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Title: Hybrid metal–organic chalcogenide nanowires with electrically conductive inorganic core through diamondoid-directed assembly

Abstract

Controlling inorganic structure and dimensionality through structure-directing agents is a versatile approach for new materials synthesis that has been used extensively for metal–organic frameworks and coordination polymers. However, the lack of ‘solid’ inorganic cores requires charge transport through single-atom chains and/or organic groups, limiting their electronic properties. Here, we report that strongly interacting diamondoid structure-directing agents guide the growth of hybrid metal–organic chalcogenide nanowires with solid inorganic cores having three-atom cross-sections, representing the smallest possible nanowires. The strong van der Waals attraction between diamondoids overcomes steric repulsion leading to a cis configuration at the active growth front, enabling face-on addition of precursors for nanowire elongation. These nanowires have band-like electronic properties, low effective carrier masses and three orders-of-magnitude conductivity modulation by hole doping. Furthermore, this discovery highlights a previously unexplored regime of structure-directing agents compared with traditional surfactant, block copolymer or metal–organic framework linkers.

Authors:
 [1];  [2];  [1];  [3];  [4];  [1];  [3];  [3];  [5];  [5]; ORCiD logo [5];  [6];  [1];  [3];  [3];  [1]
  1. Stanford Institute for Materials and Energy Sciences, Stanford, CA (United States); Dept. of Materials Science and Engineering, Stanford, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Stanford Institute for Materials and Energy Sciences, Stanford, CA (United States)
  4. Univ. Nacional Autonoma de Mexico, Coyoacan (Mexico)
  5. Justus-Liebig Univ., Giessen (Germany)
  6. Stanford Univ., Stanford, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1331967
Alternate Identifier(s):
OSTI ID: 1459387
Report Number(s):
SLAC-PUB-16852
Journal ID: ISSN 1476-1122
Grant/Contract Number:  
AC02-76SF00515; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 16; Journal Issue: 3; Journal ID: ISSN 1476-1122
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CHEM; MATSCI; SYNCHRAD

Citation Formats

Yan, Hao, Hohman, J. Nathan, Li, Fei Hua, Jia, Chunjing, Solis-Ibarra, Diego, Wu, Bin, Dahl, Jeremy E. P., Carlson, Robert M. K., Tkachenko, Boryslav A., Fokin, Andrey A., Schreiner, Peter R., Vailionis, Arturas, Kim, Taeho Roy, Devereaux, Thomas P., Shen, Zhi -Xun, and Melosh, Nicholas A. Hybrid metal–organic chalcogenide nanowires with electrically conductive inorganic core through diamondoid-directed assembly. United States: N. p., 2016. Web. doi:10.1038/nmat4823.
Yan, Hao, Hohman, J. Nathan, Li, Fei Hua, Jia, Chunjing, Solis-Ibarra, Diego, Wu, Bin, Dahl, Jeremy E. P., Carlson, Robert M. K., Tkachenko, Boryslav A., Fokin, Andrey A., Schreiner, Peter R., Vailionis, Arturas, Kim, Taeho Roy, Devereaux, Thomas P., Shen, Zhi -Xun, & Melosh, Nicholas A. Hybrid metal–organic chalcogenide nanowires with electrically conductive inorganic core through diamondoid-directed assembly. United States. doi:10.1038/nmat4823.
Yan, Hao, Hohman, J. Nathan, Li, Fei Hua, Jia, Chunjing, Solis-Ibarra, Diego, Wu, Bin, Dahl, Jeremy E. P., Carlson, Robert M. K., Tkachenko, Boryslav A., Fokin, Andrey A., Schreiner, Peter R., Vailionis, Arturas, Kim, Taeho Roy, Devereaux, Thomas P., Shen, Zhi -Xun, and Melosh, Nicholas A. Mon . "Hybrid metal–organic chalcogenide nanowires with electrically conductive inorganic core through diamondoid-directed assembly". United States. doi:10.1038/nmat4823. https://www.osti.gov/servlets/purl/1331967.
@article{osti_1331967,
title = {Hybrid metal–organic chalcogenide nanowires with electrically conductive inorganic core through diamondoid-directed assembly},
author = {Yan, Hao and Hohman, J. Nathan and Li, Fei Hua and Jia, Chunjing and Solis-Ibarra, Diego and Wu, Bin and Dahl, Jeremy E. P. and Carlson, Robert M. K. and Tkachenko, Boryslav A. and Fokin, Andrey A. and Schreiner, Peter R. and Vailionis, Arturas and Kim, Taeho Roy and Devereaux, Thomas P. and Shen, Zhi -Xun and Melosh, Nicholas A.},
abstractNote = {Controlling inorganic structure and dimensionality through structure-directing agents is a versatile approach for new materials synthesis that has been used extensively for metal–organic frameworks and coordination polymers. However, the lack of ‘solid’ inorganic cores requires charge transport through single-atom chains and/or organic groups, limiting their electronic properties. Here, we report that strongly interacting diamondoid structure-directing agents guide the growth of hybrid metal–organic chalcogenide nanowires with solid inorganic cores having three-atom cross-sections, representing the smallest possible nanowires. The strong van der Waals attraction between diamondoids overcomes steric repulsion leading to a cis configuration at the active growth front, enabling face-on addition of precursors for nanowire elongation. These nanowires have band-like electronic properties, low effective carrier masses and three orders-of-magnitude conductivity modulation by hole doping. Furthermore, this discovery highlights a previously unexplored regime of structure-directing agents compared with traditional surfactant, block copolymer or metal–organic framework linkers.},
doi = {10.1038/nmat4823},
journal = {Nature Materials},
number = 3,
volume = 16,
place = {United States},
year = {2016},
month = {12}
}

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Cited by: 16 works
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Figures / Tables:

Figure 1 Figure 1: Schematic of synthesis and structure of MOC crystals. a, Schematic of the twophase synthetic strategy for MOC crystals. R = adamantane or diamantane, M = Cu. EG = ethylene glycol. b, Representative scanning electron microscopy (SEM) micrograph of 1ADCu crystals. Inset: Atomic force microscopy (AFM) of the 1ADCumore » crystals. Scale bars: 10 µm (SEM), 1 µm (AFM). c, Refined single crystal XRD structure (SC-XRD) of 1ADCu viewed along the chain elongation direction. Cu, S and C are represented by brown, yellow and black colors, respectively. The blue spheres denote the vdW radii of the adamantane side group. d, Side-view of individual 1ADCu NW structure solved by SC-XRD. The atoms are represented by their 50%-probability ellipsoids. Only the $\alpha$-carbons in the adamantyl sidegroups are shown for clarity. The yellow and red triangles represent the three-atom S and Cu rings respectively. e, Unit cell of the 1ADCu crystal solved by SC-XRD. Cu and S atoms are represented by red and yellow spheres, and the adamantyl groups are represented by the grey capped stick model. Hydrogen atoms are omitted for clarity. The blue dots denote the centroid of the adamantyl groups.« less

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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.