Abstract：
:Phototropin is a blue light-activated photoreceptor that plays a dominant role in the phototropism of plants. The protein contains two subunits that bind flavin mononucleotide (FMN), which are responsible for the initial steps of the light-induced reaction. It has been proposed that the photoexcited flavin molecule adds a cysteine residue of the protein backbone, thus activating autophosphorylation of the enzyme. In this study, the electronic properties of several FMN-related compounds in different charge and spin states are characterized by means of ab initio quantum mechanical calculations. The model compounds serve as idealized model chromophores for phototropism. Reaction energies are estimated for simple model reactions, roughly representing the addition of a cysteine residue to the flavin molecule. Excitation energies were calculated with the help of time-dependent density functional theory. On the basis of these calculations we propose the following mechanism for the addition reaction: (1) after photoexcitation of FMN out of the singlet ground state S0, excited singlet state(s) are populated; these relax to the lowest excited singlet state S1, and subsequently by intersystem crossing FMN in the lowest triplet state, T1 is formed; (2) the triplet easily removes the neutral hydrogen atom from the H-S group of the cysteine residue; and (3) the resulting thio radical is added.
journal_name
Photochem Photobioljournal_title
Photochemistry and photobiologyauthors
Neiss C,Saalfrank Pdoi
10.1562/0031-8655(2003)077<0101:aiqcio>2.0.co;2subject
Has Abstractpub_date
2003-01-01 00:00:00pages
101-9issue
1eissn
0031-8655issn
1751-1097journal_volume
77pub_type
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