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Controlling the non-linear optical properties of MgO by tailoring the electronic structure

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Abstract

The study of the non-linear response of matter to high electric fields has recently encompassed harmonic generation in solids at near-infrared (NIR) driving wavelengths. Interest has been driven by the prospect of ultrafast signal processing and all-optical mapping of electron wave-functions in solids. Engineering solid-state band structures to control the non-linear process has already been highlighted theoretically. Here, we show experimentally for the first time that second harmonic generation (SHG) can be enhanced by doping crystals of magnesium oxide (MgO) with chromium (Cr) atoms. We show that the degree of enhancement depends non-linearly on dopant concentration. The SHG efficiency is shown to increase when Cr dopants are introduced into pure MgO. A physical picture of the effect of Cr dopants is aided by density functional theory (DFT) calculations of the electronic structure for pure and doped samples. This work shows an unambiguous enhancement of the SHG efficiency by modifying the electronic structure. The observed effects are consistent with an electronic structure that facilitates surface induced SHG and demonstrates a minimal angular dependence. This work highlights the potential of manipulating the electronic structure of solids to control, or test theories of, their non-linear optical response.

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Acknowledgments

This work was partially supported by the Fundação para a Ciência e Tecnologia (FCT) under the Grant Number PD/BD/135224/2017 in the framework of the Advanced Program in Plasma Science and Engineering (APPLAuSE), and the PETACom FET Open H2020, support from the French ministry of research through the ANR Grants 2016 “HELLIX”, 2017 “PACHA”, the DGA RAPID grant “SWIM” and the LABEX “PALM” (ANR-10-LABX-0039-PALM) through the Grants “Plasmon-X”, “STAMPS” and “HILAC”. We acknowledge the financial support from the French ASTRE program through the “NanoLight” grant. We are thankful to Dr. Viktoria Nefedova and Dr. David Gauthier for fruitful discussion.

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Authors and Affiliations

  1. GoLP/Instituto de Plasmas e Fusão Nuclear-Laboratório Associado, Instituto Superior Técnico, Universidade de Lisboa, 1049-001, Lisbon, Portugal

    Mukhtar Hussain, Hugo Pires, Marta Fajardo & Gareth O. Williams

  2. LIDYL, CEA, CNRS, Université Paris-Saclay, CEA Saclay, 91191, Gif-sur-Yvette, France

    Mukhtar Hussain, Willem Boutu, Dominik Franz, Rana Nicolas & Hamed Merdji

  3. Natural Sciences Department, Lebanese American University, Beirut, Lebanon

    Rana Nicolas

  4. Group of Laser Development (GoLD)/Department of Physics, COMSATS University Islamabad, Park Road, Islamabad, 44000, Pakistan

    Tayyab Imran

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  1. Mukhtar Hussain
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Hussain, M., Pires, H., Boutu, W. et al. Controlling the non-linear optical properties of MgO by tailoring the electronic structure. Appl. Phys. B 126, 46 (2020). https://doi.org/10.1007/s00340-020-7393-7

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