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Light Science & Applications

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

Published May 12, 2025• 4 citations
Publisher

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.

DOI
10.1038/s41377-025-01856-4

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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.
By utilizing notions from statistical mechanics, we develop a general and self-consistent theoretical framework capable of describing any weakly nonlinear optical multimode system involving conserved quantities. We derive the fundamental relations that govern the grand canonical ensemble through maximization of the Gibbs entropy at equilibrium. In this classical picture of statistical photo-mechanics, we obtain analytical expressions for the probability distribution, the grand partition function, and the relevant thermodynamic potentials. Our results universally apply to any other weakly nonlinear multimode bosonic system.
Thermalization of isolated quantum systems is an intriguing phenomenon at the forefront of contemporary physics. In this work, we demonstrate that nonlinear multimode optical platforms can be harnessed to induce effective quantum interactions between photons. Through numerical experiments where quantum beams propagate alongside classical light within multimode nonlinear optical systems, we reveal the thermalization of fundamental quantum light states--specifically single- and two-photon states. This thermalization is clearly manifested by the emergence of Rayleigh-Jeans and Boltzmann statistical distributions. Beyond providing a deeper understanding of how classical nonlinearities can be used to investigate quantum many-body dynamics, our findings will enable the exploration of a broader range of complex quantum phenomena, including aspects of quantum phase transitions, within readily accessible classical optical settings.
The past few years have witnessed a resurgence of interest in multimode structures, predominantly driven by the ever-increasing demand for higher information capacities. This renaissance, in turn, incited a flurry of activities in the general area of nonlinear multimode optics. The sheer complexity associated with the presence of hundreds or thousands of nonlinearly interacting modes that collectively act as a many-body system, has led to new opportunities in observing a multitude of novel optical effects that would have been otherwise impossible in single mode settings. In this talk, a thermodynamic theory capable of describing complex, highly multimoded, nonlinear optical systems is presented. It is shown that the mode occupancies in such nonlinear multimode arrangements follow a universal behavior that always tends to maximize the system’s entropy at steady-state. This thermodynamic response takes place irrespective of the type of nonlinearity involved and can be utilized to either heat or cool an optical multimode system. Aspects associated with adiabatic compressions and expansions will be discussed along with the possibility for all-optical Carnot cycles.
Usually photons are not conserved in their interaction with matter. Consequently, for the thermodynamics of photons, while we have a concept of temperature for energy conservation, there is no equivalent chemical potential for particle number conservation. However, the notion of a chemical potential is crucial in understanding a wide variety of single- and many-body effects, from transport in conductors and semiconductors to phase transitions in electronic and atomic systems. Here we show how a direct modification of the system-bath coupling via parametric oscillation creates an effective chemical potential for photons even in the thermodynamic limit. In particular, we show that the photonic system equilibrates to the temperature of the bath, with a tunable chemical potential that is set by the frequency of the parametric coupler. Specific implementations, using circuit-QED or optomechanics, are feasible using current technologies, and we show a detailed example demonstrating the emergence of Mott insulator--superfluid transition in a lattice of nonlinear oscillators. Our approach paves the way for quantum simulation, quantum sources, and even electronlike circuits with light.
Quantum frequency conversion (FC) in nonlinear optical media is a powerful tool for temporal-mode selective manipulation of light. Recent attempts at achieving high mode selectivities and/or fidelities have had to resort to multi-dimensional optimization schemes to determine the system's natural Schmidt modes. Certain combinations of relative-group velocities between the relevant frequency bands, medium length, and temporal pulse widths have been known to achieve good selectivities (exceeding 80%) for temporal modes that are nearly identical to pump pulse shapes, even for high conversion efficiencies. Working in this parameter regime using an off-the-shelf, second-harmonic generation, MgO:PPLN waveguide, and with pulses on the order of 500 fs at wavelengths around 800 nm, we verify experimentally that model-predicted Schmidt modes provide the high temporal-mode selectivity expected. The good agreement between experiment and theory paves the way to the implementation of a proposed two-stage FC scheme that is predicted by the present theory to reach near-perfect (100%) selectivity.