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arXiv:2312.04442 · Science Advances

Generation of entanglement using a short-wavelength seeded free-electron laser

Saikat Nandi, Axel Stenquist, Asimina Papoulia, Edvin Olofsson, L. Badano, Mattias Bertolino, David Busto, Carlo Callegari, Stefanos Carlström, Miltcho Bojanov Danailov, Philipp V. Demekhin, Michele Di Fraia, P. Johnsson, R. Feifel, Guillaume Gallician, Luca Giannessi, Mathieu Gisselbrecht, Michele Manfredda, Michael Meyer, Catalin Miron, Jasper Peschel, Oksana Plekan, Kevin Charles Prince, Richard James Squibb, Marco Zangrando, Felipe Zapata, Shiyang Zhong, Jan Marcus Dahlström

Published Apr 17, 2024• 31 citations
arXivHTMLPDF

Abstract

Quantum entanglement between the degrees of freedom encountered in the classical world is challenging to observe due to the surrounding environment. To elucidate this issue, we investigate the entanglement generated over ultrafast timescales in a bipartite quantum system comprising two massive particles: a free-moving photoelectron, which expands to a mesoscopic length scale, and a light-dressed atomic ion, which represents a hybrid state of light and matter. Although the photoelectron spectra are measured classically, the entanglement allows us to reveal information about the dressed-state dynamics of the ion and the femtosecond extreme ultraviolet pulses delivered by a seeded free-electron laser. The observed generation of entanglement is interpreted using the time-dependent von Neumann entropy. Our results unveil the potential for using short-wavelength coherent light pulses from free-electron lasers to generate entangled photoelectron and ion systems for studying spooky action at a distance.

DOI
10.1126/sciadv.ado0668

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This thesis investigates quantum dynamics induced in atoms by ultrashort pulses of light. The work is motivated by recent developments in free-electron lasers, which generate ultrashort pulses of intense, coherent light and enable coherent control of quantum dynamics. We develop theoretical models to study the processes of absorption and emission in laser-atom interactions. Additionally, we study photoionisation, which creates an ion and an electron, and the entanglement that can be generated between these particles. Finally, we have investigated how the spontaneous decay of the ion induces entanglement transfer from the ion-electron pair to the electron-photon pair.This thesis compiles seven papers. Paper I investigates the absorption of light from an attosecond pulse by an atom in a prepared coherent superposition of states. We show how the evolution of the phase of the superposition wave packet influences the attosecond transient absorption spectra. Paper II predicts the existence of Mollow-like triplets in the absorption spectra of strongly coupled atoms. We establish the conditions for the pulse envelope under which this triplet pattern can be supported.Paper III studies two-photon Rabi oscillations, establishing which systems can sustain such dynamics. We find that a two-photon Rabi oscillating system can induce giant counter-rotating oscillations in the population dynamics, enabling investigations of physical effects beyond the rotating-wave approximation.Paper IV studies ionisation from an atom strongly coupled by a dichromatic field, where interference between the two frequency components shapes the temporal symmetry of the atomic dynamics, allowing for coherent control of the photoelectron distribution.Paper V considers an experiment performed at a Free-Electron Laser facility where a helium atom is ionised and the resulting ion is subsequently strongly coupled. The photoelectron spectra are theoretically reproduced and the entanglement between the ion and photoelectron is studied. Paper VI investigates how the entanglement in the ion--electron pair, generated via photoionisation followed by strong coupling, can be coherently controlled by harnessing the time symmetry of the pulse. We find that the observable manifestation of the entanglement can be altered in such a way that the electron energy becomes associated with the ionic state, allowing the entanglement to be detected via coincidence measurements. Paper VII investigates how quantum correlations between the ion and the electron can be coherently controlled by sequential strong coupling of the ion. We find that both the build-up of entanglement and its manifestation can be controlled, and we establish a quantitative measure of the amplitude entanglement that explains the dynamics in an intuitive way. Paper VIII studies the process of entanglement transfer induced by the spontaneous decay of the ion. We find that the ion--electron entanglement generated during the ultrashort interaction with the laser field is transferred to the electron--photon system over the much longer timescale of fluorescence.

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Observation of Rabi dynamics with a short-wavelength free-electron laser

Saikat Nandi, Edvin Olofsson, Mattias Bertolino +26 more

Abstract Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field1. They are ubiquitous in physics with applications in different areas such as photonics2, nano-electronics3, electron microscopy4 and quantum information5. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light–matter interactions within the rotating-wave approximation6. Although intense nanometre-wavelength light sources have been available for more than a decade7–9, Rabi dynamics at such short wavelengths has not been directly observed. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser10 can drive Rabi dynamics between the ground state and an excited state in helium atoms. The measured photoelectron signal reveals an Autler–Townes doublet and an avoided crossing, phenomena that are both fundamental to coherent atom–field interactions11. Using an analytical model derived from perturbation theory on top of the Rabi model, we find that the ultrafast build-up of the doublet structure carries the signature of a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond12 and few-femtosecond13 extreme-ultraviolet pulses, our results unfold opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.

Nature•Aug 17, 2022•106 citations
Quantum entanglement between the degrees of freedom encountered in the classical world is challenging to observe due to the surrounding environment. To elucidate this issue, we investigate the entanglement generated over ultrafast timescales in a bipartite quantum system comprising two massive particles: a free-moving photoelectron, which expands to a mesoscopic length scale, and a light-dressed atomic ion, which represents a hybrid state of light and matter. Although the photoelectron spectra are measured classically, the entanglement allows us to reveal information about the dressed-state dynamics of the ion and the femtosecond extreme ultraviolet pulses delivered by a seeded free-electron laser. The observed generation of entanglement is interpreted using the time-dependent von Neumann entropy. Our results unveil the potential for using short-wavelength coherent light pulses from free-electron lasers to generate entangled photoelectron and ion systems for studying spooky action at a distance.
In coherent light-matter interactions the coherent state produced by the light pulse remains coherent during the entire period of observation. One of the well-known examples of such interactions is the Rabi oscillation—a periodic transfer of population in a two-level system induced by an external electromagnetic field. While these oscillations have been studied in light-matter interactions since the discovery of laser itself, most of the studies are limited to long wavelengths, typically ranging from microwave to visible radiation. Here, we discuss how such oscillations can be generated at shorter wavelengths, for example in the extreme ultraviolet domain, using intense femtosecond pulses from seeded free-electron lasers. When a two-level system is undergoing Rabi oscillations, it can be described via an ‘atom + photon’ dressed-state, the properties of which can be further manipulated to study quantum entanglement between massive particles. Our results offer opportunities to employ these intense laser pulses for generating and controlling coherent light-matter interactions across ultrashort timescales.
Quantitative control and measurement of quantum entanglement are essential for advancing quantum technologies. Photoionization induced by ultrashort laser pulses provides a unique platform for studying entanglement between photoelectrons and residual ions, representing one of the most intriguing quantum phenomena in attosecond physics. Although extensive studies have focused on the coherence properties within either the emitted electrons or the ions individually, the electron-ion entanglement has remained largely unexplored. In this work, we bridge this gap by investigating the resonance-enhanced multiphoton ionization of argon atoms driven by two time-delayed ultrashort ultraviolet pulses. Employing state-of-the-art first-principles multi-electron simulations, we demonstrate the ability to reconstruct and precisely manipulate the purity of electron quantum states through detailed analysis of the photoelectron angular distributions. Our results reveal distinct scattering-phase differences among various electron configurations within the same partial wave channel, providing unequivocal evidence of electron-ion correlation and entanglement. With the fast development of free-electron lasers, this study establishes an experimentally feasible framework for directly controlling quantum entanglement in ultrafast ionization processes, offering new insights and powerful methodologies for exploring complex electron dynamics in many-electron systems.
This thesis investigates quantum dynamics induced in atoms by ultrashort pulses of light. The work is motivated by recent developments in free-electron lasers, which generate ultrashort pulses of intense, coherent light and enable coherent control of quantum dynamics. We develop theoretical models to study the processes of absorption and emission in laser-atom interactions. Additionally, we study photoionisation, which creates an ion and an electron, and the entanglement that can be generated between these particles. Finally, we have investigated how the spontaneous decay of the ion induces entanglement transfer from the ion-electron pair to the electron-photon pair.This thesis compiles seven papers. Paper I investigates the absorption of light from an attosecond pulse by an atom in a prepared coherent superposition of states. We show how the evolution of the phase of the superposition wave packet influences the attosecond transient absorption spectra. Paper II predicts the existence of Mollow-like triplets in the absorption spectra of strongly coupled atoms. We establish the conditions for the pulse envelope under which this triplet pattern can be supported.Paper III studies two-photon Rabi oscillations, establishing which systems can sustain such dynamics. We find that a two-photon Rabi oscillating system can induce giant counter-rotating oscillations in the population dynamics, enabling investigations of physical effects beyond the rotating-wave approximation.Paper IV studies ionisation from an atom strongly coupled by a dichromatic field, where interference between the two frequency components shapes the temporal symmetry of the atomic dynamics, allowing for coherent control of the photoelectron distribution.Paper V considers an experiment performed at a Free-Electron Laser facility where a helium atom is ionised and the resulting ion is subsequently strongly coupled. The photoelectron spectra are theoretically reproduced and the entanglement between the ion and photoelectron is studied. Paper VI investigates how the entanglement in the ion--electron pair, generated via photoionisation followed by strong coupling, can be coherently controlled by harnessing the time symmetry of the pulse. We find that the observable manifestation of the entanglement can be altered in such a way that the electron energy becomes associated with the ionic state, allowing the entanglement to be detected via coincidence measurements. Paper VII investigates how quantum correlations between the ion and the electron can be coherently controlled by sequential strong coupling of the ion. We find that both the build-up of entanglement and its manifestation can be controlled, and we establish a quantitative measure of the amplitude entanglement that explains the dynamics in an intuitive way. Paper VIII studies the process of entanglement transfer induced by the spontaneous decay of the ion. We find that the ion--electron entanglement generated during the ultrashort interaction with the laser field is transferred to the electron--photon system over the much longer timescale of fluorescence.
Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field. They are ubiquitous in physics with applications in different areas such as photonics, nano-electronics, electron microscopy, and quantum information. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light-matter interaction within the rotating wave approximation\cite. Although intense nanometer-wavelength light-sources have been available for more than a decade, Rabi dynamics at such short wavelengths have not been observed directly. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser can drive Rabi oscillations between the ground state and an excited state in helium atoms. The measured photoemission signal revealed an Autler-Townes doublet as well as an avoided crossing, phenomena that are both trademarks of quantum optics. Using theoretical analyses that go beyond the strong-field approximation, we found that the ultrafast build-up of the doublet structure follows from a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond and few-femtosecond extreme-ultraviolet pulses, our results offer opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.
The dynamical behavior of entanglement between the atomic ensemble and the spontaneous emission is investigated by applying the femtosecond Gaussian pulses in double- lambda quantum system. In fact by solving the density matrix equations of motion in such a system and by using the von Neumann entropy, the degree of entanglement (DEM) could be measured in semi classical regime and in the multi-photon resonance condition. We interested in investigating the maximum value for DEM and controlled the DEM via relative phase. At first we consider three laser fields as CW optical laser fields and one femtosecond Gaussian field. In this case DEM has interesting behavior. When the system is applied by the other laser fields and Gaussian pulse is still there DEM can be controlled via phase but after finishing the time duration of the femtosecond Gaussian pulse DEM will be phase independent. Then we consider all the laser fields as femtosecond Gaussian pulses which interact with atomic system and we achieve to this point that the steady state entanglement can be occurred by using such ultra-short laser pulses; in this situation DEM will be phase independent. The system would be disentangled in special parameters of Rabi frequencies and all the atoms are coherently populated in a dark state in dressed state picture. Moreover when the system is entangled, there is a population distribution of the atoms in dressed states.
Abstract Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field1. They are ubiquitous in physics with applications in different areas such as photonics2, nano-electronics3, electron microscopy4 and quantum information5. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light–matter interactions within the rotating-wave approximation6. Although intense nanometre-wavelength light sources have been available for more than a decade7–9, Rabi dynamics at such short wavelengths has not been directly observed. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser10 can drive Rabi dynamics between the ground state and an excited state in helium atoms. The measured photoelectron signal reveals an Autler–Townes doublet and an avoided crossing, phenomena that are both fundamental to coherent atom–field interactions11. Using an analytical model derived from perturbation theory on top of the Rabi model, we find that the ultrafast build-up of the doublet structure carries the signature of a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond12 and few-femtosecond13 extreme-ultraviolet pulses, our results unfold opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.