecting the Si/Ge content of the corresponding precursor. The layers grow directly on Si(100) at unprecedented low temperatures of 300-450 °C and display homogeneous compositional and strain profiles, low threading defect densities, and atomically planar surfaces circumventing entirely the need for conventional graded compositions or lift-off technologies. The activation energies of all Si-Ge hydride reactions on Si(100) (Ea ≈ 1.5-2.0 eV) indicate high reactivity profiles with respect to H2 desorption, consistent with the low growth temperatures of the films. The quantum dots are obtained exclusively at higher temperatures (T > 500 °C) and represent a new family of Ge-rich compositions with narrow size distribution, defect-free microstructures, and homogeneous, precisely tuned elemental content at the atomic level.",
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