Photon–photon chemical thermodynamics of frequency conversion processes in highly multimode systems

Huizhong Ren; Georgios G. Pyrialakos; Qi Zhong; Fan O. Wu; Mercedeh Khajavikhan; Demetrios N. Christodoulides

doi:10.1038/s41377-025-01856-4

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Photon–photon chemical thermodynamics of frequency conversion processes in highly multimode systems

Original Articles

- Photon–photon chemical thermodynamics of frequency conversion processes in highly multimode systems
- Light: Science & Applications Vol. 14, Issue 7, Pages: 1954-1964(2025)
- Affiliations：
  
  1.Ming Hsieh Department of Electrical and Computer Engineering, University of Southern California, Los Angeles, CA 90089, USA
  2.CREOL, College of Optics and Photonics, University of Central Florida, Orlando, FL 32816, USA
  3.Department of Physics and Astronomy, University of Southern California, Los Angeles, CA 90089, USA
  4.Present address: School of Applied and Engineering Physics, Cornell University, Ithaca, NY 14853, USA
- Author bio：
  
  Mercedeh Khajavikhan (khajavik@usc.edu)
  Demetrios N. Christodoulides (demetri@usc.edu)
- Funds：
- DOI：10.1038/s41377-025-01856-4
  CLC：
- Received：08 November 2024，
  
  Revised：27 March 2025，
  
  Accepted：31 March 2025，
  
  Published Online：12 May 2025，
  
  Published：31 July 2025
- Accepted：
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Ren, H. Z. et al. Photon–photon chemical thermodynamics of frequency conversion processes in highly multimode systems. Light: Science & Applications, 14, 1954-1964 (2025).
DOI：

Ren, H. Z. et al. Photon–photon chemical thermodynamics of frequency conversion processes in highly multimode systems. Light: Science & Applications, 14, 1954-1964 (2025). DOI： 10.1038/s41377-025-01856-4.

摘要

Abstract

Frequency generation in highly multimode nonlinear optical systems is inherently a complex process

giving rise to an exceedingly convoluted landscape of evolution dynamics. While predicting and controlling the global conversion efficiencies in such nonlinear environments has long been considered impossible

here

we formally address this challenge even in scenarios involving a very large number of spatial modes. By utilizing fundamental notions from optical statistical mechanics

we develop a universal theoretical framework that effectively treats all frequency components as chemical reactants/products

capable of undergoing optical thermodynamic reactions facilitated by a variety of multi-wave mixing effects. These photon–photon reactions are governed by conservation laws that directly determine the optical temperatures and chemical potentials of the ensued chemical equilibria for each frequency species. In this context

we develop a comprehensive stoichiometric model and formally derive an expression that relates the chemical potentials to the optical stoichiometric coefficients

in a manner akin to atomic/molecular chemical reactions. This advancement unlocks new predictive capabilities that can facilitate the optimization of frequency generation in highly multimode photonic arrangements

surpassing the limitations of conventional schemes that rely exclusively on nonlinear optical dynamics. Notably

we identify a universal regime of Rayleigh–Jeans thermalization where an optical reaction at near-zero optical temperatures can promote the complete and entropically irreversible conversion of light to the fundamental mode at a target frequency. Our theoretical results are corroborated by numerical simulations in settings where second-harmonic generation

sum-frequency generation and four-wave mixing processes can manifest.

关键词

Keywords

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