Generalized magic angle for time-resolved spectroscopy with laser pulses of arbitrary ellipticity

Schott, Sebastian; Steinbacher, Andreas; Buback, Johannes; Nuernberger, Patrick; Brixner, Tobias

doi:10.1088/0953-4075/47/12/124014

Cited by 39 publications

(42 citation statements)

References 55 publications

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“…For the VIS probe continuum, the fundamental beam, rather than the third harmonic, of the amplifier system was focused into the moving CaF 2 . Pump and probe were focused in a nearly collinear geometry at the sample position with magic-angle configuration for the linear polarization directions 47 . After passing through the sample, the probe beam was spectrally resolved via a spectrograph (Acton SP2500i) equipped with a CCD camera (Princeton Instruments Pixis 2 k).…”

Section: Methodsmentioning

confidence: 99%

Excited-state intramolecular proton transfer of 2-acetylindan-1,3-dione studied by ultrafast absorption and fluorescence spectroscopy

Verma

Steinbacher

Schmiedel

et al. 2015

Structural Dynamics

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We employ transient absorption from the deep-UV to the visible region and fluorescence upconversion to investigate the photoinduced excited-state intramolecular proton-transfer dynamics in a biologically relevant drug molecule, 2-acetylindan-1,3-dione. The molecule is a ß-diketone which in the electronic ground state exists as exocyclic enol with an intramolecular H-bond. Upon electronic excitation at 300 nm, the first excited state of the exocyclic enol is initially populated, followed by ultrafast proton transfer (≈160 fs) to form the vibrationally hot endocyclic enol. Subsequently, solvent-induced vibrational relaxation takes place (≈10 ps) followed by decay (≈390 ps) to the corresponding ground state.

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Section: Methodsmentioning

confidence: 99%

Excited-state intramolecular proton transfer of 2-acetylindan-1,3-dione studied by ultrafast absorption and fluorescence spectroscopy

Verma

Steinbacher

Schmiedel

et al. 2015

Structural Dynamics

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“…With linear probe polarization in a TA experiment, the polarization angle with a linear pump can be set to eliminate this effect in the recorded spectral kinetics. This socalled magic angle condition is more complex for TRCD as the circular probe polarization breaks the cylindrical symmetry of a linear probe [23] and should take quadrupolar light-molecule interactions into account [24,25]. Furthermore, any residual birefringence in the setup, combined with any remaining polarization sensitivity of the dispersive spectrometer after the scrambling of the probe polarization, will translate the linear dichroism of the pump-induced sample anisotropy into an artificial TRCD signal [7,26].…”

Section: Methodsmentioning

confidence: 99%

Ultrafast broadband circular dichroism in the deep ultraviolet

Oppermann¹,

Bauer²,

Rossi³

et al. 2019

Optica

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The measurement of chirality and its temporal evolution are crucial for the understanding of a large range of biological functions and chemical reactions. Steady-state circular dichroism (CD) is a standard analytical tool for measuring chirality in chemistry and biology. Nevertheless, its push into the ultrafast time domain and in the deep-ultraviolet has remained a challenge, with only some isolated reports of subnanosecond CD. Here, we present a broadband time-resolved CD spectrometer in the deep ultraviolet (UV) spectral range with femtosecond time resolution. The setup employs a photoelastic modulator to achieve shot-to-shot polarization switching of a 20 kHz pulse train of broadband femtosecond deep-UV pulses (250-370 nm). The resulting sequence of alternating left-and right-circularly polarized probe pulses is employed in a pump-probe scheme with shot-to-shot dispersive detection and thus allows for the acquisition of broadband CD spectra of ground-and excited-state species. Through polarization scrambling of the probe pulses prior to detection, artifact-free static and transient CD spectra of enantiopure Rubpy 3 2 are successfully recorded with a sensitivity of <2 × 10 −5 OD (≈0.7 mdeg). Due to its broadband deep-UV detection with unprecedented sensitivity, the measurement of ultrafast chirality changes in biological systems with amino-acid residues and peptides and of DNA oligomers is now feasible.

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“…All time-resolved measurements were performed with polarizations set to the magic angle (54.78)c ondition [43,44] to avoid anisotropy contributions. For the analysis of the TCSPC and upconversion data, af itting routine was implemented in MATLAB script, allowing fits of the data with am ultiexponential parallel model and taking into accountaconvolution with the instrument response.…”

Section: Methodsmentioning

confidence: 99%

Ultrafast Dynamics of a Fluorescent Tetrazolium Compound in Solution

et al. 2017

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Tetrazolium salts are exploited in various fields of research by virtue of their low reduction potentials. Increasingly, associated applications also attend to the photochemical and luminescence properties of these systems. Here, we investigate the photoinduced dynamics of phenyl-benzo[c]tetrazolo-cinnolinium chloride (PTC), one of the very few known fluorescent tetrazolium compounds, by using time-correlated single-photon counting, femtosecond fluorescence upconversion, and ultrafast transient absorption spectroscopy. PTC is generated photochemically by ultraviolet illumination of 2,3,5-triphenyl-tetrazolium chloride (TTC) in various alcohols. Time-resolved fluorescence measurements on PTC with different excitation wavelengths disclose biphasic solvation and vibrational relaxation dynamics. Depending on the solvent, the emission behavior of PTC is characterized by quantum yields on the order of several tens of percent and corresponding excited-state lifetimes of several hundreds of picoseconds. The radiative rate is basically constant for the studied alcohols, whereas the rate of the competing non-radiative process is sensitive to the solvent polarity. Hence, we discuss the possible involvement of intermediate radicals and further presumptive reaction pathways pursued after photoexcitation of PTC.

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Generalized magic angle for time-resolved spectroscopy with laser pulses of arbitrary ellipticity

Cited by 39 publications

References 55 publications

Excited-state intramolecular proton transfer of 2-acetylindan-1,3-dione studied by ultrafast absorption and fluorescence spectroscopy

Excited-state intramolecular proton transfer of 2-acetylindan-1,3-dione studied by ultrafast absorption and fluorescence spectroscopy

Ultrafast broadband circular dichroism in the deep ultraviolet

Ultrafast Dynamics of a Fluorescent Tetrazolium Compound in Solution

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