Time-resolved two-photon spectroscopy of carotenoids

Šebelík, Václav; Fuciman, Marcel; West, Robert G.; Polı́vka, Tomáš

doi:10.1016/j.chemphys.2019.02.023

Cited by 3 publications

(5 citation statements)

References 53 publications

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“…A brand-new challenge for the theoretical approaches was set by the femtosecond time-resolved two-photon excitation (2PE) experiments. − Due to its multielectron character, the S 0 -S 1 transition is one-photon forbidden, but two-photon allowed. Considering that two-photon excitation does not populate the S 2 , the 2PE transient absorption spectra can be viewed as the “pure” S 1 state, minimizing artifacts arising from the depopulation of the higher lying energy levels.…”

Section: Perspective: Vera On Two-photon Initiated Ultrafast Dynamicsmentioning

confidence: 99%

“…(The transient absorption spectra at earlier times are contaminated by the strong coherent artifact.) The experimental setup for 2PE transient absorption spectroscopy was described in detail previously . Briefly, a Spitfire Ace regenerative amplifier system (Spectra Physics), seeded with a Ti:sapphire oscillator (MaiTai SP, Spectra Physics) and pumped by a Nd:YLF laser (Empower 30, Spectra Physics), was used for generating excitation (pump) and probe pulses.…”

Section: Perspective: Vera On Two-photon Initiated Ultrafast Dynamicsmentioning

confidence: 99%

“…The experimental setup for 2PE transient absorption spectroscopy was described in detail previously. 48 Briefly, a Spitfire Ace regenerative amplifier system (Spectra Physics), seeded with a Ti:sapphire oscillator (MaiTai SP, Spectra Physics) and pumped by a Nd:YLF laser (Empower 30, Spectra Physics), was used for generating excitation (pump) and probe pulses. The two-photon excitation wavelengths were achieved through parametric amplification (TOPAS Prime, Light Conversion).…”

Section: Perspective: Vera On Two-photon Initiated Ultrafast Dynamicsmentioning

confidence: 99%

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Understanding Carotenoid Dynamics via the Vibronic Energy Relaxation Approach

et al. 2022

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Carotenoids are an integral part of natural photosynthetic complexes, with tasks ranging from light harvesting to photoprotection. Their underlying energy deactivation network of optically dark and bright excited states is extremely efficient: after excitation of light with up to 2.5 eV of photon energy, the system relaxes back to ground state on a time scale of a few picoseconds. In this article, we summarize how a model based on the vibrational energy relaxation approach (VERA) explains the main characteristics of relaxation dynamics after one-photon excitation with special emphasis on the so-called S* state. Lineshapes after two-photon excitation are beyond the current model of VERA. We outline this future line of research in our article. In terms of experimental method development, we discuss which techniques are needed to better describe energy dissipation effects in carotenoids and within the first solvation shell.

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Section: Perspective: Vera On Two-photon Initiated Ultrafast Dynamicsmentioning

confidence: 99%

Section: Perspective: Vera On Two-photon Initiated Ultrafast Dynamicsmentioning

confidence: 99%

Section: Perspective: Vera On Two-photon Initiated Ultrafast Dynamicsmentioning

confidence: 99%

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Understanding Carotenoid Dynamics via the Vibronic Energy Relaxation Approach

et al. 2022

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“…In the lutein/ Chl a mixture, the kinetics decay with a 14 ps lifetime, proving that the signal indeed is due to the S 1 state of lutein, in agreement with recent 2PE transient absorption data on carotenoids in solution. 25 The 540 nm band in LHCII decays much faster, and to exclude the possibility that the fast component is due to carotenoid−Chl EET, we add data showing the carotenoid S 1 decay after 1PE of LHCII at 490 nm. These data represent the selective 1PE of carotenoid in LHCII, thus the kinetics reflect the decay of the carotenoid S 1 state in LHCII.…”

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confidence: 99%

Transient Absorption of Chlorophylls and Carotenoids after Two-Photon Excitation of LHCII

Šebelík

Kuznetsova

Lokstein

et al. 2021

J. Phys. Chem. Lett.

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Femtosecond transient absorption spectroscopy following two-photon excitation (2PE) is used to determine the contributions of carotenoids and chlorophylls to the 2PE signals in the main plant light-harvesting complex (LHCII). For 2PE, excitation at 1210 and 1300 nm was used, being within the known 2PE profile of LHCII. At both excitation wavelengths, the transient absorption spectra exhibit a shape characteristic of excited chlorophylls with only a minor contribution from carotenoids. We compare the 2PE data measured for LHCII with those obtained from 2PE of a lutein/chlorophyll a mixture in acetone. We estimate that although the 2PE cross section of a single carotenoid in acetone is ∼1.7 times larger than that of a Chl a, due to the 1:3.5 carotenoid/Chl ratio in LHCII, only one-third of the absorbed 2PE photons excite carotenoids in LHCII in the 1200−1300 nm range.

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“…However, the mechanisms of the quenching process are not yet fully investigated and various different models have been proposed that are either based on distinct chlorophyll (Chl)–carotenoid (Car) interactions or on Chl–Chl interactions, only . Here, we study the potential role of energy transfer between optically forbidden states of Cars and the Chls which can be assessed by two‐photon excitation (TPE) . It has been suggested that these forbidden states comprise more than one state – typically termed Car S 1 , Car S x , or Car S* – but for the sake of simplicity, we will name the forbidden states by Car S 1 in the following.…”

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PsbS‐dependent and ‐independent mechanisms regulate carotenoid‐chlorophyll energy coupling in grana thylakoids

et al. 2019

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In higher plants, PsbS is known to play a key role in the regulation of photosynthetic light harvesting. However, the molecular mechanism and role of electronic carotenoid–chlorophyll (Chl) interactions for the downregulation of excess excitation (nonphotochemical energy quenching, NPQ) are still poorly understood. Here, we explored carotenoid → Chl energy transfer in isolated grana thylakoid membranes from mutants either deficient in or overexpressing PsbS. Since it was suggested that PsbS regulates the supramolecular protein network to control NPQ, we varied this network by diluting the grana protein densities. Our results indicate that different electronic quenching mechanisms are operative in grana thylakoids: a PsbS‐dependent mechanism and a membrane protein density‐dependent mechanism that is also operative in the absence of PsbS.

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Time-resolved two-photon spectroscopy of carotenoids

Cited by 3 publications

References 53 publications

Understanding Carotenoid Dynamics via the Vibronic Energy Relaxation Approach

Understanding Carotenoid Dynamics via the Vibronic Energy Relaxation Approach

Transient Absorption of Chlorophylls and Carotenoids after Two-Photon Excitation of LHCII

PsbS‐dependent and ‐independent mechanisms regulate carotenoid‐chlorophyll energy coupling in grana thylakoids

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