Strong coupling between plasmonic Fabry–Pérot cavity mode and magnetic plasmon

In this letter, we investigated the modification of oscillator strength of an asymmetric stretching band of CS2 by strong coupling to an infrared cavity photon. This is achieved by placing liquid CS2 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 CS2 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.

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Cavity Catalysis ‒Accelerating Reactions under Vibrational Strong Coupling‒

10.26434/chemrxiv.7234721.v3 ◽

2018 ◽

Cited By ~ 8

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

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 ℏΩR of 92 meV (740 cm−1), 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 102 times and that of ammonia borane by 104 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.

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Cavity Catalysis ‒Accelerating Reactions under Vibrational Strong Coupling‒

10.26434/chemrxiv.7234721.v2 ◽

2018 ◽

Cited By ~ 2

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

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 ℏΩR of 92 meV (740 cm−1), 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 102 times and that of ammonia borane by 104 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.

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Vacuum-Field Catalysis: Accelerated Reactions by Vibrational Ultra Strong Coupling

10.26434/chemrxiv.7234721.v4 ◽

2019 ◽

Cited By ~ 2

Author(s):

Hidefumi Hiura ◽

Atef Shalabney ◽

Jino George

Keyword(s):

Strong Coupling ◽

Reaction Rate ◽

Cavity Mode ◽

Reaction Path ◽

Vacuum Field ◽

Coupling Ratio ◽

Fabry Perot ◽

Fresh Perspective ◽

Light Matter Interaction ◽

Splitting Energy

In conventional catalysis, the reactants interact with specific sites of the catalyst in such a way that the reaction barrier is lowered by changing the reaction path, causing the reaction rate to be accelerated. Here we take a radically different approach to catalysis by ultra-strongly coupling the vibrations of the reactants to the infrared vacuum electromagnetic field. To demonstrate the possibility of such vacuum-field catalysis (or cavity catalysis), we have studied hydrolysis reactions under the vibrational ultra strong coupling (V-USC) of the OH stretching mode of water to a Fabry-Pérot microfluidic cavity mode. This results in a giant Rabi splitting energy (92 meV), indicating the system is in the V-USC regime. We have found that V-USC water enhances the hydrolysis reaction rate of cyanate ions by 102-fold and that of ammonia borane by 104-fold. This catalytic ability is found to depend upon the coupling ratio of the vibrational light-matter interaction. Given the vital importance of water for life and human activities, we expect that our finding not only offers an unconventional way of controlling chemical reactions by vacuum-field catalysis but also brings a fresh perspective to science and technology.

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Vacuum-Field Catalysis: Accelerated Reactions by Vibrational Ultra Strong Coupling

10.26434/chemrxiv.7234721.v5 ◽

2021 ◽

Author(s):

Hidefumi Hiura ◽

Atef Shalabney

Keyword(s):

Strong Coupling ◽

Reaction Rate ◽

Cavity Mode ◽

Reaction Path ◽

Vacuum Field ◽

Coupling Ratio ◽

Fabry Perot ◽

Fresh Perspective ◽

Light Matter Interaction ◽

Splitting Energy

In conventional catalysis, the reactants interact with specific sites of the catalyst in such a way that the reaction barrier is lowered by changing the reaction path, causing the reaction rate to be accelerated. Here we take a radically different approach to catalysis by ultra-strongly coupling the vibrations of the reactants to the infrared vacuum electromagnetic field. To demonstrate the possibility of such vacuum-field catalysis (or cavity catalysis), we have studied hydrolysis reactions under the vibrational ultra strong coupling (V-USC) of the OH stretching mode of water to a Fabry-Pérot microfluidic cavity mode. This results in a giant Rabi splitting energy (92 meV), indicating the system is in the V-USC regime. We have found that V-USC water enhances the hydrolysis reaction rate of cyanate ions by 102-fold and that of ammonia borane by 104-fold. This catalytic ability is found to depend upon the coupling ratio of the vibrational light-matter interaction. Given the vital importance of water for life and human activities, we expect that our finding not only offers an unconventional way of controlling chemical reactions by vacuum-field catalysis but also brings a fresh perspective to science and technology.

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

10.26434/chemrxiv.14060636.v1 ◽

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 CS2 by strong coupling to an infrared cavity photon. This is achieved by placing liquid CS2 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 CS2 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.

Download Full-text

Vacuum-Field Catalysis: Accelerated Reactions by Vibrational Ultra Strong Coupling

10.26434/chemrxiv.7234721 ◽

2019 ◽

Cited By ~ 1

Author(s):

Hidefumi Hiura ◽

Atef Shalabney ◽

Jino George

Keyword(s):

Strong Coupling ◽

Reaction Rate ◽

Cavity Mode ◽

Reaction Path ◽

Vacuum Field ◽

Coupling Ratio ◽

Fabry Perot ◽

Fresh Perspective ◽

Light Matter Interaction ◽

Splitting Energy

In conventional catalysis, the reactants interact with specific sites of the catalyst in such a way that the reaction barrier is lowered by changing the reaction path, causing the reaction rate to be accelerated. Here we take a radically different approach to catalysis by ultra-strongly coupling the vibrations of the reactants to the infrared vacuum electromagnetic field. To demonstrate the possibility of such vacuum-field catalysis (or cavity catalysis), we have studied hydrolysis reactions under the vibrational ultra strong coupling (V-USC) of the OH stretching mode of water to a Fabry-Pérot microfluidic cavity mode. This results in a giant Rabi splitting energy (92 meV), indicating the system is in the V-USC regime. We have found that V-USC water enhances the hydrolysis reaction rate of cyanate ions by 102-fold and that of ammonia borane by 104-fold. This catalytic ability is found to depend upon the coupling ratio of the vibrational light-matter interaction. Given the vital importance of water for life and human activities, we expect that our finding not only offers an unconventional way of controlling chemical reactions by vacuum-field catalysis but also brings a fresh perspective to science and technology.

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SPONTANEOUS EMISSION BY MOVING ATOMS UNDERGOING TWO PHOTON-TRANSITION IN THE STRONG COUPLING REGIME

Modern Physics Letters B ◽

10.1142/s0217984996001012 ◽

1996 ◽

Vol 10 (19) ◽

pp. 891-901

Author(s):

AMITABH JOSHI

Keyword(s):

Strong Coupling ◽

Spontaneous Emission ◽

Cavity Mode ◽

Strong Coupling Regime ◽

Mode Structure ◽

Field Mode ◽

Two Photon ◽

Photon Transition ◽

Fabry Perot ◽

Excitation Probability

The dependence of spontaneous emission on atomic motion for an atom undergoing two-photon transition and moving along the axis of a Fabry-Perot cavity is analyzed here. For this purpose we consider the strong coupling limit of atom and cavity field mode and demonstrate the effects of atomic velocity and spatial mode structure of cavity mode on the excitation probability of atom.

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Cavity Catalysis ‒Accelerating Reactions under Vibrational Strong Coupling‒

10.26434/chemrxiv.7234721.v1 ◽

2018 ◽

Cited By ~ 2

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

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 ℏΩR of 92 meV (740 cm−1), 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 102 times and that of ammonia borane by 104 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.

Download Full-text