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Title: Controlled Sculpture of Black Phosphorus Nanoribbons

Black phosphorus (BP) is a highly anisotropic allotrope of phosphorus with high promise for fast functional electronics and optoelectronics. We demonstrate that high-resolution and controlled structural modification of few-layer BP along arbitrary crystal direction can be achieved with nanometer-scale precision on a few-minute timescales leading to the formation of sub-nm wide armchair and zigzag BP nanoribbons. The nanoribbons are assembled, along with nanopores and nanogaps, using a combination of mechanical-liquid exfoliation and in situ transmission electron microscope (TEM) and scanning TEM nanosculpting. Here we report time-dependent structural properties of the one-dimensional systems under electron irradiation and probe their oxidation properties with electron energy-loss spectroscopy (EELS). Finally, we demonstrate the use of STEM to controllably narrow and thin the nanoribbons until they break into nanogaps. The observations are rationalized using density functional theory for transition state calculations and electronic band-structure evolution for the various stages of the narrowing procedure. In particular, we predict that the sub- and few-nm wide BP nanoribbons realized experimentally possess clear one-dimensional quantum confinement, even when the systems are made up of a few layers. We find the demonstration of this procedure is key for the development of BP-based electronic, optoelectronic, thermoelectric, and other applications in reducedmore » dimensions.« less
Authors:
 [1] ;  [2] ;  [3] ;  [1] ;  [4] ;  [3] ;  [5] ;  [5] ;  [5] ;  [3] ;  [1]
  1. Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Physics and Astronomy
  2. Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Physics and Astronomy; Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of of Electrical and Systems Engineering
  3. Rensselaer Polytechnic Inst., Troy, NY (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  5. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Publication Date:
OSTI Identifier:
1260088
Grant/Contract Number:
AC05-00OR22725; SC0001299; R21HG007856; FRI-1542707
Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 10; Journal Issue: 6; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org:
ORNL LDRD Director's R&D; USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY armchair; few-layer black phosphorus; nanopore; nanoribbon; phosphorene; zigzag