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Acta Physica Sinica

The theoretical study of terahertz-streaking photoionization for ultrafast imaging of density matrix in rubidium atom

Zhong-Huo Ling, Shuai Wang, Jincang Zhang, Yi-Zhu Zhang, Tian-Min Yan, Yuhai Jiang

Published Jan 1, 2020• 0 citations
Publisher

Abstract

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.

DOI
10.7498/aps.69.20200218

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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.
A time-resolved spectroscopic protocol exploiting terahertz-assisted photoionization is proposed to reconstruct transient density matrix. Population and coherence elements are effectively mapped onto spectrally separated peaks in photoionization spectra. The beatings of coherence dynamics can be temporally resolved beyond the pulse duration, and the relative phase between involved states is directly readable from the oscillatory spectral distribution. As demonstrated by a photoexcited multilevel open quantum system, the method shows potential applications for subfemtosecond time-resolved measurements of coherent dynamics with free electron lasers and tabletop laser fields.
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.
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.
Laser-dressed photoemission spectroscopy has established itself as the gold standard of attosecond temporal metrology.In this technique, the attosecond structure of an extreme-ultraviolet pulse is retrieved from the wave function of the electron wave packet released during photoionization.Here, we show that this electron wave packet should rather be described using the density matrix formalism, thus allowing one to account for all processes that can affect its coherence, from the attosecond pulse generation to the photoemission and the measurement processes.Using this approach, we reconstruct experimentally a partially coherent electron wave packet with a purity of 0.11 (1 for full coherence).Comparison with theoretical models then allows us to identify the origins of this decoherence and to overcome several limitations such as beam-line instabilities or spectrometer resolution.Furthermore, we show numerically how this method gives access to the coherence and eigencomponents of complex photoelectron wave packets.It thus goes beyond the current measurement of photoionization time delays and provides a general framework for the analysis and understanding of complex photoemission processes.
An experimental continuous-wave (cw) pump-probe scheme is demonstrated by investigating the population and photoionization dynamics of an atomic system. Specifically, 6^66Li atoms are initially prepared in optically pumped 22S1/22^{2}S_{1/2}22S1/2​ and 22P3/22^{2}P_{3/2}22P3/2​ states before being excited via multi-photon absorption from a tunable femtosecond laser. The subsequent cascade back to the ground state is analyzed by ionizing the atoms in the field of a cw optical dipole trap laser. Conventional spectroscopic methods such as standard cold-target recoil-ion momentum spectroscopy (COLTRIMS) or velocity map imaging (VMI) cannot provide simultaneous momentum and time-resolved information on an event-by-event basis for the system investigated here. The new approach overcomes this limitation by leveraging electron-recoil ion coincidences, momentum conservation, and the cyclotron motion of the photoelectron in the magnetic spectrometer field. This enables the reconstruction of ionization times and time-of-flight of the charged target fragments with nanosecond resolution. As a result, not only can three-dimensional photoelectron momentum vectors be determined, but the (incoherent) population dynamics of the atomic system also become accessible. Future applications exploring coherent atomic dynamics on the nanosecond timescale would not only expand the scope of time-resolved spectroscopy but can also aid in developing coherent control schemes for precise atomic manipulation.
An experimental continuous-wave (cw) pump-probe scheme is demonstrated by investigating the population and photoionization dynamics of an atomic system. In particular, 6Li atoms are initially prepared in optically pumped 22S1/2 and 22P3/2 states before being excited via multi-photon absorption from a tunable femtosecond laser. The subsequent cascade back to the ground state is analyzed by ionizing the atoms in the field of a cw optical dipole trap laser. Conventional spectroscopic methods, such as standard cold-target recoil ion momentum spectroscopy or velocity map imaging, cannot provide simultaneous momentum and time-resolved information on an event-by-event basis for the system investigated here. The new approach overcomes this limitation by leveraging electron-recoil ion coincidences, momentum conservation, and the cyclotron motion of the photoelectron in the magnetic spectrometer field. This enables the reconstruction of ionization times and time-of-flight of the charged target fragments with nanosecond resolution. As a result, not only can three-dimensional photoelectron momentum vectors be determined, but the (incoherent) population dynamics of the atomic system also become accessible. Future applications exploring coherent atomic dynamics on the nanosecond timescale would not only expand the scope of time-resolved spectroscopy but can also aid in developing coherent control schemes for precise atomic manipulation.