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Measuring the energy spectra of unknown samples using coherent control of the complex phase of X-rays

Benedikt Herkommer

Published Jan 1, 2019• 1 citation
OpenAlex

Abstract

The field of quantum optics describes the interaction of electromagnetic radiation with matter whereby both are described quantum mechanically. So far the used frequencies of the radiation, were restricted to the operation range of lasers, which is between microwave to ultraviolet radiation. With the availability of new radiation sources such as sychrotrons, the field of X-ray quantum optics could be established. The high energy of the X-rays offer new possibilities, such as the examination of the interaction of radiation the nuclei of atoms. Unfortunately, X-ray source limitations still prohibit the direct transfer of control or detection schemes. One approach to overcome such limitations are mechanical motions of resonant absorber, which induces an additional phase at nuclear forward scattering. In this thesis the use of oscillating resonant absorber is examined theoretically. The phase offset of the oscillation offers an additional and controllable degree of freedom, which in uences the time and energy spectrum of a scattered wave packet. One problem occurring due to the high energy, is the lack of methods to measure the energy spectrum. To solve this problem, a new approach is developed, using the phase offset to measure the energy spectrum and the complex phase in the energy domain.

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The field of quantum optics describes the interaction of electromagnetic radiation with matter whereby both are described quantum mechanically. So far the used frequencies of the radiation, were restricted to the operation range of lasers, which is between microwave to ultraviolet radiation. With the availability of new radiation sources such as sychrotrons, the field of X-ray quantum optics could be established. The high energy of the X-rays offer new possibilities, such as the examination of the interaction of radiation the nuclei of atoms. Unfortunately, X-ray source limitations still prohibit the direct transfer of control or detection schemes. One approach to overcome such limitations are mechanical motions of resonant absorber, which induces an additional phase at nuclear forward scattering. In this thesis the use of oscillating resonant absorber is examined theoretically. The phase offset of the oscillation offers an additional and controllable degree of freedom, which in uences the time and energy spectrum of a scattered wave packet. One problem occurring due to the high energy, is the lack of methods to measure the energy spectrum. To solve this problem, a new approach is developed, using the phase offset to measure the energy spectrum and the complex phase in the energy domain.
This work aims at development of new dynamical methods to control a resonant light-matter interaction as well as at their application for producing new sources of coherent intense sub-fs radiation in x-ray range. The dynamical control is based on modulation in time and in space of the parameters of the atomic transition (coupled to the resonant high-frequency field) by means of sufficiently strong off-resonant low-frequency control field. In particular, it may result in efficient transfer of quasi-monochromatic VUV or XUV radiation into ultrashort pulses via its resonant interaction with atomic hydrogen gas or plasma of hydrogen-like ions respectively by means of two different techniques: time and space dependent linear Stark effect or interruption of resonant interaction by the tunneling ionization, as shown in previous works of our group. \n\nIn this thesis, I further develop these ideas and demonstrate their important potential applications. First of all, both techniques are extended to arbitrary (non-hydrogen-like) atomic medium. Furthermore, advanced analytical and numerical solutions describing a process of pulses formation are found and shown to be in excellent agreement with each other. A deep physical analogy between the processes of coherent forward scattering of γ-ray radiation in the vibrated quasi-resonant nuclear absorber and the XUV field propagation in the quasi-resonant atomic medium in the presence of the moderately strong IR field is established. \n\nFinally, the application of the developed techniques for production of intense coherent attosecond sources of soft X-ray radiation, including so-called “water window” range (2.2-4.3nm) (especially promising for dynamical imaging of the proteins in a living cell) is proposed. Two different paths towards production of intense coherent attosecond pulses in a soft X-ray range are suggested: (i) via efficient transformation of the picosecond radiation of the high energy pulses of the existing x-ray plasma lasers into the trains of attosecond pulses in the resonant passive plasma, and (ii) via amplification of the low energy pulses of the existing high harmonic sources in the resonant active plasma of x-ray lasers.
Means to coherently control single x-ray photons in resonant scattering of light off nuclei by electric or magnetic fields are investigated theoretically. In order to derive the time response in nuclear forward scattering, we adapt the Maxwell–Bloch equations known from quantum optics to describe the resonant light pulse propagation through a nuclear medium. Two types of time-dependent perturbations of nuclear forward scattering are considered for coherent control of the resonantly scattered x-ray quanta. Firstly, the simultaneous coherent propagation of two pulses through the nuclear sample is addressed. We find that the signal of a weak pulse can be enhanced or suppressed by a stronger pulse simultaneously propagating through the sample in counter-propagating geometry. Secondly, the effect of a time-dependent hyperfine splitting is investigated and we put forward a scheme that allows parts of the spectrum to be shifted forward in time. This is the inverse effect of coherent photon storage and may become a valuable technique if single x-ray photon wavepackets are to become the information carriers in future photonic circuits.
This thesis describes quantum optical experiments with x-rays with the aim of reaching the strong-coupling regime of light and matter. We make use of the interaction which arisesbetween resonant matter and x-rays in specially designed thin-film nanostructures which form x-ray cavities. Here, the resonant matter are Tantalum atoms and the Iron isotope 57^{57}57Fe. Both limit the number of modes available to the resonant atoms for interaction, and enhances the interaction strength. Thus we have managed to observe a number of phenomena well-known in quantum optics, which are the building blocks for sophisticated applications in e.g. metrology. Among these are the strong coupling of light and matter and the concurrent exchange of virtual photons, often called Rabi oscillations. Furthermore we have designed and tested a type of cavity hitherto unused in x-ray optics. Finally, we develop a new method for synchrotron Mössbauer spectroscopy, which not only promises to yield high-resolution spectra, but also enables the retrieval of the phase of the scattered light. The results open new avenues for quantum optical experiments with x-rays, particularly with regards to the ongoing development of high-brilliance x-ray free-electron lasers.
This report results from a contract tasking Moscow State University as follows: Exploration of methods to control the radiative gamma- processes in nuclei is currently one of the most promising investigation directions of the modern Quantum Nucleonics - a new realm of contemporary Physics which spreads the basic conceptual ideas and methods of optical Quantum Electronics of atoms and molecules to the gamma-ray range and atomic nuclei and even anti-particles. One of the most important problems in this field is the generation of coherent gamma-radiation by a Gamma-ray Lasing (GRL) process which makes use of excited nuclei as an amplifying medium. The most likely medium for gamma-ray lasers is an ensemble of metastable nuclear isomers, Direct excitation of these isomeric states by electrons or X-ray photons will also create a deeper understanding of nuclear structure and properties.
The coherent storage and phase modulation of x-ray single-photon wave packets in the resonant scattering of light off nuclei is theoretically investigated. We show that by switching off and on again the magnetic field in the nuclear sample, phase-sensitive storage of photons in the keV regime can be achieved. Corresponding π phase modulation of the stored photon can be accomplished if the retrieving magnetic field is rotated by 180°. The development of such x-ray single-photon control techniques is a first step towards forwarding quantum optics and quantum information to shorter wavelengths and more compact photonic devices.
We report a method for coherent control of γ-photons, enabling the shaping of γ-ray intensity in nearly arbitrary waveforms. Different intensity waveforms are created by adjusting the motion profile of a resonant absorber (an ensemble of Mössbauer nuclei) and tuning the energy of the incident radiation. A crucial aspect of this method is the use of a low fundamental frequency of vibrations, which broadens the possibilities for γ-ray control. The results of numerical simulations are experimentally validated by generating single and double γ-pulses and inducing short-term absorption. For this, a resonant absorber containing 57Fe nuclei was vibrated with different motion profiles composed of 12 harmonics with a fundamental frequency of 1 MHz. The proposed technique represents an advancement in the manipulation of γ-rays, and potentially x rays, paving the way for the performance of unique types of γ-ray or x-ray quantum experiments and the development of tools such as adjustable table-top γ-pulse sources or γ-ray or x-ray delays and gates. Moreover, inverse application of the method enables investigation of motion at the picometer scale.