Second-order nonlinear processes like Sum-Frequency Generation (SFG) are essentially defined in the electric dipolar approximation. However, when dealing with the SFG responses of bulk, big nanoparticles, highly symmetric objects, or chiral species, magnetic and quadrupolar contributions play a significant role in the process too. We extend the diagrammatic theory for linear and nonlinear optics to include these terms for single objects as well as for multipartite systems in interaction. Magnetic and quadrupolar quantities are introduced in the formalism as incoming fields, interaction intermediates, and sources of optical nonlinearity. New response functions and complex nonlinear processes are defined, and their symmetry properties are analyzed. This leads to a focus on several kinds of applications involving nanoscale coupled objects, symmetric molecular systems, and chiral materials, both in line with the existing literature and opening new possibilities for original complex systems.
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14 January 2024
Research Article|
January 09 2024
Diagrammatic theory of magnetic and quadrupolar contributions to sum-frequency generation in composite systems
Special Collection:
Recent Developments in Nonlinear Optics at Interfaces
Thomas Noblet
;
Thomas Noblet
a)
(Conceptualization, Investigation, Methodology, Writing – original draft, Writing – review & editing)
1
GRASP-Biophotonics, CESAM, University of Liege, Institute of Physics
, Allée du 6 août 17, 4000 Liège, Belgium
a)Author to whom correspondence should be addressed: [email protected]
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Bertrand Busson
Bertrand Busson
(Conceptualization, Investigation, Methodology, Writing – original draft, Writing – review & editing)
2
Université Paris-Saclay, CNRS, Institut de Chimie Physique, UMR 8000
, 91405 Orsay, France
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a)Author to whom correspondence should be addressed: [email protected]
J. Chem. Phys. 160, 024704 (2024)
Article history
Received:
November 14 2023
Accepted:
December 15 2023
Citation
Thomas Noblet, Bertrand Busson; Diagrammatic theory of magnetic and quadrupolar contributions to sum-frequency generation in composite systems. J. Chem. Phys. 14 January 2024; 160 (2): 024704. https://doi.org/10.1063/5.0187520
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