Relaxation Dynamics of Tryptophan in Water: A UV Fluorescence Up-Conversion and Molecular Dynamics Study

被引：33

作者：

Braem, O. ^{[1
]}

Ajdarzadeh Oskouei, A. ^{[1
]}

Tortschanoff, A. ^{[1
]}

van Mourik, F. ^{[1
]}

Madrid, M. ^{[2
]}

Echave, J. ^{[2
,3
]}

Cannizzo, A. ^{[1
]}

Chergui, M. ^{[1
]}

机构：

[1] Ecole Polytech Fed Lausanne, ISIC, Lab Spect Ultrarapide, SB, CH-1015 Lausanne, Switzerland

[2] Univ Nacl La Plata, Inst Nacl Invest Fisicoquim Teor & Aplicadas, RA-1900 La Plata, Argentina

[3] Univ Nacl San Martin, Escuela Ciencia & Tecnol, RA-1650 Buenos Aires, DF, Argentina

来源：

JOURNAL OF PHYSICAL CHEMISTRY A | 2010年 / 114卷 / 34期

基金：

瑞士国家科学基金会;

关键词：

RESONANCE ENERGY-TRANSFER; EXCITED-STATE DYNAMICS; PARTICLE MESH EWALD; ECHO PEAK SHIFT; HYDRATION DYNAMICS; SOLVATION DYNAMICS; FEMTOSECOND RESOLUTION; HYBRID SIMULATIONS; BIOLOGICAL WATER; PROTEIN SURFACE;

D O I：

10.1021/jp101778u

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

We report on an ultrafast experimental and simulations study of the early relaxation events of photoexcited tryptophan in water. Experimentally, we used fluorescence up-conversion in both polychromatic and single wavelength detection modes in the 300-480 nm range with polarization dependence. We report on the time evolution of the Stokes shift, bandwidth, and anisotropy from tens of femtoseconds to picoseconds. These observables contain signatures of the simultaneous occurrence of intramolecular and solvent-molecule interactions, which we disentangle with the help of nonequilibrium molecular dynamics simulations. We also observe a breakdown of the linear response approximation to describe our results.

引用

页码：9034 / 9042

页数：9

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