Pretražite po imenu i prezimenu autora, mentora, urednika, prevoditelja

Napredna pretraga

Pregled bibliografske jedinice broj: 900314

Mechanism of ultrafast non-reactive deactivation of the retinal chromophore in non-polar solvents


Mališ, Momir; Novak, Jurica; Zgrablić, Goran; Parmigiani, Fulvio; Došlić, Nađa
Mechanism of ultrafast non-reactive deactivation of the retinal chromophore in non-polar solvents // Physical chemistry chemical physics, 19 (2017), 38; 25970-25978 doi:10.1039/C7CP03293E (međunarodna recenzija, članak, znanstveni)


CROSBI ID: 900314 Za ispravke kontaktirajte CROSBI podršku putem web obrasca

Naslov
Mechanism of ultrafast non-reactive deactivation of the retinal chromophore in non-polar solvents

Autori
Mališ, Momir ; Novak, Jurica ; Zgrablić, Goran ; Parmigiani, Fulvio ; Došlić, Nađa

Izvornik
Physical chemistry chemical physics (1463-9076) 19 (2017), 38; 25970-25978

Vrsta, podvrsta i kategorija rada
Radovi u časopisima, članak, znanstveni

Ključne riječi
Non-reactive deactivation ; Retinal ; Nonadiabatic dynamics ; Protonated Schiff base of retinal ; Pump-probe spectroscopy

Sažetak
The photoisomerization of the all-trans protonated Schiff base of retinal (SBR+) in solution is highly inefficient. The present theoretical and experimental investigation aims at disclosing the mechanisms of ultrafast, non-reactive relaxation of SBR+ that lead to the drastic decrease in the isomerization yield in non- polar solvents. Our pump–probe measurements demonstrate the sensitivity of the all-trans SBR+ excited-state dynamics on the electrostatic interaction with the surrounding counterions and the crucial importance of the chromophore microenvironment. Our computational study focuses for the first time on the retinal chromophore–counterion pairs that are formed in non-polar solvents. By employing TDDFT-based nonadiabatic dynamics simulations and ADC(2) reaction paths calculations we found that internal conversion from the initially excited state to an inter- molecular charge transfer state with excitation localized on the counterion, leads to dissociation of the chromophore–counterion pair and to the abortion of isomerization. Barriers to conical intersection with the inter-molecular charge transfer state were found in the range 0.42–0.67 eV at the ADC(2) level. The existence of a barrier along the non-reactive relaxation pathways explains the observation that in solution the excitation on the blue edge of the SBR+ absorption leads to decrease in the isomerization yield with respect to the excitation at the red edge.

Izvorni jezik
Engleski

Znanstvena područja
Fizika, Kemija



POVEZANOST RADA


Projekt / tema
HRZZ-IP-2013-11-8238 - Računalna rješenja u bioznanostima: Značaj savitljivosti molekula (CompSoLS-MolFlex) (Matthew Smith, David, HRZZ - 2013-11 )

Ustanove
Institut "Ruđer Bošković", Zagreb

Profili:

Avatar Url Jurica Novak (autor)

Avatar Url Goran Zgrablić (autor)

Avatar Url Nađa Došlić (autor)

Avatar Url Momir Mališ (autor)

Citiraj ovu publikaciju

Mališ, Momir; Novak, Jurica; Zgrablić, Goran; Parmigiani, Fulvio; Došlić, Nađa
Mechanism of ultrafast non-reactive deactivation of the retinal chromophore in non-polar solvents // Physical chemistry chemical physics, 19 (2017), 38; 25970-25978 doi:10.1039/C7CP03293E (međunarodna recenzija, članak, znanstveni)
Mališ, M., Novak, J., Zgrablić, G., Parmigiani, F. & Došlić, N. (2017) Mechanism of ultrafast non-reactive deactivation of the retinal chromophore in non-polar solvents. Physical chemistry chemical physics, 19 (38), 25970-25978 doi:10.1039/C7CP03293E.
@article{article, year = {2017}, pages = {25970-25978}, DOI = {10.1039/C7CP03293E}, keywords = {Non-reactive deactivation, Retinal, Nonadiabatic dynamics, Protonated Schiff base of retinal, Pump-probe spectroscopy}, journal = {Physical chemistry chemical physics}, doi = {10.1039/C7CP03293E}, volume = {19}, number = {38}, issn = {1463-9076}, title = {Mechanism of ultrafast non-reactive deactivation of the retinal chromophore in non-polar solvents}, keyword = {Non-reactive deactivation, Retinal, Nonadiabatic dynamics, Protonated Schiff base of retinal, Pump-probe spectroscopy} }

Časopis indeksira:


  • Current Contents Connect (CCC)
  • Web of Science Core Collection (WoSCC)
    • Science Citation Index Expanded (SCI-EXP)
    • SCI-EXP, SSCI i/ili A&HCI
  • Scopus
  • MEDLINE


Citati





    Contrast
    Increase Font
    Decrease Font
    Dyslexic Font