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We present a new first-principle theory for the calculation of the macroscopic second-order susceptibility chi^(2), based on the Time-Dependent Density-Functional Theory approach. Our method allows to include straightforwardly the many-body…

Materials Science · Physics 2010-01-15 Eleonora Luppi , Hannes Hübener , Valérie Véniard

We report on the linear and nonlinear optical response of metamaterials evoked by first and second order multipoles. The analytical ground on which our approach bases permits for new insights into the functionality of metamaterials. For the…

The optical properties of two-dimensional materials are exceptional in several respects. They are highly anisotropic and frequently dominated by excitonic effects. Dipole-allowed second order non-linear optical properties require broken…

Mesoscale and Nanoscale Physics · Physics 2023-07-05 M. F. C. Martins Quintela , T. Garm Pedersen

Excitonic effects in the linear optical response of semiconductors are well-known and the subject of countless experimental and theoretical studies. For the technologically important second order nonlinear response, however, description of…

Strongly Correlated Electrons · Physics 2007-05-23 Thomas G. Pedersen , Horia D. Cornean

Second-order nonlinear spectroscopy has proven to be a powerful tool in elucidating key chemical and structural characteristics at a variety of interfaces. However, the presence of interfacial potentials may lead to complications regarding…

Materials Science · Physics 2017-10-19 Paul E. Ohno , Hong-fei Wang , Franz M. Geiger

We apply scaling and the theory of the fundamental limits of the second-order molecular susceptibility to identify material classes with ultralarge nonlinear-optical response. Size effects are removed by normalizing all nonlinearities to…

Optics · Physics 2016-11-03 Javier Perez-Moreno , Shoresh Shafei , Mark G. Kuzyk

We have performed first principles electron-correlated calculations employing large basis sets to optimize the geometries, and to compute linear optical absorption spectra of various low-lying conformers of silicon hydrides:…

Atomic and Molecular Clusters · Physics 2019-10-16 Pritam Bhattacharyya , Deepak Kumar Rai , Alok Shukla

Understanding the linear response of any system is the first step towards analyzing its linear and nonlinear dynamics, stability properties, as well as its behavior in the presence of noise. In non-Hermitian Hamiltonian systems, calculating…

Linear and nonlinear optical effect has been widely discussed in large quantity of materials using theoretical or experimental methods. Except linear optical conductivity, higher-order nonlinear responses are not studied fully. Starting…

Materials Science · Physics 2025-08-12 Maoyuan Wang , Jianhui Zhou , Yugui Yao

The nonlinear optical response of an excitonic insulator coupled to lattice degrees of freedom is shown to depend in strong and characteristic ways on whether the insulating behavior originates primarily from electron-electron or…

Strongly Correlated Electrons · Physics 2021-01-04 Denis Golez , Zhiyuan Sun , Yuta Murakami , Antoine Georges , Andrew J. Millis

Plasmonic metasurfaces are promising as enablers of nanoscale nonlinear optics and flat nonlinear optical components. Nonlinear optical responses of such metasurfaces are determined by the nonlinear optical properties of individual…

Interpretation of time-resolved spectroscopies such as transient absorption (TA) or two-dimensional (2D) spectroscopy often relies on the perturbative description of light-matter interaction. In many cases the third order of nonlinear…

The non-linear response of infinite periodic solids to homogenous electric fields and collective atomic displacements is discussed in the framework of density functional perturbation theory. The approach is based on the 2n + 1 theorem…

Materials Science · Physics 2007-05-23 M. Veithen , X. Gonze , Ph. Ghosez

The scaling of the fundamental limits of the second hyperpolarizability is used to define the intrinsic second hyperpolarizability, which aids in identifying material classes with ultralarge nonlinear-optical response per unit of molecular…

Optics · Physics 2016-11-03 Javier Perez-Moreno , Shoresh Shafei , Mark G. Kuzyk

Nonlinear optical (NLO) phenomena such as harmonic generation, Kerr, and Pockels effects are of great technological importance for lasers, frequency converters, modulators, switches, etc. Recently, two-dimensional (2D) materials have drawn…

Structuring optical materials on a nanometer scale can lead to artificial effective media, or metamaterials, with strongly altered optical behavior. Metamaterials can provide a wide range of linear optical properties such as negative…

Nonlinear optical responses are becoming increasingly relevant for characterizing the symmetries and quantum geometry of electronic phases in materials. Here, we develop an expanded diagrammatic scheme for calculating spatially dispersive…

Mesoscale and Nanoscale Physics · Physics 2023-08-16 Steven Gassner , Eugene J. Mele

To add the detailed information to the existed knowledge of nonlinear optics field, the nonlinear optical processes of the second and third order have been discussed in their respective susceptibility tensors in the presence of degenerate…

Optics · Physics 2018-01-29 A Srinivasa Rao

The second-order optical susceptibility of semiconductors $\chi_{ijk}^{(2)}(-2\omega;\omega,\omega)$ finds application in metrology, spectroscopy, telecommunications, material characterization, and quantum information. Pioneering…

Materials Science · Physics 2026-02-03 Angiolo Huaman , Luis Enrique Rosas-Hernandez , Salvador Barraza-Lopez

Nonlinear optical responses provide a powerful way to understand the microscopic interactions between laser fields and matter. They are critical for plenty of applications, such as in lasers, integrated photonic circuits, biosensing and…

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