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The Review of Laser Engineering

Ultrafast Multiphoton Manipulation of Quantum States by Intense Laser Pulses

Mizuho Fushitani, Akiyoshi Hishikawa

Published Jan 1, 2017• 0 citations
Publisher

Abstract

Coherent light-matter interaction drives a variety of interesting processes in a quantum system. Rabi oscillation is one such process offering a periodic population transfer between quantum states in an ultrashort time scale. Here we demonstrate a robust and simple scheme to achieve femtosecond twophoton Rabi oscillations by intense NIR laser pulses, using excited He atoms prepared by EUV-FEL. The extension to multiphoton regime will expand the applicability to highly excited or dipole-forbidden states.

DOI
10.2184/lsj.45.8_493

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Coherent light-matter interaction drives a variety of interesting processes in a quantum system. Rabi oscillation is one such process offering a periodic population transfer between quantum states in an ultrashort time scale. Here we demonstrate a robust and simple scheme to achieve femtosecond twophoton Rabi oscillations by intense NIR laser pulses, using excited He atoms prepared by EUV-FEL. The extension to multiphoton regime will expand the applicability to highly excited or dipole-forbidden states.
Abstract Quantum-state manipulation through coherent interaction with a radiation field is a fundamental process with broad implications in quantum optics and quantum information processing. However, current quantum control methods are limited by their operation at Rabi frequencies below the gigahertz range, which restricts their applicability to systems with long coherence times. To overcome this limitation, alternative approaches utilizing ultrafast driving lasers have garnered great interest. In this work, we demonstrate two-photon Rabi oscillations in the excited states of argon operating at terahertz frequencies driven by ultrafast laser pulses. Leveraging quantum-path interferometry, we are able to measure and manipulate both the amplitudes and phases of the transition dipoles by exploiting the intensity and polarization state of the driving laser. This precise control enables femtosecond population transfer and coherent accumulation of geometric phase. Our findings provide valuable insights into the all-optical manipulation of extreme-ultraviolet radiations and demonstrate the possibility of ultrafast quantum control through interferometric multiphoton transitions.
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.
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.
We demonstrate Rabi oscillations in nonlinear ionization of argon by an intense femtosecond extreme ultraviolet (XUV) laser field produced by high-harmonic generation. We monitor the formation of Ar2+\mathrm{A}{\mathrm{r}}^{2+}Ar2+ as a function of the time delay between the XUV pulse and an additional near-infrared (NIR) femtosecond laser pulse, and show that the population of an Ar+∗\mathrm{A}{\mathrm{r}}^{+*}Ar+∗ intermediate resonance exhibits strong modulations both due to an NIR laser-induced Stark shift and XUV-induced Rabi cycling between the ground state of Ar+\mathrm{A}{\mathrm{r}}^{+}Ar+ and the Ar+∗\mathrm{A}{\mathrm{r}}^{+*}Ar+∗ excited state. Our experiment represents a direct experimental observation of a Rabi-cycling process in the XUV regime.
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.