High-Order Nonlinear Dipole Response Characterized by Extreme-Ultraviolet Ellipsometry

Posted on 05.04.2021 - 20:07
Polarization engineering and characterization over a wide spectral range are essential to investigate the symmetry properties in matter and to control light-matter interactions. This work for the first time demonstrates that high-harmonic ellipsometry, using the polarization degree of freedom, is able to unveil the quantum nature of the high-order nonlinear dipole response. An advanced high-harmonic ellipsometry technique is driven by two non-collinear ellipticity-controlled laser fields, and makes use of a new energy-resolved extreme-ultraviolet polarimeter that allows us to fully characterize the polarization for every high-harmonic order. High harmonic ellipsometry reveals that both amplitude and phase of high-harmonic dipole scale more rapidly with the driving field in higher-order harmonics, and especially in low-ionization-potential gases. This study also clearly points out that the variation of non-perturbative dipole phase induced by the inhomogeneity of fundamentals limits power scaling of high order harmonic generation. Our theoretical simulations allow us to corroborate the retrieved experimental results. This novel high-harmonic ellipsometry with attosecond accuracy opens up new prospects to precisely quantify strong field dynamics of fundamental processes associated with energy and angular momentum transfer between electron/spin systems, and symmetry-dependent properties of molecules and solid-state materials.


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Chang, Kuang-Yu; Huang, Long-Cheng; Asaga, Koji; Tsai, Ming-Shian; Cabezas, Laura Rego; Huang, Pei-Chi; et al. (2021): High-Order Nonlinear Dipole Response Characterized by Extreme-Ultraviolet Ellipsometry. The Optical Society. Collection. https://doi.org/10.6084/m9.figshare.c.5251200.v2




Kuang-Yu Chang
Long-Cheng Huang
Koji Asaga
Ming-Shian Tsai
Laura Rego Cabezas
Pei-Chi Huang
Hiroki Mashiko
Katsuya Oguri
Carlos Hernandez-Garcia
Ming-Chang Chen


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