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Science Advances

Coherent control of collective nuclear quantum states via transient magnons

Lars Bocklage, Jakob Gollwitzer, C. Strohm, Christian F. Adolff, Kai Schlage, I. Sergueev, O. Leupold, Hans‐Christian Wille, Guido Meier, Ralf Röhlsberger

Published Jan 29, 2021• 19 citations
Publisher

Abstract

Ultrafast and precise control of quantum systems at x-ray energies involves photons with oscillation periods below 1 as. Coherent dynamic control of quantum systems at these energies is one of the major challenges in hard x-ray quantum optics. Here, we demonstrate that the phase of a quantum system embedded in a solid can be coherently controlled via a quasi-particle with subattosecond accuracy. In particular, we tune the quantum phase of a collectively excited nuclear state via transient magnons with a precision of 1 zs and a timing stability below 50 ys. These small temporal shifts are monitored interferometrically via quantum beats between different hyperfine-split levels. The experiment demonstrates zeptosecond interferometry and shows that transient quasi-particles enable accurate control of quantum systems embedded in condensed matter environments.

DOI
10.1126/sciadv.abc3991

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Ultrafast and precise control of quantum systems at x-ray energies involves photons with oscillation periods below 1 as. Coherent dynamic control of quantum systems at these energies is one of the major challenges in hard x-ray quantum optics. Here, we demonstrate that the phase of a quantum system embedded in a solid can be coherently controlled via a quasi-particle with subattosecond accuracy. In particular, we tune the quantum phase of a collectively excited nuclear state via transient magnons with a precision of 1 zs and a timing stability below 50 ys. These small temporal shifts are monitored interferometrically via quantum beats between different hyperfine-split levels. The experiment demonstrates zeptosecond interferometry and shows that transient quasi-particles enable accurate control of quantum systems embedded in condensed matter environments.
Advancements in x-ray sources extend the scope of light-matter interactions into the x-ray-nuclear regime. Precise temporal control of quantum phases provides fundamental insights into quantum systems and serves as a cornerstone for numerous quantum technologies. Nevertheless, achieving phase control of quantum systems with high temporal and spatial resolution remains a substantial challenge in the realm of hard x-ray quantum optics due to the ultrashort oscillation periods of photons. In this study, we propose to manipulate the magnetic properties of a thin 57Fe^{57}\text{Fe}57Fe film using near-infrared (NIR) pulses characterized by a high repetition rate. By calculating the evolution of quantum beats, we can theoretically extract the phase information of the nuclear response. Coherence within the nuclear ensemble is preserved throughout the entire process. This control scheme achieves quantum shifts with zeptosecond precision and modulates the spectral line shape within the frequency domain. Our proposal introduces a high-resolution method for rapidly manipulating nuclear states using optical laser pulses.
The direct interaction between nuclei and strong electromagnetic fields generated by novel coherent x-ray light sources such as the x-ray free electron laser is studied. We investigate the case of various stable or long-lived isotopes with energetically low-lying excited states, where the laser drives the nuclear transition from the ground to the first excited state. We therefore consider the nucleus as a two-level system including the corresponding hyperfine levels in our theoretical description. The performance of present and upcoming x-ray free electron laser facilities in coherently controlling the nuclear excited state population is analyzed for setups involving both solid state as well as accelerated nuclear targets to bridge the gap between photon and transition frequency. Current and predicted laser parameters are applied to calculate excited state populations and signal photon rates of nuclei after a radiation pulse, finding significant improvements compared to former calculations. Furthermore, we determine the parameters necessary to transfer substantial amounts of the nuclear ground state population to the excited state, and therefore to bring nuclear Rabi-oscillation within reach. Additionally, we take into account for the first time collective effects that take place in solid state targets and show that they may provide a significant effect in broadening natural linewidths of nuclear levels depending on the experimental setup. Our findings support the case of nuclear quantum optics for XFEL applications. Therefore, one hopes that eventually coherent control of nuclear transitions can be successfully applied in a number of areas in nuclear physics including preparation, control and detection methods.
Abstract We demonstrate the generation of a train of attosecond XUV pulses that are in a superposition of wavefront states. Such superposition yields a high precision, self-referencing, common path XUV interferometer setup to produce pairs of spatially separated and independently controllable XUV pulses that are locked in phase and time with a temporal jitter of 3.5 zs (zs = zeptoseconds = 10 − 21 s ). In our approach, we can independently control the relative phase/delay of the two optical beams with a resolution of 52 zs. Since the jitter is on the order of the Compton time scale τ C = λ C / m e c 2 , we explore the level of correlation between the non-local photons by comparing different spatial mode superpositions. Further, thanks to the stability of the interferometer we can retrieve the interference pattern through photon counting. Through post-selection of different particle events we can analyze one, two or more photon events. We argue that this zeptosecond level of temporal precision will open the door for new dynamical quantum electrodynamics (QED) tests at lower intensities while photon counting experiments can also have an impact on the emerging field of quantum light in strong fields. We also discuss the potential impact on other areas, such as time-dependent QED, imaging, measurements of non-locality, and molecular quantum tomography.
Modern x-ray light sources promise access to structure and dynamics of matter in largely unexplored spectral regions. However, the desired information is encoded in the light intensity and phase, whereas detectors register only the intensity. This phase problem is ubiquitous in crystallography and imaging and impedes the exploration of quantum effects at x-ray energies. Here, we demonstrate phase-sensitive measurements characterizing the quantum state of a nuclear two-level system at hard x-ray energies. The nuclei are initially prepared in a superposition state. Subsequently, the relative phase of this superposition is interferometrically reconstructed from the emitted x rays. Our results form a first step towards x-ray quantum state tomography and provide new avenues for structure determination and precision metrology via x-ray Fano interference.
The fastest possible collective response of a quantum many-body system is related to its excitations at the highest possible energy. In condensed matter systems, the time scale for such "ultrafast" processes is typically set by the Fermi energy. Taking advantage of fast and precise control of interactions between ultracold atoms, we observed nonequilibrium dynamics of impurities coupled to an atomic Fermi sea. Our interferometric measurements track the nonperturbative quantum evolution of a fermionic many-body system, revealing in real time the formation dynamics of quasi-particles and the quantum interference between attractive and repulsive states throughout the full depth of the Fermi sea. Ultrafast time-domain methods applied to strongly interacting quantum gases enable the study of the dynamics of quantum matter under extreme nonequilibrium conditions.
Abstract Control of interference between wave packets is one of the basic concepts in coherent control that enables quantum manipulation of populations and reaction pathways in matter. We have recently shown a new method to achieve coherent control in the extreme ultraviolet and attosecond regime using synchrotron radiation. This method is based on the use of longitudinal coherence of light wave packets that are naturally included in the undulator radiation. For quantum manipulation of atomic systems, wave packet interference is precisely controlled by tuning the time delay between the light wave packets. Here we show that the quantum phase controlled by the time delay can be monitored as an initial phase of the quantum beat oscillation in fluorescence decay.