scholarly journals Communication: Autodetachment versus internal conversion from the S1 state of the isolated GFP chromophore anion

2013 ◽  
Vol 139 (7) ◽  
pp. 071104 ◽  
Author(s):  
Christopher W. West ◽  
Alex S. Hudson ◽  
Steven L. Cobb ◽  
Jan R. R. Verlet
Keyword(s):  
Internal Conversion ◽  
Gfp Chromophore

scholarly journals Internal conversion of the anionic GFP chromophore: in and out of the I-twisted S1/S0 conical intersection seam

2022 ◽  
Author(s):  
Nanna H. List ◽  
Chey M. Jones ◽  
Todd J. Martínez
Keyword(s):  
Quantum Yield ◽  
Internal Conversion ◽  
Conical Intersection ◽  
Statistical Dynamics ◽  
Statistical Behavior ◽  
Gfp Chromophore

The Z–E photoisomerization quantum yield of the HBDI− chromophore is a result of early, non-statistical dynamics around a less reactive I-twisted intersection and later, statistical behavior around the more reactive, near-enantiomeric counterpart.

scholarly journals Internal Conversion of the Anionic GFP Chromophore: In and Out of the I-twisted S1/S0 Conical Intersection Seam

2021 ◽  
Author(s):  
Nanna Holmgaard List ◽  
Chey Marcel Jones ◽  
Todd J. Martínez
Keyword(s):  
Internal Conversion ◽  
Fluorescent Protein ◽  
Dynamical Behavior ◽  
Super Resolution ◽  
Ultrafast Relaxation ◽  
Gfp Chromophore ◽  
Adiabatic Dynamics ◽  
Dynamics Simulations ◽  
Green Fluorescent ◽  
Super Resolution Microscopy

<p>The functional diversity of the green fluorescent protein (GFP) family is intimately connected to the interplay between competing photo-induced transformations of the chromophore motif, anionic <i>p</i>-hydroxybenzylidene-2,3-dimethylimidazolinone (HBDI<sup>–</sup>). Its propensity to undergo <i>Z/E</i> photoisomerization following excitation to the S<sub>1</sub>(pp<sup>*</sup>) state is of particular importance for super-resolution microscopy and emerging opportunities in optogenetics. However, key dynamical aspects of this process and its range of tunability still remain elusive. Here, we investigate the internal conversion behavior intrinsic to HBDI<sup>–</sup> with focus on competing deactivation pathways, rate and yield of photoisomerization. Based on non-adiabatic dynamics simulations, we confirm that non-selective progress along the two bridge-torsional (i.e., phenolate, P, or imidazolinone, I) pathways can account for the three decay constants reported experimentally, leading to competing ultrafast relaxation along the I-twisted pathway and S<sub>1 </sub>trapping along the P-torsion. The majority of the population (~70%) is transferred to S<sub>0</sub> in the vicinity of two near-symmetry-related minima on the I-twisted intersection seam (MECI-Is). Despite their reactant-biased topographies, our account of inertial effects suggests that isomerization not only occurs as a thermal process on the vibrationally hot ground state but also as a direct photoreaction with a total quantum yield of ~40%.</p><p>By comparing the non-adiabatic dynamics to a photoisomerization committor analysis, we provide a detailed mapping of the intrinsic photoreactivity and dynamical behavior of the two MECI-Is. Our work offers new insight into the internal conversion process of HBDI<sup>–</sup> that enlightens principles for the design of chromophore derivatives and protein variants with improved photoswitching properties.</p>

scholarly journals Strong electron donation induced differential nonradiative decay pathways for para and meta GFP chromophore analogues

2015 ◽  
Vol 17 (32) ◽  
pp. 20515-20521 ◽  
Author(s):  
Tanmay Chatterjee ◽  
Mrinal Mandal ◽  
Venkatesh Gude ◽  
Partha Pratim Bag ◽  
Prasun K. Mandal
Keyword(s):  
Charge Transfer ◽  
Internal Conversion ◽  
Strong Electron ◽  
Nonradiative Decay ◽  
Gfp Chromophore ◽  
Electron Donation

Charge transfer induced nonradiative internal conversion for meta GFP chromophore analogues is studied.

Viscosity-Dependent Fluorescence Decay of the GFP Chromophore in Solution Due to Fast Internal Conversion

2002 ◽  
Vol 106 (30) ◽  
pp. 7554-7559 ◽  
Author(s):  
Andreas D. Kummer ◽  
Christian Kompa ◽  
Haruki Niwa ◽  
Takashi Hirano ◽  
Satoshi Kojima ◽  
...  
Keyword(s):  
Internal Conversion ◽  
Fluorescence Decay ◽  
Gfp Chromophore

scholarly journals Internal Conversion of the Anionic GFP Chromophore: In and Out of the I-twisted S1/S0 Conical Intersection Seam

2021 ◽  
Author(s):  
Nanna Holmgaard List ◽  
Chey Marcel Jones ◽  
Todd J. Martínez
Keyword(s):  
Internal Conversion ◽  
Fluorescent Protein ◽  
Dynamical Behavior ◽  
Super Resolution ◽  
Ultrafast Relaxation ◽  
Gfp Chromophore ◽  
Adiabatic Dynamics ◽  
Dynamics Simulations ◽  
Green Fluorescent ◽  
Super Resolution Microscopy

<p>The functional diversity of the green fluorescent protein (GFP) family is intimately connected to the interplay between competing photo-induced transformations of the chromophore motif, anionic <i>p</i>-hydroxybenzylidene-2,3-dimethylimidazolinone (HBDI<sup>–</sup>). Its propensity to undergo <i>Z/E</i> photoisomerization following excitation to the S<sub>1</sub>(pp<sup>*</sup>) state is of particular importance for super-resolution microscopy and emerging opportunities in optogenetics. However, key dynamical aspects of this process and its range of tunability still remain elusive. Here, we investigate the internal conversion behavior intrinsic to HBDI<sup>–</sup> with focus on competing deactivation pathways, rate and yield of photoisomerization. Based on non-adiabatic dynamics simulations, we confirm that non-selective progress along the two bridge-torsional (i.e., phenolate, P, or imidazolinone, I) pathways can account for the three decay constants reported experimentally, leading to competing ultrafast relaxation along the I-twisted pathway and S<sub>1 </sub>trapping along the P-torsion. The majority of the population (~70%) is transferred to S<sub>0</sub> in the vicinity of two near-symmetry-related minima on the I-twisted intersection seam (MECI-Is). Despite their reactant-biased topographies, our account of inertial effects suggests that isomerization not only occurs as a thermal process on the vibrationally hot ground state but also as a direct photoreaction with a total quantum yield of ~40%.</p><p>By comparing the non-adiabatic dynamics to a photoisomerization committor analysis, we provide a detailed mapping of the intrinsic photoreactivity and dynamical behavior of the two MECI-Is. Our work offers new insight into the internal conversion process of HBDI<sup>–</sup> that enlightens principles for the design of chromophore derivatives and protein variants with improved photoswitching properties.</p>

Structural Evidence of Photoisomerization Pathways in Fluorescent Proteins

2019 ◽  
Author(s):  
Jeffrey Chang ◽  
Matthew Romei ◽  
Steven Boxer
Keyword(s):  
Rational Design ◽  
Fluorescent Protein ◽  
Fluorescent Proteins ◽  
Super Resolution ◽  
Unit Cell Size ◽  
Chlorine Substituent ◽  
Gfp Chromophore ◽  
The One ◽  
Green Fluorescent ◽  
Super Resolution Microscopy

<p>Double-bond photoisomerization in molecules such as the green fluorescent protein (GFP) chromophore can occur either via a volume-demanding one-bond-flip pathway or via a volume-conserving hula-twist pathway. Understanding the factors that determine the pathway of photoisomerization would inform the rational design of photoswitchable GFPs as improved tools for super-resolution microscopy. In this communication, we reveal the photoisomerization pathway of a photoswitchable GFP, rsEGFP2, by solving crystal structures of <i>cis</i> and <i>trans</i> rsEGFP2 containing a monochlorinated chromophore. The position of the chlorine substituent in the <i>trans</i> state breaks the symmetry of the phenolate ring of the chromophore and allows us to distinguish the two pathways. Surprisingly, we find that the pathway depends on the arrangement of protein monomers within the crystal lattice: in a looser packing, the one-bond-flip occurs, whereas in a tighter packing (7% smaller unit cell size), the hula-twist occurs.</p><p> </p><p> </p><p> </p><p> </p><p> </p><p> </p> <p> </p>

Autoradiography with Isotopes Emitting Internal Conversion Electrons and Auger Electrons

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

scholarly journals The internal conversion of gamma-rays.—Part II

1928 ◽  
Vol 121 (787) ◽  
pp. 447-456
Keyword(s):  
Magnetic Field ◽  
Quantum Mechanics ◽  
Wave Equation ◽  
Gamma Rays ◽  
Internal Conversion ◽  
Scalar Potential ◽  
X Ray ◽  
Electro Magnetic Field ◽  
Γ Rays ◽  
Electro Magnetic

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)

Lattice effect in solid state internal conversion

2009 ◽  
Vol 79 (3) ◽  
Author(s):  
Péter Kálmán ◽  
Tamás Keszthelyi
Keyword(s):  
Solid State ◽  
Internal Conversion ◽  
Lattice Effect
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