Exciton energy transfer reveals spectral signatures of excited states in clusters
Exciton energy transfer reveals spectral signatures of excited states in clusters
复制标题
激子能量转移揭示了团簇中激发态的光谱特征
DOI：
10.1039/d0cp02042g
复制
发表时间：
2020
影响因子：
3.3
通讯作者：
Ahmed, Musahid
中科院分区：
文献类型：
--
作者：
Lu, Wenchao;Metz, Ricardo B.;Troy, Tyler P.;Kostko, Oleg;Ahmed, Musahid
利用同步辐射光电离质谱和电子结构计算研究了氩-乙炔团簇在超声膨胀过程中的电子激发和伴随的能量转移导致的Penning电离.氩-乙炔混合团簇光电离效率的光谱特征揭示了氩原子2 P1/2和2 P3/2激发态的蓝移。对这一特征的分析表明，氩团簇的激发态将能量传递给乙炔，导致其电离并连续蒸发氩。理论计算的Arn（n = 2-6）团簇光谱与实验观测非常吻合，并提供了对团簇结构和电离动力学的深入了解。氩-乙炔和氩-水团簇之间的比较表明，氩更好地溶剂化水，允许更高阶的激子和里德堡态被填充。这些结果解释了各自的结合能和结构的理论计算。
Electronic excitation and concomitant energy transfer leading to Penning ionization in argon–acetylene clusters generated in a supersonic expansion are investigated with synchrotron-based photoionization mass spectrometry and electronic structure calculations. Spectral features in the photoionization efficiency of the mixed argon–acetylene clusters reveal a blue shift from the 2P1/2 and 2P3/2 excited states of atomic argon. Analysis of this feature suggests that excited states of argon clusters transfer energy to acetylene, resulting in its ionization and successive evaporation of argon. Theoretically calculated Arn (n = 2–6) cluster spectra are in excellent agreement with experimental observations, and provide insight into the structure and ionization dynamics of the clusters. A comparison between argon–acetylene and argon–water clusters reveals that argon solvates water better, allowing for higher-order excitons and Rydberg states to be populated. These results are explained by theoretical calculations of respective binding energies and structures.