Collisional Deactivation of Vibrationally Highly Excited Azulene in Supercritical Fluids

D. Schwarzer, J. Troe, M. Votsmeier, M. Zerezke
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引用次数: 71

Abstract

The collisional deactivation of vibrationally highly excited azulene was studied from gas into compressed liquid phase by pump-and-probe picosecond laser spectroscopy. Collisional deactivation rates were compared with solvatochromic shifts Δν of the azulene S3←S0 absorption band under identical conditions. Employing supercritical fluids at pressures between 0.03 and 4000 bars and temperatures between 298 and 640 K, measurements covering the complete gas–liquid transition were performed. For the energy transfer experiments, azulene with an energy of ∼20000 cm−1 was generated by laser excitation into the S1- and internal conversion to the S0*-ground state. The subsequent loss of vibrational energy was monitored by following the transient absorption at the red wing of the S3←S0 absorption band near 290 nm. Transient signals were converted into energy-time profiles using hot band absorption coefficients from shock wave experiments for calibration and accounting for solvent shifts of the spectra. Under all con...
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超临界流体中振动高激发Azulene的碰撞失活
采用泵探皮秒激光光谱技术研究了振动高激发azulene从气体到压缩液相的碰撞失活过程。在相同条件下,比较了碰撞失活率和azulene S3←S0吸收带的溶剂变色位移Δν。在0.03 ~ 4000bar的压力和298 ~ 640k的温度下,采用超临界流体进行了完整的气液转变测量。在能量转移实验中,通过激光激发到S1-和内部转换到S0*-基态,产生能量为~ 20000 cm−1的azulene。随后的振动能量损失通过跟踪S3←S0吸收带红翼290 nm附近的瞬态吸收来监测。利用激波实验的热带吸收系数将瞬态信号转换为能量-时间谱,用于校准和计算光谱的溶剂位移。无论如何……
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