Quantum Control of Ultrafast Internal Conversion Using Nanoconfined Virtual Photons

2020 ◽  
Vol 11 (3) ◽  
pp. 1013-1021 ◽  
Author(s):  
Aleksandr G. Avramenko ◽  
Aaron S. Rury
2019 ◽  
Author(s):  
Aleksandr Avramenko ◽  
Aaron Rury

<div> <div> <div> <p>The rational control of non-radiative relaxation remains an unfulfilled goal for synthetic chemistry. In this study, we show strongly coupling an ensemble of molecules to the virtual photons of an electromagnetic cavity provides a rational handle over ultrafast, non-radiative dynamics. Specifically, we control the concentration of zinc tetraphenyl porphyrin molecules within nano-scale Fabry-Perot cavity structures to show a variable collective vacuum Rabi splitting between the polaritons coincides with changes in internal conversion rates. We find these changes obey a power law dependence on the collective vacuum Rabi splitting, but de- viate from the predictions of so-called gap laws. We also show simple theories of structural changes caused by polariton formation cannot explain discrepancies between our results and established theoretical predictions. Our results demonstrate a mechanism by which cavity polariton formation controls the fundamental photo-physics of light harvesting and photo- catalytic molecular moieties and the gap remaining in our fundamental understanding of these mechanisms. </p> </div> </div> </div>


2019 ◽  
Author(s):  
Aleksandr Avramenko ◽  
Aaron Rury

<div> <div> <div> <p>The rational control of non-radiative relaxation remains an unfulfilled goal for synthetic chemistry. In this study, we show strongly coupling an ensemble of molecules to the virtual photons of an electromagnetic cavity provides a rational handle over ultrafast, non-radiative dynamics. Specifically, we control the concentration of zinc tetraphenyl porphyrin molecules within nano-scale Fabry-Perot cavity structures to show a variable collective vacuum Rabi splitting between the polaritons coincides with changes in internal conversion rates. We find these changes obey a power law dependence on the collective vacuum Rabi splitting, but de- viate from the predictions of so-called gap laws. We also show simple theories of structural changes caused by polariton formation cannot explain discrepancies between our results and established theoretical predictions. Our results demonstrate a mechanism by which cavity polariton formation controls the fundamental photo-physics of light harvesting and photo- catalytic molecular moieties and the gap remaining in our fundamental understanding of these mechanisms. </p> </div> </div> </div>


2006 ◽  
Vol 125 (12) ◽  
pp. 124310 ◽  
Author(s):  
P. S. Christopher ◽  
M. Shapiro ◽  
P. Brumer

1964 ◽  
Vol 2 (4) ◽  
pp. 241-262 ◽  
Author(s):  
S. Forberg ◽  
E. Odeblad ◽  
R. Söremark ◽  
S. Ullberg

In a previous paper the absorption of γ-rays in the K-X-ray levels of the atom in which they are emitted was calculated according to the Quantum Mechanics, supposing the γ-rays to be emitted from a doublet of moment f ( t ) at the centre of the atom. The non-relativity wave equation derived from the relativity wave equation for an electron of charge — ε moving in an electro-magnetic field of vector potential K and scalar potential V is h 2 ∇ 2 ϕ + 2μ ( ih ∂/∂ t + εV + ih ε/μ c (K. grad)) ϕ = 0. (1) Suppose, however, that K involves the space co-ordinates. Then, (K. grad) ϕ ≠ (grad . K) ϕ , and the expression (K . grad) ϕ is not Hermitic. Equation (1) cannot therefore be the correct non-relativity wave equation for a single electron in an electron agnetic field, and we must substitute h 2 ∇ 2 ϕ + 2μ ( ih ∂/∂ t + εV) ϕ + ih ε/ c ((K. grad) ϕ + (grad. K) ϕ ) = 0. (2)


2009 ◽  
Vol 79 (3) ◽  
Author(s):  
Péter Kálmán ◽  
Tamás Keszthelyi

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