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Ab Initio Cluster Approach for High Harmonic Generation in Liquids

[Image: see text] High harmonic generation (HHG) takes place in all phases of matter. In gaseous atomic and molecular media, it has been extensively studied and is very well understood. In solids, research is ongoing, but a consensus is forming for the dominant microscopic HHG mechanisms. In liquids...

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Autores principales: Neufeld, Ofer, Nourbakhsh, Zahra, Tancogne-Dejean, Nicolas, Rubio, Angel
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9281394/
https://www.ncbi.nlm.nih.gov/pubmed/35699241
http://dx.doi.org/10.1021/acs.jctc.2c00235
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author Neufeld, Ofer
Nourbakhsh, Zahra
Tancogne-Dejean, Nicolas
Rubio, Angel
author_facet Neufeld, Ofer
Nourbakhsh, Zahra
Tancogne-Dejean, Nicolas
Rubio, Angel
author_sort Neufeld, Ofer
collection PubMed
description [Image: see text] High harmonic generation (HHG) takes place in all phases of matter. In gaseous atomic and molecular media, it has been extensively studied and is very well understood. In solids, research is ongoing, but a consensus is forming for the dominant microscopic HHG mechanisms. In liquids, on the other hand, no established theory yet exists, and approaches developed for gases and solids are generally inapplicable, hindering our current understanding. We develop here a powerful and reliable ab initio cluster-based approach for describing the nonlinear interactions between isotropic bulk liquids and intense laser pulses. The scheme is based on time-dependent density functional theory and utilizes several approximations that make it feasible yet accurate in realistic systems. We demonstrate our approach with HHG calculations in water, ammonia, and methane liquids and compare the characteristic response of polar and nonpolar liquids. We identify unique features in the HHG spectra of liquid methane that could be utilized for ultrafast spectroscopy of its chemical and physical properties, including a structural minimum at 15–17 eV that is associated solely with the liquid phase. Our results pave the way to accessible calculations of HHG in liquids and illustrate the unique nonlinear nature of liquid systems.
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spelling pubmed-92813942022-07-15 Ab Initio Cluster Approach for High Harmonic Generation in Liquids Neufeld, Ofer Nourbakhsh, Zahra Tancogne-Dejean, Nicolas Rubio, Angel J Chem Theory Comput [Image: see text] High harmonic generation (HHG) takes place in all phases of matter. In gaseous atomic and molecular media, it has been extensively studied and is very well understood. In solids, research is ongoing, but a consensus is forming for the dominant microscopic HHG mechanisms. In liquids, on the other hand, no established theory yet exists, and approaches developed for gases and solids are generally inapplicable, hindering our current understanding. We develop here a powerful and reliable ab initio cluster-based approach for describing the nonlinear interactions between isotropic bulk liquids and intense laser pulses. The scheme is based on time-dependent density functional theory and utilizes several approximations that make it feasible yet accurate in realistic systems. We demonstrate our approach with HHG calculations in water, ammonia, and methane liquids and compare the characteristic response of polar and nonpolar liquids. We identify unique features in the HHG spectra of liquid methane that could be utilized for ultrafast spectroscopy of its chemical and physical properties, including a structural minimum at 15–17 eV that is associated solely with the liquid phase. Our results pave the way to accessible calculations of HHG in liquids and illustrate the unique nonlinear nature of liquid systems. American Chemical Society 2022-06-14 2022-07-12 /pmc/articles/PMC9281394/ /pubmed/35699241 http://dx.doi.org/10.1021/acs.jctc.2c00235 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Neufeld, Ofer
Nourbakhsh, Zahra
Tancogne-Dejean, Nicolas
Rubio, Angel
Ab Initio Cluster Approach for High Harmonic Generation in Liquids
title Ab Initio Cluster Approach for High Harmonic Generation in Liquids
title_full Ab Initio Cluster Approach for High Harmonic Generation in Liquids
title_fullStr Ab Initio Cluster Approach for High Harmonic Generation in Liquids
title_full_unstemmed Ab Initio Cluster Approach for High Harmonic Generation in Liquids
title_short Ab Initio Cluster Approach for High Harmonic Generation in Liquids
title_sort ab initio cluster approach for high harmonic generation in liquids
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9281394/
https://www.ncbi.nlm.nih.gov/pubmed/35699241
http://dx.doi.org/10.1021/acs.jctc.2c00235
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