scholarly journals Nonlinear infrared polaritonic interaction between cavities mediated by molecular vibrations at ultrafast time scale

2021 ◽  
Vol 7 (19) ◽  
pp. eabf6397
Author(s):  
Bo Xiang ◽  
Jiaxi Wang ◽  
Zimo Yang ◽  
Wei Xiong
Keyword(s):  
Strong Coupling ◽  
Chemical Reactions ◽  
Time Scale ◽  
Cavity Mode ◽  
Science And Technology ◽  
Nonlinear Interactions ◽  
Vibrational Modes ◽  
Molecular Vibrations ◽  
Quantum Simulations ◽  
Molecular Vibrational Modes

Realizing nonlinear interactions between spatially separated particles can advance molecular science and technology, including remote catalysis of chemical reactions, ultrafast processing of information in infrared (IR) photonic circuitry, and advanced platforms for quantum simulations with increased complexity. Here, we achieved nonlinear interactions at ultrafast time scale between polaritons contained in spatially adjacent cavities in the mid-IR regime, altering polaritons in one cavity by pumping polaritons in an adjacent one. This was done by strong coupling molecular vibrational modes with photon modes, a process that combines characteristics of both photon delocalization and molecular nonlinearity. The dual photon/molecule character of polaritons enables delocalized nonlinearity—a property that neither molecular nor cavity mode would have alone.

scholarly journals Cavity Catalysis ‒Accelerating Reactions under Vibrational Strong Coupling‒

2018 ◽  
Author(s):  
Hidefumi Hiura ◽  
Atef Shalabney ◽  
Jino George
Keyword(s):  
Electromagnetic Field ◽  
Strong Coupling ◽  
Chemical Reactions ◽  
Reaction Rate ◽  
Cavity Mode ◽  
Coupling Ratio ◽  
Strong Light ◽  
Rabi Splitting ◽  
Fabry Perot ◽  
Splitting Energy

<p>In conventional catalysis the reactants interact with specific sites of the catalyst in such a way that the reaction barrier is lowered and the reaction rate is accelerated. Here we take a radically different approach to catalysis by strongly coupling the vibrations of the reactants to the vacuum electromagnetic field of a cavity. To demonstrate the possibility of such cavity catalysis, we have studied hydrolysis reactions under strong coupling of the OH stretching mode of water to a Fabry-Pérot (FP) microfluidic cavity mode. This results in an exceptionally large Rabi splitting energy ℏΩ<sub>R</sub> of 92 meV (740 cm<sup>−1</sup>), indicating the system is in vibrational ultra-strong coupling (V-USC) regime and we have found that it enhances the hydrolysis reaction rate of cyanate ions by 10<sup>2</sup> times and that of ammonia borane by 10<sup>4</sup> times. This catalytic ability is shown to depend only upon the cavity tuning and the coupling ratio. Given the vital importance of water for life and human activities, we expect our finding not only offers an unconventional way of controlling chemical reactions by ultra-strong light-matter interactions, but also changes the landscape of chemistry in a fundamental way.</p>

scholarly journals Cavity Catalysis ‒Accelerating Reactions under Vibrational Strong Coupling‒

2018 ◽  
Author(s):  
Hidefumi Hiura ◽  
Atef Shalabney ◽  
Jino George
Keyword(s):  
Electromagnetic Field ◽  
Strong Coupling ◽  
Chemical Reactions ◽  
Reaction Rate ◽  
Cavity Mode ◽  
Coupling Ratio ◽  
Strong Light ◽  
Rabi Splitting ◽  
Fabry Perot ◽  
Splitting Energy

<p>In conventional catalysis the reactants interact with specific sites of the catalyst in such a way that the reaction barrier is lowered and the reaction rate is accelerated. Here we take a radically different approach to catalysis by strongly coupling the vibrations of the reactants to the vacuum electromagnetic field of a cavity. To demonstrate the possibility of such cavity catalysis, we have studied hydrolysis reactions under strong coupling of the OH stretching mode of water to a Fabry-Pérot (FP) microfluidic cavity mode. This results in an exceptionally large Rabi splitting energy ℏΩ<sub>R</sub> of 92 meV (740 cm<sup>−1</sup>), indicating the system is in vibrational ultra-strong coupling (V-USC) regime and we have found that it enhances the hydrolysis reaction rate of cyanate ions by 10<sup>2</sup> times and that of ammonia borane by 10<sup>4</sup> times. This catalytic ability is shown to depend only upon the cavity tuning and the coupling ratio. Given the vital importance of water for life and human activities, we expect our finding not only offers an unconventional way of controlling chemical reactions by ultra-strong light-matter interactions, but also changes the landscape of chemistry in a fundamental way.</p>

Infrarot-Photochemie mit Lasern? / Infrared Photochemistry with Lasers?

1972 ◽  
Vol 27 (2) ◽  
pp. 89-94 ◽  
Author(s):  
Karl L. Kompa
Keyword(s):  
Energy Transfer ◽  
Chemical Reactions ◽  
Degrees Of Freedom ◽  
Reaction Rates ◽  
Chemical Processes ◽  
Experimental Results ◽  
Vibrational Modes ◽  
Selective Heating ◽  
Molecular Vibrational Modes ◽  
Resonance Laser

The possibility of controlled chemical reactions by resonance laser activation of molecular vibrational modes is considered. This produces a selective heating of one or more vibrational degrees of freedom and a correspondingly rapid increase in the reaction rates. The competition between chemical processes and relaxation by energy transfer to other degrees of freedom is discussed. The verification of this new reaction principle requires lasers with realistic parameters. A few experimental results are reviewed.

scholarly journals Cavity Catalysis ‒Accelerating Reactions under Vibrational Strong Coupling‒

2018 ◽  
Author(s):  
Hidefumi Hiura ◽  
Atef Shalabney ◽  
Jino George
Keyword(s):  
Electromagnetic Field ◽  
Strong Coupling ◽  
Chemical Reactions ◽  
Reaction Rate ◽  
Cavity Mode ◽  
Coupling Ratio ◽  
Strong Light ◽  
Rabi Splitting ◽  
Fabry Perot ◽  
Splitting Energy

<p>In conventional catalysis the reactants interact with specific sites of the catalyst in such a way that the reaction barrier is lowered and the reaction rate is accelerated. Here we take a radically different approach to catalysis by strongly coupling the vibrations of the reactants to the vacuum electromagnetic field of a cavity. To demonstrate the possibility of such cavity catalysis, we have studied hydrolysis reactions under strong coupling of the OH stretching mode of water to a Fabry-Pérot (FP) microfluidic cavity mode. This results in an exceptionally large Rabi splitting energy ℏΩ<sub>R</sub> of 92 meV (740 cm<sup>−1</sup>), indicating the system is in vibrational ultra-strong coupling (V-USC) regime and we have found that it enhances the hydrolysis reaction rate of cyanate ions by 10<sup>2</sup> times and that of ammonia borane by 10<sup>4</sup> times. This catalytic ability is shown to depend only upon the cavity tuning and the coupling ratio. Given the vital importance of water for life and human activities, we expect our finding not only offers an unconventional way of controlling chemical reactions by ultra-strong light-matter interactions, but also changes the landscape of chemistry in a fundamental way.</p>

Weak Coupling Strategy for Multi-Physics CFD Simulation in Engineering Problems

2011 ◽  
Author(s):  
Makoto Yamamoto ◽  
Masaya Suzuki
Keyword(s):  
Strong Coupling ◽  
Time Scale ◽  
Weak Coupling ◽  
Particle Deposition ◽  
Cfd Simulation ◽  
The Other ◽  
Cfd Simulations ◽  
Sand Erosion ◽  
Coupling Strategy ◽  
The Difference

Multi-Physics CFD Simulation will be one of key technologies in various engineering fields. There are two strategies to simulate a multi-physics phenomenon. One is “Strong Coupling”, and the other is “Weak Coupling”. Each can be employed, based on time-scales of physics embedded in a problem. That is, when a time-scale of one physics is nearly same as that of the other physics, we have to use Strong Coupling to take into account the interaction between two physics. On the other hand, when one time-scale is quite different from the other one, Weak Coupling can be applied. Considering the present computer performance, Strong Coupling is difficult to be used in engineering design processes now. Therefore, we are focusing on Weak Coupling, and it has been applied to a number of multi-physics CFD simulations in engineering. We have successfully simulated sand erosion, ice accretion, particle deposition, electro-chemical machining and so on, with using Weak Coupling method. In the present study, the difference between strong and weak couplings is briefly described, and two examples of our multi-physics CFD simulations are expressed. The numerical results indicate that Weak Coupling strategy is promising in a lot of multi-physics CFD simulations.

scholarly journals Boosting Self-interaction of Molecular Vibrations under Ultra-strong Coupling Condition

2021 ◽  
Author(s):  
Akhila Kadyan ◽  
Anil Shaji ◽  
Jino George
Keyword(s):  
Oscillator Strength ◽  
Strong Coupling ◽  
Cavity Mode ◽  
Linear Increase ◽  
Vacuum Field ◽  
New Paradigm ◽  
Coupling Condition ◽  
Field Coupling ◽  
Fabry Perot ◽  
Set Up

In this letter, we investigated the modification of oscillator strength of an asymmetric stretching band of CS<sub>2</sub> by strong coupling to an infrared cavity photon. This is achieved by placing liquid CS<sub>2</sub> in a Fabry-Perot resonator and tune the cavity mode position to match with the molecular vibrational transition. Ultra-strong coupling improves the self-interaction of transition dipoles of asymmetric stretching band of CS<sub>2</sub> that resulted in an increase of its own oscillator strength. We experimentally proved this by taking the area ratio of asymmetric stretching and combination band by selectively coupling the former one. A non-linear increase in the oscillator strength of the asymmetric stretching band is observed upon varying the coupling strength. This is explained by a quantum mechanical model that predicts quadratic behavior under ultra-strong coupling condition. These findings will set up a new paradigm for understanding chemical reaction modification by vacuum field coupling.

scholarly journals Resonant catalysis of thermally activated chemical reactions with vibrational polaritons

2019 ◽  
Vol 10 (1) ◽  
Author(s):  
Jorge A. Campos-Gonzalez-Angulo ◽  
Raphael F. Ribeiro ◽  
Joel Yuen-Zhou
Keyword(s):  
Electron Transfer ◽  
Chemical Kinetics ◽  
Chemical Reactions ◽  
Cavity Mode ◽  
Resonant Cavity ◽  
Quantum States ◽  
Transfer Model ◽  
Dark State ◽  
Thermally Activated ◽  
Two Hybrid

Abstract Interaction between light and matter results in new quantum states whose energetics can modify chemical kinetics. In the regime of ensemble vibrational strong coupling (VSC), a macroscopic number $$N$$ N of molecular transitions couple to each resonant cavity mode, yielding two hybrid light–matter (polariton) modes and a reservoir of $$N-1$$ N − 1 dark states whose chemical dynamics are essentially those of the bare molecules. This fact is seemingly in opposition to the recently reported modification of thermally activated ground electronic state reactions under VSC. Here we provide a VSC Marcus–Levich–Jortner electron transfer model that potentially addresses this paradox: although entropy favors the transit through dark-state channels, the chemical kinetics can be dictated by a few polaritonic channels with smaller activation energies. The effects of catalytic VSC are maximal at light–matter resonance, in agreement with experimental observations.

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