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

Author(s):  
Akhila Kadyan ◽  
Anil Shaji ◽  
Jino George

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.

2021 ◽  
Author(s):  
Akhila Kadyan ◽  
Anil Shaji ◽  
Jino George

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.


Author(s):  
Hidefumi Hiura ◽  
Atef Shalabney ◽  
Jino George

<p>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<br>approach to catalysis by ultra-strongly coupling the vibrations of the reactants to the infrared vacuum electromagnetic field. To demonstrate the possibility of such<br>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<br>10<sup>2</sup>-fold and that of ammonia borane by 10<sup>4</sup>-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.</p>


2021 ◽  
Author(s):  
Hidefumi Hiura ◽  
Atef Shalabney

<p>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<br>approach to catalysis by ultra-strongly coupling the vibrations of the reactants to the infrared vacuum electromagnetic field. To demonstrate the possibility of such<br>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<br>10<sup>2</sup>-fold and that of ammonia borane by 10<sup>4</sup>-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.</p>


Author(s):  
Hidefumi Hiura ◽  
Atef Shalabney ◽  
Jino George

<p>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<br>approach to catalysis by ultra-strongly coupling the vibrations of the reactants to the infrared vacuum electromagnetic field. To demonstrate the possibility of such<br>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<br>10<sup>2</sup>-fold and that of ammonia borane by 10<sup>4</sup>-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.</p>


Author(s):  
Hidefumi Hiura ◽  
Atef Shalabney ◽  
Jino George

<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>


Author(s):  
Hidefumi Hiura ◽  
Atef Shalabney ◽  
Jino George

<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>


1996 ◽  
Vol 10 (19) ◽  
pp. 891-901
Author(s):  
AMITABH JOSHI

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.


Author(s):  
Hidefumi Hiura ◽  
Atef Shalabney ◽  
Jino George

<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>


2013 ◽  
Vol 38 (10) ◽  
pp. 1591 ◽  
Author(s):  
Zheng Xi ◽  
Yonghua Lu ◽  
Wenhai Yu ◽  
Peijun Yao ◽  
Pei Wang ◽  
...  

2021 ◽  
Author(s):  
Abbas Hamouleh-Alipour ◽  
Ali Mir ◽  
Ali Farmani

Abstract Bolometer sensors are prominent and excellent choice in technology because they do not need cooling. The trade-off between high sensitivity, fast response time, and strong light absorption is a key important challenge in bolometer sensors. Here, the bolometric effect for a high resistance sensitivity plasmonic sensing of total and profile infusion of radiation is studied for the proposed bolometer sensor based on plasmonic multilayer structure at 26° C. In the present study, by generating strong coupling condition between incident wave and surface plasmon polaritons (SPPs), a very narrow absorption spectra with high figure of merit (FoM) is achieved. The analytical model and numerical simulation are fulfilled based on the transfer matrix method (TMM) and 3-D finite-difference time-domain (FDTD), respectively. The narrow absorption spectra that generate by strong coupling with SPPs heats the silver thin film that leads to variation in temperature and supports TE surface mode. This temperature change rectifies the resistance of the metal thin film by the bolometric effect. So, optical characteristics of the proposed metasurface bolometer sensor, including quality factor (Q), sensitivity, and figure of merit (FoM) are calculated that Max sensitivity, FoM, and Q are 17.2 RIU-1, 530 and 434.5, respectively. Finally, we analytically simulate the temperature coefficient of resistance (TCR) in terms of wavelength and refractive index of analyte (na) that this resistance change can be monitored by an external electric model. The proposed plasmonic multilayer configuration is a very compact footprint structure that achieved high resistance sensitivity and FoM in comparison with any previous reports. This proposed thermal, optical, and electric plasmonic metasurface bolometer sensor can be used in different applications such as biophysics, biology, and environmental science.


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