Dissipative Quantum Dynamics in Cavity Quantum Electrodynamics

1989 ◽  
pp. 607-608
Author(s):  
H. J. Kimble ◽  
M. G. Raizen ◽  
R. J. Thompson ◽  
R. J. Brecha ◽  
H. J. Carmichael ◽  
...  
2020 ◽  
Author(s):  
Sutirtha N. Chowdhury ◽  
Arkajit Mandal ◽  
Pengfei Huo

We use the ring-polymer (RP) representation to quantize the radiation field inside an optical cavity to investigate polariton quantum dynamics. Using a charge transfer model coupled to an optical cavity, we demonstrate that the RP quantization of the photon field provides accurate rate constants of the polariton mediated electron transfer (PMET) reaction compared to the Fermi's Golden rule. Because RP quantization uses extended phase space to describe the photon field, it significantly reduces the computational costs compared to the commonly used Fock states description of the radiation field. Compared to the other quasi-classical descriptions of the photon field, such as the classical Wigner model, the RP representation provides a much more accurate description of the polaritonic quantum dynamics, because it properly preserves the quantum distribution of the photonic DOF throughout the quantum dynamics propagation of the molecule-cavity hybrid system, whereas the classical Wigner model fails to do so. This work demonstrates the possibility of using the ring-polymer description to treat the quantized radiation field in polariton chemistry, offering an accurate and efficient approach for future investigations in cavity quantum electrodynamics.


1992 ◽  
pp. 316-316
Author(s):  
H. J. Kimble ◽  
G. Rempe ◽  
R. J. Thompson ◽  
R. J. Brecha

2019 ◽  
Author(s):  
Arkajit Mandal ◽  
Pengfei Huo

We perform quantum dynamics simulations to investigate new chemical reactivities enabled by cavity quantum electrodynamics. The quantum light-matter interactions between the molecule and the quantized radiation mode inside an optical cavity create a set of hybridized electronic-photonic states, so-called polaritons. The polaritonic states adapt the curvatures from both the ground and the excited electronic states, opening up new possibilities to control photochemical reactions by exploiting intrinsic quantum behaviors of light-matter interactions. With direct quantum dynamics simulations, we demonstrate that the selectivity of a model photo-isomerization reaction can be controlled by tuning the photon frequency of the cavity mode or the light-matter coupling strength, providing new ways to manipulate chemical reactions via light-matter interaction. We further investigate collective quantum effects enabled by coupling quantized radiation mode to multiple molecules. Our results suggest that in the resonance case, a photon is recycled among molecules to enable multiple excited state reactions, thus effectively functioning as a catalyst. In the non-resonance case, molecules emit and absorb virtual photons to initiate excited state reactions through fundamental quantum electrodynamics processes. These results from direct quantum dynamics simulations reveal basic principles of polariton photochemistry as well as promising reactivities that take advantage of intrinsic quantum behaviors of photons.


2019 ◽  
Author(s):  
Arkajit Mandal ◽  
Pengfei Huo

We perform quantum dynamics simulations to investigate new chemical reactivities enabled by cavity quantum electrodynamics. The quantum light-matter interactions between the molecule and the quantized radiation mode inside an optical cavity create a set of hybridized electronic-photonic states, so-called polaritons. The polaritonic states adapt the curvatures from both the ground and the excited electronic states, opening up new possibilities to control photochemical reactions by exploiting intrinsic quantum behaviors of light-matter interactions. With direct quantum dynamics simulations, we demonstrate that the selectivity of a model photo-isomerization reaction can be controlled by tuning the photon frequency of the cavity mode or the light-matter coupling strength, providing new ways to manipulate chemical reactions via light-matter interaction. We further investigate collective quantum effects enabled by coupling quantized radiation mode to multiple molecules. Our results suggest that in the resonance case, a photon is recycled among molecules to enable multiple excited state reactions, thus effectively functioning as a catalyst. In the non-resonance case, molecules emit and absorb virtual photons to initiate excited state reactions through fundamental quantum electrodynamics processes. These results from direct quantum dynamics simulations reveal basic principles of polariton photochemistry as well as promising reactivities that take advantage of intrinsic quantum behaviors of photons.


2020 ◽  
Author(s):  
Sutirtha N. Chowdhury ◽  
Arkajit Mandal ◽  
Pengfei Huo

We use the ring-polymer (RP) representation to quantize the radiation field inside an optical cavity to investigate polariton quantum dynamics. Using a charge transfer model coupled to an optical cavity, we demonstrate that the RP quantization of the photon field provides accurate rate constants of the polariton mediated electron transfer (PMET) reaction compared to the Fermi's Golden rule. Because RP quantization uses extended phase space to describe the photon field, it significantly reduces the computational costs compared to the commonly used Fock states description of the radiation field. Compared to the other quasi-classical descriptions of the photon field, such as the classical Wigner model, the RP representation provides a much more accurate description of the polaritonic quantum dynamics, because it properly preserves the quantum distribution of the photonic DOF throughout the quantum dynamics propagation of the molecule-cavity hybrid system, whereas the classical Wigner model fails to do so. This work demonstrates the possibility of using the ring-polymer description to treat the quantized radiation field in polariton chemistry, offering an accurate and efficient approach for future investigations in cavity quantum electrodynamics.


2018 ◽  
Vol 115 (50) ◽  
pp. 12662-12667 ◽  
Author(s):  
Po-Hsun Ho ◽  
Damon B. Farmer ◽  
George S. Tulevski ◽  
Shu-Jen Han ◽  
Douglas M. Bishop ◽  
...  

In cavity quantum electrodynamics, optical emitters that are strongly coupled to cavities give rise to polaritons with characteristics of both the emitters and the cavity excitations. We show that carbon nanotubes can be crystallized into chip-scale, two-dimensionally ordered films and that this material enables intrinsically ultrastrong emitter–cavity interactions: Rather than interacting with external cavities, nanotube excitons couple to the near-infrared plasmon resonances of the nanotubes themselves. Our polycrystalline nanotube films have a hexagonal crystal structure, ∼25-nm domains, and a 1.74-nm lattice constant. With this extremely high nanotube density and nearly ideal plasmon–exciton spatial overlap, plasmon–exciton coupling strengths reach 0.5 eV, which is 75% of the bare exciton energy and a near record for room-temperature ultrastrong coupling. Crystallized nanotube films represent a milestone in nanomaterials assembly and provide a compelling foundation for high-ampacity conductors, low-power optical switches, and tunable optical antennas.


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