From designer clusters to synthetic crystalline nanoassemblies

A. Welford Castleman, Shiv N. Khanna, Ayusman Sen, Arthur C. Reber, Meichun Qian, Kevin M. Davis, Samuel J. Peppernick, Angel Ugrinov, Mark D. Merritt

Research output: Contribution to journalArticlepeer-review

94 Scopus citations

Abstract

Clusters have the potential to serve as building blocks of materials, enabling the tailoring of materials with novel electronic or magnetic properties. Historically, there has been a disconnect between magic clusters found in the gas phase and the synthetic assembly of cluster materials. We approach this challenge through a proposed protocol that combines gas-phase investigations to examine feasible units, theoretical investigations of energetic compositional diagrams and geometrical shapes to identify potential motifs, and synthetic chemical approaches to identify and characterize cluster assemblies in the solid state. Through this approach, we established As 73- as a potential stable species via gas-phase molecular beam experiments consistent with its known existence in molecular crystals with As to K ratios of 7:3. Our protocol also suggests another variant of this material. We report the synthesis of a cluster compound, As7K 1.5(crypt222-K)1.5, composed of a lattice of As 7 clusters stabilized by charge donation from cryptated K atoms and bound by sharing K atoms. The bond dimensions of this supercluster assembled material deduced by X-ray analysis are found to be in excellent agreement with the theoretical calculations. The new compound has a significantly larger band gap than the hitherto known solid. Thus, our approach allows the tuning of the electronic properties of solid cluster assemblies.

Original languageEnglish (US)
Pages (from-to)2734-2741
Number of pages8
JournalNano Letters
Volume7
Issue number9
DOIs
StatePublished - Sep 1 2007

All Science Journal Classification (ASJC) codes

  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering

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