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Interatomic processes play a crucial role in weakly bound complexes exposed to ionizing radiation; therefore, gaining a thorough understanding of their efficiency is of fundamental importance. Here, we directly measure the timescale of interatomic Coulombic decay (ICD) in resonantly excited helium nanodroplets using a high-resolution, tunable, extreme ultraviolet free-electron laser. Over an extensive range of droplet sizes and laser intensities, we discover the decay to be surprisingly fast, with decay times as short as 400 fs, nearly independent of the density of the excited states. Using a combination of timedependent density functional theory and ab initio quantum chemistry calculations, we elucidate the mechanisms of this ultrafast decay process, where pairs of excited helium atoms in one droplet strongly attract each other and form merging void bubbles, which drastically accelerates ICD.
Jian Wang, Matthias Finger, Qian Wang, Yiming Li, Matthias Wolf, Varun Sharma, Yi Zhang, Konstantin Androsov, Jan Steggemann, Xin Chen, Rakesh Chawla, Matteo Galli, Anna Mascellani, João Miguel das Neves Duarte, Tagir Aushev, Tian Cheng, Yixing Chen, Werner Lustermann, Andromachi Tsirou, Alexis Kalogeropoulos, Andrea Rizzi, Ioannis Papadopoulos, Paolo Ronchese, Hua Zhang, Siyuan Wang, Tao Huang, David Vannerom, Michele Bianco, Sebastiana Gianì, Sun Hee Kim, Kun Shi, Abhisek Datta, Federica Legger, Gabriele Grosso, Ji Hyun Kim, Donghyun Kim, Zheng Wang, Sanjeev Kumar, Wei Li, Yong Yang, Geng Chen, Ajay Kumar, Ashish Sharma, Georgios Anagnostou, Joao Varela, Csaba Hajdu, Muhammad Ahmad, Ioannis Evangelou, Milos Dordevic, Meng Xiao, Sourav Sen, Xiao Wang, Kai Yi, Jing Li, Rajat Gupta, Zhen Liu, Hui Wang, Seungkyu Ha, Long Wang, Pratyush Das, Anton Petrov, Xin Sun, Valérie Scheurer, Giovanni Mocellin, Muhammad Ansar Iqbal, Lukas Layer
Alessandro Mapelli, Radoslav Marchevski, Alina Kleimenova
Fabrizio Carbone, Simone Gargiulo