Coherent X-ray−optical control of nuclear excitons

Kilian P. Heeg, Andreas Kaldun, Cornelius Strohm, Christian Ott, Rajagopalan Subramanian, Dominik Lentrodt, Johann Haber, Hans-Christian Wille, Stephan Goerttler, Rudolf Rüffer, Christoph H. Keitel, Ralf Röhlsberger, Thomas Pfeifer and Jörg Evers ()
Additional contact information
Kilian P. Heeg: Max-Planck-Institut für Kernphysik
Andreas Kaldun: Max-Planck-Institut für Kernphysik
Cornelius Strohm: Deutsches Elektronen-Synchrotron DESY
Christian Ott: Max-Planck-Institut für Kernphysik
Rajagopalan Subramanian: Max-Planck-Institut für Kernphysik
Dominik Lentrodt: Max-Planck-Institut für Kernphysik
Johann Haber: Deutsches Elektronen-Synchrotron DESY
Hans-Christian Wille: Deutsches Elektronen-Synchrotron DESY
Stephan Goerttler: Max-Planck-Institut für Kernphysik
Rudolf Rüffer: The European Synchrotron Radiation Facility (ESRF)
Christoph H. Keitel: Max-Planck-Institut für Kernphysik
Ralf Röhlsberger: Deutsches Elektronen-Synchrotron DESY
Thomas Pfeifer: Max-Planck-Institut für Kernphysik
Jörg Evers: Max-Planck-Institut für Kernphysik

Nature, 2021, vol. 590, issue 7846, 401-404

Abstract: Abstract Coherent control of quantum dynamics is key to a multitude of fundamental studies and applications1. In the visible or longer-wavelength domains, near-resonant light fields have become the primary tool with which to control electron dynamics2. Recently, coherent control in the extreme-ultraviolet range was demonstrated3, with a few-attosecond temporal resolution of the phase control. At hard-X-ray energies (above 5–10 kiloelectronvolts), Mössbauer nuclei feature narrow nuclear resonances due to their recoilless absorption and emission of light, and spectroscopy of these resonances is widely used to study the magnetic, structural and dynamical properties of matter4,5. It has been shown that the power and scope of Mössbauer spectroscopy can be greatly improved using various control techniques6–16. However, coherent control of atomic nuclei using suitably shaped near-resonant X-ray fields remains an open challenge. Here we demonstrate such control, and use the tunable phase between two X-ray pulses to switch the nuclear exciton dynamics between coherent enhanced excitation and coherent enhanced emission. We present a method of shaping single pulses delivered by state-of-the-art X-ray facilities into tunable double pulses, and demonstrate a temporal stability of the phase control on the few-zeptosecond timescale. Our results unlock coherent optical control for nuclei, and pave the way for nuclear Ramsey spectroscopy17 and spin-echo-like techniques, which should not only advance nuclear quantum optics18, but also help to realize X-ray clocks and frequency standards19. In the long term, we envision time-resolved studies of nuclear out-of-equilibrium dynamics, which is a long-standing challenge in Mössbauer science20.

Date: 2021
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DOI: 10.1038/s41586-021-03276-x

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