Appearance of coherent artifact signals in femtosecond
transient absorption spectroscopy in dependence on detector design

Dietzek, Benjamin; Pascher, Torbjörn; Sundström, Villy; Yartsev, Arkady

doi:10.1002/lapl.200610070

Cited by 87 publications

(71 citation statements)

References 16 publications

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“…The pulse-overlap region was ignored during the fitting process to make sure that no contributions from coherent artefacts affect the data analysis. [42,51] The setup used to record the long-time window differential absorption data is described in detail by De et al [52] Steady-state experiments were performed in solutions with aerated acetonitrile at room temperature (22 8C). The steady-state absorption spectra were recorded with a Jasco V-670 spectrophotometer.…”

Section: Methodsmentioning

confidence: 99%

Tuning of Photocatalytic Hydrogen Production and Photoinduced Intramolecular Electron Transfer Rates by Regioselective Bridging Ligand Substitution

et al. 2011

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Artificial photosynthesis based on supramolecular photocatalysts offers the unique possibility to study the molecular processes underlying catalytic conversion of photons into chemical fuels in great detail and to tune the properties of the photocatalyst by alterations of the molecular framework. Herein we focus on both possibilities in studying the photocatalytic reduction of protons by derivatives of the well-known photocatalyst [(tbbpy)(2)Ru(tpphz)PdCl(2)](PF(6))(2) [4,4'-di-tert-butyl-2,2'-bipyridine (tbbpy), tetrapyrido[3,2-a:2',3'-c:3'',2''-h:2''',3'''-j]phenazine (tpphz)]. We report on a modified photocatalyst where the crucial bridging ligand tpphz is substituted by bromine and investigate the effect of the structural variation on the catalytic properties of the complex and its ultrafast intramolecular charge transfer behavior. It is found that structural modification stabilizes the phenanthroline-centered metal-to-ligand charge-transfer state on the tpphz moiety, thereby reducing the electron transfer gradient across the entire electron-relaying bridging ligand and at the same time accelerating nanosecond ground-state recovery. The same structural modifications cause an overall reduction of the catalytic activity of the complex. Thus, the results highlight the potential of small structural variations in the molecular framework of supramolecular catalysts in understanding the photoinduced charge-transfer processes and optimizing their catalytic performance.

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Section: Methodsmentioning

confidence: 99%

Tuning of Photocatalytic Hydrogen Production and Photoinduced Intramolecular Electron Transfer Rates by Regioselective Bridging Ligand Substitution

et al. 2011

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“…If the injection products absorb at the selected wavelength, the electron injection would be underestimated. With the 100 fs temporal resolution of the used setup and due to the contribution from coherent artifacts, [47,48] charge-injection processes occurring on a faster timescale (e.g. electron injection from 1 MLCT states) cannot be addressed in the present experiment.…”

Section: Excited-state Dynamics Of Ru1-sensitized Tio 2 Filmsmentioning

confidence: 99%

Photophysics of a Ruthenium 4H‐Imidazole Panchromatic Dye in Interaction with Titanium Dioxide

et al. 2015

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The photophysics of bis(4,4'-di-tert-butyl-2,2'-bipyridine-κ(2)N,N')[2-(4-carboxyphenyl)-4,5-bis(p-tolylimino-κN)imidazolato]ruthenium(II) hexafluorophosphate is investigated, both in solution and attached to a nanocrystalline TiO2 film. The studied substitution pattern of the 4H-imidazole ligand is observed to block a photoinduced structural reorganization pathway within the 4H-imidazole ligand that has been previously investigated. Protonation at the 4H-imidazole ring decreases the excited-state lifetime in solution. When the unprotonated dye is anchored to TiO2, photoinduced electron injection occurs from thermally nonrelaxed triplet metal-to-ligand charge transfer ((3)MLCT) states with a characteristic time constant of 0.5 ps and an injection efficiency of roughly 25%. Electron injection from the subsequently populated thermalized (3)MLCT state of the dye does not take place. The energy of this state seems to be lower than the conduction band edge of TiO2.

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“…Thereby most of the laser fluctuations in both probe channels can be removed and hence high-quality transient-anisotropy data can be obtained. Spectrally integrated detection of the probe light suppresses the observation of coherent artefact signals [22] and allows unravelling the photoinduced dynamics at very short time-scales. The time-dependent anisotropy is calculated from both polarization channels according to (C) Steady-state absorption spectrum (black solid line) and differential absorption spectra taken 1 and 100 ps after excitation at 625 nm (black dashed-dotted line and grey dashed-dotted line).…”

Section: Ultrafast Spectroscopymentioning

confidence: 99%

Dynamics of charge separation in the excited-state chemistry of protochlorophyllide

Dietzek¹,

Tschierlei²,

Hanf³

et al. 2010

Chemical Physics Letters

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Appearance of coherent artifact signals in femtosecond transient absorption spectroscopy in dependence on detector design

Cited by 87 publications

References 16 publications

Tuning of Photocatalytic Hydrogen Production and Photoinduced Intramolecular Electron Transfer Rates by Regioselective Bridging Ligand Substitution

Tuning of Photocatalytic Hydrogen Production and Photoinduced Intramolecular Electron Transfer Rates by Regioselective Bridging Ligand Substitution

Photophysics of a Ruthenium 4H‐Imidazole Panchromatic Dye in Interaction with Titanium Dioxide

Dynamics of charge separation in the excited-state chemistry of protochlorophyllide

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