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Chinese Physics Letters

Rabi Oscillations and Coherence Dynamics in Terahertz Streaking-Assisted Photoelectron Spectrum

Shuai Wang, Zhiyuan Zhu, Yizhu Zhang, Tian-Min Yan, Yuhai Jiang

Published Jan 1, 2021• 4 citations
Publisher

Abstract

We present an approach, a Terahertz streaking-assisted photoelectron spectrum (THz SAPS), to achieve direct observations of ultrafast coherence dynamics with timescales beyond the pulse duration. Using a 24 fs probe pulse, the THz SAPS enables us to well visualize Rabi oscillations of 11.76 fs and quantum beats of 2.62 fs between the 5S 1/2 and 5P 3/2 in rubidium atoms. The numerical results show that the THz SAPS can simultaneously achieve high resolution in both frequency and time domains without the limitation of Heisenberg uncertainty of the probe pulse. The long probe pulse promises sufficiently high frequency resolution in photoelectron spectroscopy allowing to observe Autler–Townes splittings, whereas the streaking THz field enhances temporal resolution for not only Rabi oscillations but also quantum beats between the ground and excited states. The THz SAPS demonstrates a potential applicability for observation and manipulation of ultrafast coherence processes in frequency and time domains.

DOI
10.1088/0256-307x/38/1/013401

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We present an approach, a Terahertz streaking-assisted photoelectron spectrum (THz SAPS), to achieve direct observations of ultrafast coherence dynamics with timescales beyond the pulse duration. Using a 24 fs probe pulse, the THz SAPS enables us to well visualize Rabi oscillations of 11.76 fs and quantum beats of 2.62 fs between the 5S 1/2 and 5P 3/2 in rubidium atoms. The numerical results show that the THz SAPS can simultaneously achieve high resolution in both frequency and time domains without the limitation of Heisenberg uncertainty of the probe pulse. The long probe pulse promises sufficiently high frequency resolution in photoelectron spectroscopy allowing to observe Autler–Townes splittings, whereas the streaking THz field enhances temporal resolution for not only Rabi oscillations but also quantum beats between the ground and excited states. The THz SAPS demonstrates a potential applicability for observation and manipulation of ultrafast coherence processes in frequency and time domains.
Terahertz-streaking photoionization can be exploited to resolve ultrafast quantum beating and reconstruct the ultrafast evolution of density matrix. Here, we propose an experimental strategy to implement the method merely with the tabletop femtosecond system and magneto-optical trap reaction microscopy. The probe pulse consists of an ultraviolet pulse with pulse duration of about 30 fs and a strong terahertz pulse with strength of about 2.6 fs in rubidium-atom superposition. The population and coherence terms of the density matrix can be projected into different positions of the photoelectron momentum distribution. The reconstruction algorithm was designed to acquire the ultrafast evolution of density matrix from the time-dependent photoelectron spectrum. The experimental conception can demonstrate the newly proposed transient spectral method only with the commercial femtosecond laser system and magneto-optical trap reaction microscopy, thus preventing the complex laser system, such as extreme ultraviolet free electron lasers and attosecond higher harmonics, allowing a new metrology to explore the coherence dynamics of quantum systems.
We study the photoelectron spectra of hydrogen and helium ionized by intense ultrafast two-color XUV laser pulses by numerically solving the time-dependent Schrödinger equation.The photon energy of the pump pulse is tuned to the 1s-2p excitation energy, inducing Rabi oscillations between these bound states and forming an Autler-Townes (AT) doublet of dressed states.When ionized by a time-delayed ultrafast XUV pulse with duration shorter than the Rabi oscillation period, we find novel and drastically enhanced AT splittings in the photoionization spectrum.We identify their origin in terms of the temporal interference of two attosecond wave packets whose spectral distribution is controlled by the interplay between Rabi frequency and bandwidth of the probe pulse.These time-dependent features in the spectra can be much larger than the standard AT spacing induced by the pump pulse alone and can be controlled by the time delay and the duration of the probe pulse.
Quantum coherence is of potential applications from quantum computation using simple atoms to optimized energy transports in biomolecular complexes. Here, a time-resolved spectroscopic protocol exploiting a terahertz-assisted field locked with the probe pulse is proposed for full observations of the evolution of elements in transient density matrix. Coherence contributions of off-diagonal elements are detectable in the spotlight. The coherence dynamics for photoexcitation of hydrogen atom are explicitly demonstrated with significantly improved temporal resolution beyond the probe pulse duration. Present approach with improving time resolution and highlighting coherence dynamics displays potential applications for sub-femtosecond or attosecond time-resolved measurements in free electron lasers and tabletop laser fields.
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.
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.
Abstract Based on numerical solutions of the time-dependent Schrödinger equation, we theoretically investigate the photoelectron spectrum of hydrogen atoms ionized by a pair of ultrashort, intense, and orthogonally polarized laser pulses with a relative time delay in a pump–probe configuration. The pump pulse resonantly excites electrons from the 1s and 2p levels, inducing Rabi oscillations. The resulting dynamically enhanced Autler–Townes (AT) splitting is observed in the photoelectron energy spectrum upon interaction with the second probe pulse. In contrast to the previous parallel-polarization scheme, the proposed orthogonal-polarization configuration enables the resolution of dynamically enhanced AT splitting over a considerably wider range of probe photon energies.