2019
DOI: 10.1021/acs.biochem.8b01275
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Reverse Photodynamics of the Noncanonical Red/Green NpR3784 Cyanobacteriochrome from Nostoc punctiforme

Abstract: In the companion paper (10.1021/acs.biochem.8b01274), we examined the forward P r photodynamics of NpR3784 (UniProtKB B2J457), a representative member of a noncanonical red/green (R/G) cyanobacteriochrome (CBCR) subfamily. Here the reverse P g → P r photodynamics of NpR3784 was studied by broadband transient absorption pump−probe spectroscopy. Primary (100 fs to 10 ns) and secondary (10 ns to 1 ms) photodynamics were characterized over nine decades of time, which also were complemented with temperature-jump cr… Show more

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Cited by 7 publications
(6 citation statements)
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“…The earliest signals after excitation of Pg samples (Fig. 5 A, 100 ps) are also in good agreement with the literature on Slr-g3 [13] and related red/green CBCRs [49,50]. Here, the positive signal around 700 nm was assigned to ESA, while the negative features at 525 and 625 nm correspond to GSB and SE, respectively.…”
Section: Pg* Decay Vis Spectral Rangesupporting
confidence: 89%
“…The earliest signals after excitation of Pg samples (Fig. 5 A, 100 ps) are also in good agreement with the literature on Slr-g3 [13] and related red/green CBCRs [49,50]. Here, the positive signal around 700 nm was assigned to ESA, while the negative features at 525 and 625 nm correspond to GSB and SE, respectively.…”
Section: Pg* Decay Vis Spectral Rangesupporting
confidence: 89%
“…The double-bump structure of the 180 to 220 K spectra (Figure B) does not compare well with that of the Meta-R y SADS from the primary and secondary signals (Figures B and B). A similar equilibrium was observed in the cryokinetics signals of the NpR6012g4 domain and likely corresponds to coexisting Meta-R o (615 nm) and Meta-R y (570 nm) populations (Figure B). The terminal 230 K spectrum blue-shifts into a green-absorbing Meta-R g intermediate that evolves into 15 E P g at higher temperatures (Figure and Figure S7).…”
Section: Resultsmentioning
confidence: 98%
“…The observation of unproductive 15 E P g * subpopulations in one or more CBCRs in all three classes suggests that inhomogeneity is a consistent trend for the reverse photoreaction of all three classes of red/green CBCRs. Such unproductive excited-state populations likely are present in the majority of photoactive biliproteins, as they have been reported in noncanonical red/green (NpR3784), noncanonical orange/green (NpF2164g7), green/red (RcaE), , and insert-cysteine (NpF2164g3) CBCRs. For the reverse reactions of NpF2164g3 and NpF2164g7 as well as both forward and reverse reactions of RcaE, , the spectra of photoinactive and photoactive excited-state populations were indistinguishable.…”
Section: Discussionmentioning
confidence: 80%
“…The reverse reaction signals exhibit multiexponential excited-state kinetics, which argues for the use of the inhomogeneous target models previously proposed for the reverse dynamics of other CBCRs. ,, One can also model a homogeneous ground state that is excited into heterogeneous excited states, but the heterogeneous ground-state model was preferred given the evidence for ground-state inhomogeneity previously reported . The parameters for the fits are listed in Tables S1 and S2.…”
Section: Global Analysismentioning
confidence: 90%