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Experimental control of quantum-mechanical entanglement in an attosecond pump-probe experiment

Entanglement is one of the most intriguing aspects of quantum mechanics and lies at the heart of the ongoing Second Quantum Revolution, where it is a resource that is used in quantum key distribution, quantum computing and quantum teleportation. We report experiments demonstrating the crucial role that entanglement plays in pump-probe experiments involving ionization, which are a hallmark of the novel research field of attosecond science. We demonstrate that the degree of entanglement in a bipartite ion plus photoelectron system, and, as a consequence, the degree of vibrational coherence in the ion, can be controlled by tailoring the spectral properties of the attosecond extreme ultra-violet laser pulses that are used to create them.