Ab Initio Periodic Simulation of the Spectroscopic and Optical Properties of Novel Porous Graphene Phases

We present a detailed periodic ab initio quantum-mechanical simulation of two recently proposed systems, namely hydrogenated porous graphene (HPG) and biphenyl carbon (BPC), using hybrid HF-DFT functionals and all-electron Gaussian-type basis sets. The equilibrium geometry, the vibrational spectrum...

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Main Authors: De La Pierre, Marco, Karamanis, P., Baima, J., Orlando, R., Pouchan, C., Dovesi, R.
Format: Journal Article
Published: American Chemical Society 2013
Online Access:http://hdl.handle.net/20.500.11937/28558
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author De La Pierre, Marco
Karamanis, P.
Baima, J.
Orlando, R.
Pouchan, C.
Dovesi, R.
author_facet De La Pierre, Marco
Karamanis, P.
Baima, J.
Orlando, R.
Pouchan, C.
Dovesi, R.
author_sort De La Pierre, Marco
building Curtin Institutional Repository
collection Online Access
description We present a detailed periodic ab initio quantum-mechanical simulation of two recently proposed systems, namely hydrogenated porous graphene (HPG) and biphenyl carbon (BPC), using hybrid HF-DFT functionals and all-electron Gaussian-type basis sets. The equilibrium geometry, the vibrational spectrum (including IR intensities), the full set of components of the polarizability and hyperpolarizability tensors are provided, the latter evaluated through a coupled-perturbed KS/HF scheme. IR and Raman spectra for the two systems are quite different, and differ also from graphene, thus permitting their experimental identification. It is then shown that small defects inserted into the graphene sheet lead to finite values for the in-plane components of the static (hyper) polarizability tensors, spanning a relatively large range of values. By dehydrogenation of porous graphene into biphenyl carbon, a noteworthy enhancement of the nonlinear optical properties through the static second dipole hyperpolarizability can be achieved. Vibrational contributions to the polarizability are negligible for both systems.
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spelling curtin-20.500.11937-285582017-09-13T15:20:31Z Ab Initio Periodic Simulation of the Spectroscopic and Optical Properties of Novel Porous Graphene Phases De La Pierre, Marco Karamanis, P. Baima, J. Orlando, R. Pouchan, C. Dovesi, R. We present a detailed periodic ab initio quantum-mechanical simulation of two recently proposed systems, namely hydrogenated porous graphene (HPG) and biphenyl carbon (BPC), using hybrid HF-DFT functionals and all-electron Gaussian-type basis sets. The equilibrium geometry, the vibrational spectrum (including IR intensities), the full set of components of the polarizability and hyperpolarizability tensors are provided, the latter evaluated through a coupled-perturbed KS/HF scheme. IR and Raman spectra for the two systems are quite different, and differ also from graphene, thus permitting their experimental identification. It is then shown that small defects inserted into the graphene sheet lead to finite values for the in-plane components of the static (hyper) polarizability tensors, spanning a relatively large range of values. By dehydrogenation of porous graphene into biphenyl carbon, a noteworthy enhancement of the nonlinear optical properties through the static second dipole hyperpolarizability can be achieved. Vibrational contributions to the polarizability are negligible for both systems. 2013 Journal Article http://hdl.handle.net/20.500.11937/28558 10.1021/jp3103436 American Chemical Society restricted
spellingShingle De La Pierre, Marco
Karamanis, P.
Baima, J.
Orlando, R.
Pouchan, C.
Dovesi, R.
Ab Initio Periodic Simulation of the Spectroscopic and Optical Properties of Novel Porous Graphene Phases
title Ab Initio Periodic Simulation of the Spectroscopic and Optical Properties of Novel Porous Graphene Phases
title_full Ab Initio Periodic Simulation of the Spectroscopic and Optical Properties of Novel Porous Graphene Phases
title_fullStr Ab Initio Periodic Simulation of the Spectroscopic and Optical Properties of Novel Porous Graphene Phases
title_full_unstemmed Ab Initio Periodic Simulation of the Spectroscopic and Optical Properties of Novel Porous Graphene Phases
title_short Ab Initio Periodic Simulation of the Spectroscopic and Optical Properties of Novel Porous Graphene Phases
title_sort ab initio periodic simulation of the spectroscopic and optical properties of novel porous graphene phases
url http://hdl.handle.net/20.500.11937/28558