Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Hard, transparent, sp3-containing 2D phase formed from few-layer graphene under compression

Journal Article · · Carbon
 [1];  [2];  [3];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [2];  [4];  [4];  [4];  [1];  [2];  [4];  [1];  [1];  [2]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  2. Univ. Federal de Minas Gerais, Belo Horizonte (Brazil)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Univ. Federal de Ouro Preto (Brazil)

Despite several theoretically proposed two-dimensional (2D) diamond structures, experimental efforts to obtain such structures are in initial stage. Recent high-pressure experiments provided significant advancements in the field, however, expected properties of a 2D-like diamond such as sp3 content, transparency and hardness, have not been observed together in a compressed graphene system. Here, we compress few-layer graphene samples on SiO2/Si substrate in water and provide experimental evidence for the formation of a quenchable hard, transparent, sp3-containing 2D phase. Our Raman spectroscopy data indicates phase transition and a surprisingly similar critical pressure for two-, five-layer graphene and graphite in the 4e6 GPa range, as evidenced by changes in several Raman features, combined with a lack of evidence of significant pressure gradients or local non-hydrostatic stress components of the pressure medium up to ≈ 8 GPa. The new phase is transparent and hard, as evidenced from indentation marks on the SiO2 substrate, a material considerably harder than graphene systems. Furthermore, we report the lowest critical pressure (≈ 4 GPa) in graphite, which we attribute to the role of water in facilitating the phase transition. Overall, theoretical calculations and experimental data indicate a novel, surface to- bulk phase transition mechanism that gives hint of diamondene formation.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
National Science Foundation (NSF); Air Force Office of Scientific Research (AFOSR); Conselho Nacional de Desenvolvimento Cientifico e Tecnologico (CNPq); Alfred P. Sloan Foundation; USDOE National Nuclear Security Administration (NNSA), Office of Experimental Sciences; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1765362
Journal Information:
Carbon, Journal Name: Carbon Vol. 173; ISSN 0008-6223
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (59)

Room-Temperature Compression-Induced Diamondization of Few-Layer Graphene journal May 2011
Raman scattering studies of graphene under high pressure: Raman scattering studies of graphene under high pressure journal November 2017
Fast Parallel Algorithms for Short-Range Molecular Dynamics journal March 1995
The rôle of particle properties in the erosion of brittle materials journal April 1996
Computer graphics and graphical user interfaces as tools in simulations of matter at the atomic scale journal October 2003
Low temperature, pressureless sp2 to sp3 transformation of ultrathin, crystalline carbon films journal April 2019
Towards a better understanding of the structure of diamanoïds and diamanoïd/graphene hybrids journal January 2020
Raman spectroscopy analysis of number of layers in mass-produced graphene flakes journal May 2020
Modeling hardness of polycrystalline materials and bulk metallic glasses journal September 2011
Raman spectroscopy of graphene and graphite: Disorder, electron–phonon coupling, doping and nonadiabatic effects journal July 2007
Mechanochemistry of Stable Diamane and Atomically Thin Diamond Films Synthesis from Bi- and Multilayer Graphene: A Computational Study journal May 2019
Synthesis of Atomically Thin Hexagonal Diamond with Compression journal June 2020
Compression-Induced Modification of Boron Nitride Layers: A Conductive Two-Dimensional BN Compound journal May 2018
Quenchable Transparent Phase of Carbon journal January 1997
Graphite to Diamond: Origin for Kinetics Selectivity journal February 2017
Influence of Size Effect on the Electronic and Elastic Properties of Diamond Films with Nanometer Thickness journal December 2010
Converting Chemically Functionalized Few-Layer Graphene to Diamond Films: A Computational Study journal February 2015
Electronic Transport of Encapsulated Graphene and WSe 2 Devices Fabricated by Pick-up of Prepatterned hBN journal February 2015
Calibration of the ruby pressure gauge to 800 kbar under quasi-hydrostatic conditions journal January 1986
Precise determination of graphene functionalization by in situ Raman spectroscopy journal May 2017
Thermal properties of graphene and nanostructured carbon materials journal August 2011
Raman evidence for pressure-induced formation of diamondene journal July 2017
Ultrahard carbon film from epitaxial two-layer graphene journal December 2017
Chemically induced transformation of chemical vapour deposition grown bilayer graphene into fluorinated single-layer diamond journal December 2019
Crystal structure of graphite under room-temperature compression and decompression journal July 2012
The correlation between electrical conductivity and second-order Raman modes of laser-reduced graphene oxide journal January 2019
Hydrostatic limits in liquids and solids to 100 kbar journal December 1973
Compression and bonding of ice VII and an empirical linear expression for the isothermal compression of solids journal January 1975
A unified formulation of the constant temperature molecular dynamics methods journal July 1984
A reactive potential for hydrocarbons with intermolecular interactions journal April 2000
Phonon softening and crystallographic orientation of strained graphene studied by Raman spectroscopy journal April 2009
Large bandgap of pressurized trilayer graphene journal April 2019
The SIESTA method for ab initio order- N materials simulation journal March 2002
Layer dependence of graphene-diamene phase transition in epitaxial and exfoliated few-layer graphene using machine learning journal June 2019
A semi-automated general statistical treatment of graphene systems journal March 2020
Inhomogeneous Electron Gas journal November 1964
Self-Consistent Equations Including Exchange and Correlation Effects journal November 1965
Finite Elastic Strain of Cubic Crystals journal June 1947
Graphite under pressure: Equation of state and first-order Raman modes journal June 1989
Optical reflectivity of graphite under pressure journal July 1989
Efficient pseudopotentials for plane-wave calculations journal January 1991
High-pressure in situ x-ray-diffraction study of the phase transformation from graphite to hexagonal diamond at room temperature journal September 1992
Equation of state of ice VII up to 106 GPa journal September 1997
Resonant Raman spectroscopy of disordered, amorphous, and diamondlike carbon journal July 2001
Collective stabilization of hydrogen chemisorption on graphenic surfaces journal November 2003
Structural and electronic properties of carbon in hybrid diamond-graphite structures journal December 2005
High-pressure Raman spectroscopy of graphene journal August 2009
Raman spectroscopy of graphene at high pressure: Effects of the substrate and the pressure transmitting media journal July 2013
Superhard Monoclinic Polymorph of Carbon journal April 2009
Body-Centered Tetragonal C 4 : A Viable s p 3 Carbon Allotrope journal March 2010
Low-Temperature Phase Transformation from Graphite to s p 3 Orthorhombic Carbon journal February 2011
Crystal Structure of Cold Compressed Graphite journal February 2012
Efficacious Form for Model Pseudopotentials journal May 1982
Generalized Gradient Approximation Made Simple journal October 1996
Bonding Changes in Compressed Superhard Graphite journal October 2003
Control of Graphene's Properties by Reversible Hydrogenation: Evidence for Graphane journal January 2009
Carbon: A New Crystalline Phase journal May 1963
Light-Transparent Phase Formed by Room-Temperature Compression of Graphite journal June 1991
Recent Advances in Superhard Materials journal July 2016

Similar Records

High-pressure phase of cold-compressed bulk graphite and graphene nanoplatelets
Journal Article · Thu May 04 00:00:00 EDT 2023 · Physical Review. B · OSTI ID:2377452