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Diverse Phases of Carbonaceous Materials from Stochastic Simulations

Monti, Susanna and Barcaro, Giovanni and Goddard, William A., III and Fortunelli, Alessandro (2021) Diverse Phases of Carbonaceous Materials from Stochastic Simulations. ACS Nano, 15 (4). pp. 6369-6385. ISSN 1936-0851. doi:10.1021/acsnano.0c08029.

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Amorphous carbon systems are emerging to have unparalleled properties at multiple length scales, making them the preferred choice for creating advanced materials in many sectors, but the lack of long-range order makes it difficult to establish structure/property relationships. We propose an original computational approach to predict the morphology of carbonaceous materials for arbitrary densities that we apply here to graphitic phases at low densities from 1.15 to 0.16 g/cm³, including glassy carbon. This approach, dynamic reactive massaging of the potential energy surface (DynReaxMas), uses the ReaxFF reactive force field in a simulation protocol that combines potential energy surface (PES) transformations with global optimization within a multidescriptor representation. DynReaxMas enables the simulation of materials synthesis at temperatures close to experiment to correctly capture the interplay of activated vs entropic processes and the resulting phase morphology. We then show that DynReaxMas efficiently and semiautomatically produces atomistic configurations that span wide relevant regions of the PES at modest computational costs. Indeed, we find a variety of distinct phases at the same density, and we illustrate the evolution of competing phases as a function of density ranging from uniform vs bimodal distributions of pore sizes at higher and intermediate density (1.15 g/cm³ and 0.50 g/cm³) to agglomerated vs sparse morphologies, further partitioned into boxed vs hollow fibrillar morphologies, at lower density (0.16 g/cm³). Our observations of diverse phases at the same density agree with experiment. Some of our identified phases provide descriptors consistent with available experimental data on local density, pore sizes, and HRTEM images, showing that DynReaxMas provides a systematic classification of the complex field of amorphous carbonaceous materials that can provide 3D structures to interpret experimental observations.

Item Type:Article
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URLURL TypeDescription
Monti, Susanna0000-0002-3419-7118
Barcaro, Giovanni0000-0002-5520-5914
Goddard, William A., III0000-0003-0097-5716
Fortunelli, Alessandro0000-0001-5337-4450
Additional Information:© 2021 American Chemical Society. Received: September 23, 2020; Accepted: March 11, 2021; Published: March 15, 2021. A.F. and W.A.G. acknowledge support from NSF (Grant CBET 1805022). Computational support from CINECA Supercomputing Centre within the ISCRA programme is gratefully acknowledged. Author Contributions: SM. and G.B. contributed equally to this work. The authors declare no competing financial interest.
Funding AgencyGrant Number
Subject Keywords:PES transformations, global optimization, graphitic phases, pore-size distribution, amorphous carbon, glassy carbon, carbon nanotubes
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Issue or Number:4
Record Number:CaltechAUTHORS:20210316-071031936
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Official Citation:Diverse Phases of Carbonaceous Materials from Stochastic Simulations. Susanna Monti, Giovanni Barcaro, William A. Goddard, and Alessandro Fortunelli. ACS Nano 2021 15 (4), 6369-6385; DOI: 10.1021/acsnano.0c08029
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:108444
Deposited By: Tony Diaz
Deposited On:19 Mar 2021 02:22
Last Modified:06 Jun 2021 01:36

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