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Journal of Physics Conference Series

Coherent control of atoms in the extreme ultraviolet and attosecond regime by synchrotron radiation

T. Kaneyasu, Y. Hikosaka, Masaki Fujimoto, Hiroshi Iwayama, Masahiro Katoh

Published Dec 1, 2022• 0 citations
Publisher

Abstract

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.

DOI
10.1088/1742-6596/2380/1/012115

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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.
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Coherent control is a technique to manipulate the amplitudes and phases of wave functions by exploiting the coherent property of light. It is of great importance for the development of quantum technologies including quantum information processing and chemical reaction control as well as for addressing fundamental problems in quantum mechanics such as the quantum–classical boundary. In this chapter, we describe the development and applications of coherent control based on wave-packet interferometry with attosecond precision, which has been made possible by tuning the delay between two laser pulses on the attosecond time scale. This technique has been applied to several different hierarchies from simple to complex quantum systems: (i) isolated iodine molecules in the gas phase, (ii) molecular crystals of para-hydrogen, and (iii) single crystals of bismuth. In system (i), we have controlled and visualized the interference of vibrational wave packets in the isolated iodine molecules, and that wave-packet interference has been utilized to develop a molecular computer, which executes ultrafast Fourier transform. In system (ii), we have manipulated vibrational wave-functions delocalized in a para-hydrogen crystal. The long coherence lifetime of para-hydrogen crystals is a promising resource to preserve quantum information in bulk solids. In system (iii), we have controlled the excitation ratio of two orthogonal coherent phonon modes, whose coherent superposition has allowed for active control of ultrafast two-dimensional atomic motions in a single crystal of bismuth. Those atomic motions have been visualized by density functional theory calculations. Finally, the coherent control of an ensemble of ultracold Rydberg atoms is briefly discussed as future perspectives for exploring the quantum–classical boundary.
We have performed the double-pulse coherent control of nuclear wave packets, where the sequence of two identical femtosecond laser pulses generates two identical nuclear wave packets in the A30+ state of the single Hg–Ar van der Waals complex. The time delay between the two laser pulses is tuned with an accuracy in attosecond time scale to induce constructive and destructive interferences of the two nuclear wave packets. The interferogram measured by scanning the time delay shows a high-frequency oscillation with a period of 830 attoseconds. Wave packets have been manipulated in attosecond time scale for the first time.
Ultrafast high harmonic beams provide new opportunities for coherently controlling excitation and ionization processes in atoms, molecules, and materials on attosecond time scales by employing multiphoton two-pathway electron-wave-packet quantum interferences. Here we use spectrally tailored and frequency tuned vacuum and extreme ultraviolet harmonic combs, together with two phase-locked infrared laser fields, to show how the total single and double photoionization yields of argon can be coherently modulated by controlling the relative phases of both optical and electronic-wave-packet quantum interferences. This Letter is the first to apply quantum control techniques to double photoionization, which is a fundamental process where a single, high-energy photon ionizes two electrons simultaneously from an atom.
Attosecond chronoscopy enables the exploration of correlated electron dynamics in real time. One key observable of attosecond physics is the determination of "time zero" of photoionization, the time delay with which the wave packet of the ionized electron departs from the ionic core. This observable has become accessible by experimental advances in attosecond streaking and reconstruction of attosecond beating by interference of two-photon transitions (RABBIT) techniques. In this Letter, we explore photoionization time delays by strong extreme ultraviolet fields beyond the linear-response limit. We identify novel signatures in time delays signifying strong coupling between atoms and light fields and the light-field dressing of the ion. As a prototypical case, we study the interelectronic coherence and entanglement in helium driven by a strong extreme ultraviolet field. By the numerical solution of the time-dependent Schrödinger equation in its full dimensionality, we show that the time delay of the photoionized electron allows one to monitor the ultrafast variations of coherence dynamics and entanglement in real time.
The generation and control of extreme ultraviolet (XUV) radiation by high harmonic generation (HHG) have advanced ultrafast science, providing direct insights into electron dynamics on their natural time scale. Attosecond science has established the capability to resolve ultrafast quantum phenomena in matter by characterizing and controlling the classical properties of the high harmonics. Recent theoretical proposals have introduced novel schemes for generating and manipulating XUV HHG with distinct quantum features, paving the way to attosecond quantum optics. In this work, we transfer fundamental concepts in quantum optics into attosecond science. By driving the HHG process with a combination of an infrared bright squeezed vacuum (BSV, a non-classical state of light), and a strong coherent field, we imprint the quantum correlations of the input BSV onto both the ultrafast electron wavefunction and the harmonics' field. Performing in-situ HHG interferometry provides an insight into the underlying sub-cycle dynamics, revealing squeezing in the statistical properties of one of the most fundamental strong-field phenomena -- field induced tunneling. Our measurement allows the reconstruction of the quantum state of the harmonics through homodyne-like tomography, resolving correlated fluctuations in the harmonic field that mirror those of the input BSV. By controlling the delay between the two driving fields, we manipulate the photon statistics of the emitted attosecond pulses with sub-cycle accuracy. The ability to measure and control quantum correlations in both electrons and XUV attosecond pulses establishes a foundation for attosecond electrodynamics, manipulating the quantum state of electrons and photons with sub-cycle precision.