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Entanglement is one of the most intriguing aspects of quantum mechanics andlies at the heart of the ongoing Second Quantum Revolution, where it is aresource that is used in quantum key distribution, quantum computing andquantum teleportation. We report experiments demonstrating the crucial rolethat entanglement plays in pump-probe experiments involving ionization, whichare a hallmark of the novel research field of attosecond science. Wedemonstrate that the degree of entanglement in a bipartite ion plusphotoelectron system, and, as a consequence, the degree of vibrationalcoherence in the ion, can be controlled by tailoring the spectral properties ofthe attosecond extreme ultra-violet laser pulses that are used to create them.

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