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Imagen de intersección cónica CF₃I y dinámica de fotodisociación con difracción de electrones ultrarrápida

Jie Yang^1,2, Xiaolei Zhu^2,3, Thomas J A Wolf²

¹SLAC National Accelerator Laboratory, Menlo Park, CA, USA. jieyang@slac.stanford.edu todd.martinez@stanford.edu martin.centurion@unl.edu wangxj@slac.stanford.edu.

Science (New York, N.Y.)

|July 7, 2018

Resumen

La difracción de electrones ultrarrápida tomó imágenes de paquetes de ondas moleculares en intersecciones cónicas. Este estudio observó la bifurcación de paquetes de ondas nucleares y los modos de vibración en CF3I, validando los cálculos teóricos.

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Área de la Ciencia:

Química Física
Dinámica molecular
Química Cuántica

Sus antecedentes:

Las intersecciones cónicas son cruciales para la dinámica molecular de estado excitado y los procesos no adiabáticos.
La imagen directa de las trayectorias de paquetes de ondas a través de intersecciones cónicas ha sido un desafío debido a las limitaciones en la resolución espacial.

Objetivo del estudio:

Caracterizar experimentalmente los canales de excitación de un fotón y dos fotones en moléculas aisladas de CF3I.
Para obtener una imagen directa de la dinámica de paquetes de ondas nucleares a través de intersecciones cónicas.

Principales métodos:

Se ha utilizado la difracción de electrones en fase gaseosa ultrarrápida (UF-GED).
Se estudiaron simultáneamente las vías de excitación de un fotón y dos fotones.
Aplicación de cálculos dinámicos no adiabáticos para la validación.

Principales resultados:

Trajectorias mapeadas en el espacio real de un paquete de onda nuclear coherente en el canal de dos fotones.
Observación de la bifurcación de paquetes de ondas en dos superficies de energía potencial en una intersección cónica.
Resolución de la excitación de los modos de vibración paraguas y respiración en el fragmento CF3 en múltiples dimensiones en el canal de un fotón.

Conclusiones:

Demostró la capacidad de UF-GED para sondear dinámicas moleculares ultrarrápidas en intersecciones cónicas.
Proporcionó evidencia experimental directa del comportamiento de los paquetes de onda en las intersecciones cónicas.
Modelos teóricos validados para procesos moleculares no adiabáticos.