Engineering single-atom dynamics with electron irradiation

A vector-space formalism is developed for optimizing single-atom manipulation outcomes under focused electron irradiation. Atomic engineering is envisioned to involve selectively inducing the desired dynamics of single atoms and combining these steps for larger-scale assemblies. Here, we focus on the first part by surveying the single-step dynamics of graphene dopants, primarily phosphorus, caused by electron irradiation both in experiment and simulation, and develop a theory for describing the probabilities of competing configurational outcomes depending on the postcollision momentum vector of the primary knock-on atom. The predicted branching ratio of configurational transformations agrees well with our atomically resolved experiments. This suggests a way for biasing the dynamics toward desired outcomes, paving the road for designing and further upscaling atomic engineering using electron irradiation.

[1]  David B. Williams,et al.  The Transmission Electron Microscope , 2009 .

[2]  Subra Suresh,et al.  Deep elastic strain engineering of bandgap through machine learning , 2019, Proceedings of the National Academy of Sciences.

[3]  J. Kotakoski,et al.  Influence of temperature on the displacement threshold energy in graphene , 2018, Scientific Reports.

[4]  Travis S Humble,et al.  Directed Atom-by-Atom Assembly of Dopants in Silicon. , 2018, ACS nano.

[5]  Andreas Mittelberger,et al.  Electron-Beam Manipulation of Silicon Dopants in Graphene , 2017, Nano letters.

[6]  Ondrej Dyck,et al.  Placing single atoms in graphene with a scanning transmission electron microscope , 2017 .

[7]  Jannik C. Meyer,et al.  Towards atomically precise manipulation of 2D nanostructures in the electron microscope , 2017, 1708.08780.

[8]  Sergei V. Kalinin,et al.  Single atom manipulation and control in a scanning transmission electron microscope , 2017, 1708.01523.

[9]  J. Kong,et al.  Revealing the Bonding of Nitrogen Impurities in Monolayer Graphene , 2017, Microscopy and Microanalysis.

[10]  Jannik C Meyer,et al.  Manipulating low-dimensional materials down to the level of single atoms with electron irradiation. , 2017, Ultramicroscopy.

[11]  Jannik C. Meyer,et al.  Single-atom spectroscopy of phosphorus dopants implanted into graphene , 2016, 1610.03419.

[12]  Jannik C. Meyer,et al.  Isotope analysis in the transmission electron microscope , 2016, Nature Communications.

[13]  F E Kalff,et al.  A kilobyte rewritable atomic memory. , 2016, Nature nanotechnology.

[14]  Q. Ramasse,et al.  Electronic Structure Modification of Ion Implanted Graphene: The Spectroscopic Signatures of p- and n-Type Doping. , 2015, ACS Nano.

[15]  Takashi Taniguchi,et al.  Direct observation of dopant atom diffusion in a bulk semiconductor crystal enhanced by a large size mismatch. , 2014, Physical review letters.

[16]  Clemens Mangler,et al.  Silicon-carbon bond inversions driven by 60-keV electrons in graphene. , 2014, Physical review letters.

[17]  Paola Cappellaro,et al.  Atomic-Scale Nuclear Spin Imaging Using Quantum-Assisted Sensors in Diamond , 2014, 1407.3134.

[18]  Clemens Mangler,et al.  Imaging atomic-level random walk of a point defect in graphene , 2014, Nature Communications.

[19]  Q. Ramasse,et al.  Ion implantation of graphene-toward IC compatible technologies. , 2013, Nano letters.

[20]  P. Nellist,et al.  Probing the bonding in nitrogen-doped graphene using electron energy loss spectroscopy. , 2013, ACS nano.

[21]  S. Pennycook,et al.  Direct visualization of reversible dynamics in a Si6 cluster embedded in a graphene pore , 2013, Nature Communications.

[22]  R. Egerton.  Beam-Induced Motion of Adatoms in the Transmission Electron Microscope , 2013, Microscopy and Microanalysis.

[23]  Ursel Bangert,et al.  Probing the bonding and electronic structure of single atom dopants in graphene with electron energy loss spectroscopy. , 2013, Nano letters.

[24]  Ji Feng,et al.  Two-dimensional carbon allotrope with strong electronic anisotropy , 2012, 1211.4680.

[25]  S. Pennycook,et al.  Direct determination of the chemical bonding of individual impurities in graphene. , 2012, Physical review letters.

[26]  Jannik C. Meyer,et al.  Atomistic description of electron beam damage in nitrogen-doped graphene and single-walled carbon nanotubes. , 2012, ACS nano.

[27]  K. Novoselov,et al.  Graphene reknits its holes. , 2012, Nano letters.

[28]  Jannik C. Meyer,et al.  Accurate measurement of electron beam induced displacement cross sections for single-layer graphene. , 2012, Physical review letters.

[29]  A. Krasheninnikov,et al.  Stone-Wales-type transformations in carbon nanostructures driven by electron irradiation , 2011, 1105.1617.

[30]  K. Suenaga,et al.  Atom-by-atom spectroscopy at graphene edge , 2010, Nature.

[31]  R. Egerton.  Physical Principles of Electron Microscopy: An Introduction to TEM, SEM, and AEM , 2010 .

[32]  A. Krasheninnikov,et al.  Electron knock-on damage in hexagonal boron nitride monolayers , 2010 .

[33]  J. Shan,et al.  Ultrafast photoluminescence from graphene. , 2010, Physical review letters.

[34]  Pablo A. Denis,et al.  Band gap opening of monolayer and bilayer graphene doped with aluminium, silicon, phosphorus, and sulfur , 2010 .

[35]  S. Pennycook,et al.  Atom-by-atom structural and chemical analysis by annular dark-field electron microscopy , 2010, Nature.

[36]  Enge Wang,et al.  Stone-Wales defects in graphene and other planar sp(2)-bonded materials , 2009 .

[37]  P. Batson.  Local crystal anisotropy obtained in the small probe geometry. , 2008, Micron.

[38]  Gary S. Was,et al.  Fundamentals of Radiation Materials Science: Metals and Alloys , 2007 .

[39]  G. Seifert,et al.  Electron knock-on cross section of carbon and boron nitride nanotubes , 2007 .

[40]  M. Grüning,et al.  Exchange-correlation energy and potential as approximate functionals of occupied and virtual Kohn-Sham orbitals: Application to dissociating H-2 , 2003 .

[41]  Burke,et al.  Generalized Gradient Approximation Made Simple. , 1996, Physical review letters.

[42]  Kresse,et al.  Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. , 1996, Physical review. B, Condensed matter.

[43]  D. Eigler,et al.  Positioning single atoms with a scanning tunnelling microscope , 1990, Nature.

[44]  Herman Feshbach,et al.  The Coulomb Scattering of Relativistic Electrons by Nuclei , 1948 .