Ultrafast UV spectroscopy: from a local to a global view of dynamical processes in macromolecules

Cannizzo, Andrea

doi:10.1039/c2cp40567a

Cited by 30 publications

(27 citation statements)

References 175 publications

(261 reference statements)

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“…The benefits of the extension of 2D spectroscopy into the UV have been envisioned in recent perspective papers [15,20,21] as it allows one to address the absorption and ultrafast dynamics of aromatic amino acids in proteins and DNA bases and thus the investigation of the energy and charge transfer flow in these systems. The potential of this method is however even larger, as one can decipher spectrally overlapping bands in chromophore complexes and even in single chromophores.…”

Section: Introductionmentioning

confidence: 99%

Two-dimensional Fourier transform spectroscopy in the ultraviolet with sub-20 fs pump pulses and 250–720 nm supercontinuum probe

et al. 2013

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Experimental realizations of two-dimensional (2D) electronic spectroscopy in the ultraviolet (UV) must so far contend with a limited bandwidth in both the excitation and particularly the probe frequency. The pump bandwidth is at best 1500 cm −1 (full width at half maximum) at a fixed wavelength of 267 nm or 400 cm −1 for tunable pulses. The use of a replica of the pump pulse as a probe limits the observation of photochemical processes to the excitation region and makes the disentanglement of overlapping signal contributions difficult. We show that 2D Fourier transform spectroscopy can be conducted in a shaper-assisted collinear setup comprising fully tunable UV pulse pairs and supercontinuum probe spanning 250-720 nm. The pump pulses are broadened up to a useable spectral coverage of 2000 cm −1 (25 nm at 316 nm) by self-phase modulation in bulk CaF 2 and compressed to 18 fs. By referencing the white light probe and eliminating pump stray light contributions, high signal-to-noise ratios even for weak probe intensities are achieved. Data acquisition times as short as 4 min for a selected population time allow the rapid recording of 2D spectra for photolabile biological samples even with the

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Section: Introductionmentioning

confidence: 99%

Two-dimensional Fourier transform spectroscopy in the ultraviolet with sub-20 fs pump pulses and 250–720 nm supercontinuum probe

et al. 2013

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“…A variety of approaches have now been used to carry out 2D spectroscopies at wavelengths greater than 260 nm with data quality that is comparable to the best measurements in the visible wavelength range [43][44][45][46][47][48][49]. Biologically interesting applications to DNA and proteins are on the horizon [44,46,47,49].…”

Section: Discussionmentioning

confidence: 98%

“…Solutions to challenges including high-precision control over pulse delays and interferometric phase stability enabled subsequent applications in the visible wavelength range [40][41][42]. Further extension of 2D spectroscopy to the deep ultraviolet, hereafter termed 2DUV, is primarily motivated by biological systems whose lowest frequency resonances are found in this spectral range (200-300 nm) [43][44][45][46][47][48][49]. Such experiments must contend with several problems including the attainment of adequate laser bandwidth, interferometric phase stability, and the suppression of undesired nonlinearities in solutions (e.g., photoionization of solute and solvent).…”

Section: Introductionmentioning

confidence: 99%

Uncovering molecular relaxation processes with nonlinear spectroscopies in the deep UV

et al. 2013

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a b s t r a c tNonlinear laser spectroscopies in the deep UV spectral range are motivated by studies of biological systems and elementary processes in small molecules. This perspective article discusses recent technical advances in this area with a particular emphasis on diffractive optic based approaches to four-wave mixing spectroscopies. Applications to two classes of systems illustrate present experimental capabilities. First, experiments on DNA components at cryogenic temperatures are used to uncover features of excited state potential energy surfaces and vibrational cooling mechanisms. Second, sub-200 fs internal conversion processes and coherent wavepacket motions are investigated in cyclohexadiene and a-terpinene.Finally, we propose new experimental directions that combine methods for producing few-cycle UV laser pulses in noble gases with incoherent detection methods (e.g., photoionization) in experiments with time resolution near a singlefemtosecond. These measurements are motivated by knowledge of extremely fast non-adiabatic dynamics and the resolution of electronic wavepacket motions in molecules.

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“…A more detailed discussion about the ongoing developments in this area are found in Refs. [48] and [49]. 2D UV transient absorption spectroscopy has recently been implemented with very broad continua (>60 nm) [50] and used to investigate electron and energy transfer involving Trp in myoglobins [51].…”

Section: Introductionmentioning

confidence: 99%

Ultraviolet transient absorption, transient grating and photon echo studies of aqueous tryptophan

et al. 2013

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a b s t r a c tWe compare UV transient grating (TG) experiments of aqueous tryptophan with transient absorption (TA) and fluorescence up-conversion measurements. The TG and TA signals show a bi-exponential rise with sub-ps and ps time constants, which are consistent with the fluorescence studies. Using experimental data, we provide an equation for the homodyne-detected TG signal, taking into account the sub-100 fs internal conversion of tryptophan after excitation. In addition, we measure a sub-100 fs homogeneous electronic dephasing time for tryptophan in water by the photon echo (PE) technique. These measurements provide a consistent picture of excited state dynamics of aqueous tryptophan that may serve as a basis for coherent 2D-UV spectroscopy of biosystems.

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Ultrafast UV spectroscopy: from a local to a global view of dynamical processes in macromolecules

Cited by 30 publications

References 175 publications

Two-dimensional Fourier transform spectroscopy in the ultraviolet with sub-20 fs pump pulses and 250–720 nm supercontinuum probe

Two-dimensional Fourier transform spectroscopy in the ultraviolet with sub-20 fs pump pulses and 250–720 nm supercontinuum probe

Uncovering molecular relaxation processes with nonlinear spectroscopies in the deep UV

Ultraviolet transient absorption, transient grating and photon echo studies of aqueous tryptophan

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