Echo-peak shift fails to resolve the liquid–glass phase transition

Lazonder, Kees; Pshenichnikov, Maxim S.; Wiersma, Douwe A.

doi:10.1016/j.cplett.2007.10.069

Cited by 2 publications

(3 citation statements)

References 33 publications

(48 reference statements)

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“…From all IR spectroscopic signatures, the homogeneous dephasing rate responds the most sensitive to the glass transition in proteins. − That is, the homogeneous dephasing rate of proteins in aqueous solution is only weakly temperature dependent below the glass transition and rises steeply above. Also, for a dye dissolved in a glass forming mixture, the same biphasic behavior has been observed . In the present paper, we use 2D-IR spectroscopy to measure the effective homogeneous dephasing rate of a spectrally isolated carbonyl vibration (by isotope labeling), and we will show that its temperature dependence resembles that of the vibrational energy transport efficiency.…”

Section: Introductionsupporting

confidence: 59%

“…Also, for a dye dissolved in a glass forming mixture, the same biphasic behavior has been observed. 28 In the present paper, we use 2D-IR spectroscopy to measure the effective neous dephasing of a spectrally isolated carbonyl vibration (by isotope labeling), and we will show that its temperature dependence resembles that of the vibrational energy transport efficiency.…”

Section: Introductionmentioning

confidence: 93%

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Dynamical Transition in a Small Helical Peptide and Its Implication for Vibrational Energy Transport

et al. 2009

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The two-dimensional infrared spectrum of an octameric helical peptide in chloroform was measured as a function of temperature. Isotope labeling of the carbonyl group of one of the amino acids was used to obtain information for an isolated vibration. The antidiagonal width of the 2D-IR signal, which is a measure of the homogeneous dephasing time T(2), is constant from 220 to 260 K (within experimental error), and increases steeply above. The homogeneous dephasing time of the carbonyl vibration is attributed to the flexibility of the system and/or its immediate surrounding. The system undergoes a dynamical transition at about 270 K, with similarities to the protein dynamical transition. Furthermore, the temperature dependence of the antidiagonal width strongly resembles that of the efficiency of vibrational energy transport along the helix, which has been studied in a recent paper (J. Phys. Chem. B 2008, 112, 15487). The connection between the two processes, structural flexibility and energy transport mechanism, is discussed.

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Section: Introductionsupporting

confidence: 59%

Section: Introductionmentioning

confidence: 93%

Dynamical Transition in a Small Helical Peptide and Its Implication for Vibrational Energy Transport

et al. 2009

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“…As the solution is cooled, this relaxation takes longer due to slower solvent reorganization. In a simple system, ellipticity is a good measure of the system-bath correlation function [6,7]:…”

Section: Discussion and Summarymentioning

confidence: 99%

Two-dimensional electronic spectroscopy signatures of the glass transition

et al. 2010

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Two-dimensional electronic spectroscopy is a sensitive probe of solvation dynamics. Using a pump–probe geometry with a pulse shaper [Optics Express15(2007), 16681-16689;Optics Express16(2008), 17420-17428], we present temperature dependent 2D spectra of laser dyes dissolved in glass-forming solvents. At low waiting times, the system has not yet relaxed, resulting in a spectrum that is elongated along the diagonal. At longer times, the system loses its memory of the initial excitation frequency, and the 2D spectrum rounds out. As the temperature is lowered, the time scale of this relaxation grows, and the elongation persists for longer waiting times. This can be measured in the ratio of the diagonal width to the anti-diagonal width; the behavior of this ratio is representative of the frequency–frequency correlation function [Optics Letters31(2006), 3354–3356]. Near the glass transition temperature, the relaxation behavior changes. Understanding this change is important for interpreting temperature-dependent dynamics of biological systems.

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Echo-peak shift fails to resolve the liquid–glass phase transition

Abstract: Echo-peak shift fails to resolve the liquid-glass phase transition Lazonder, Kees; Pshenichnikov, Maxim S.; Wiersma, Douwe A.

Cited by 2 publications

References 33 publications

Dynamical Transition in a Small Helical Peptide and Its Implication for Vibrational Energy Transport

Dynamical Transition in a Small Helical Peptide and Its Implication for Vibrational Energy Transport

Two-dimensional electronic spectroscopy signatures of the glass transition

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