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Temporal Superresolution Mapping of Ultrafast Coherent Dynamics in Terahertz-Assisted Laser Field

Yizhu Zhang, Tian-Min Yan, Y. H. Jiang

Published Nov 17, 2017• 0 citations
OpenAlex

Abstract

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.

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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.
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.
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 present a fully quantum theory of time-resolved transient absorption spectroscopy, providing a general framework for describing the linear response of a nonequilibrium target to quantum probe fields beyond the semiclassical approximation. We elucidate how quantum correlations between probe-field frequency modes couple to coherences in the target and derive a simple expression for computing the resulting spectroscopic signals. We identify conditions under which quantum light can modify transient absorption spectra beyond the limits achievable with classical fields. Our work establishes a theoretical foundation for exploiting quantum light in ultrafast spectroscopy and suggests new routes for resolving dynamics in matter on timescales shorter than the duration of the probe pulse.
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.
Quantum entanglement has emerged as a great resource for spectroscopy and its importance in two-photon spectrum and microscopy has been demonstrated. Current studies focus on the two-photon absorption, whereas the Raman spectroscopy with quantum entanglement still remains elusive, with outstanding issues of temporal and spectral resolutions. Here we study the new capabilities provided by entangled photons in coherent Raman spectroscopy. An ultrafast frequency-resolved Raman spectroscopy with entangled photons is developed for condensed-phase molecules, to probe the electronic and vibrational coherences. Using quantum correlation between the photons, the signal shows the capability of both temporal and spectral resolutions not accessible by either classical pulses or the fields without entanglement. We develop a microscopic theory for this Raman spectroscopy, revealing the electronic coherence dynamics even at timescale of 50fs. This suggests new paradigms of optical signals and spectroscopy, with potential to push detection below standard quantum limit.
Time-resolved measurements of quantum dynamics are based on the availability of controlled events that are shorter than the typical evolution time scale of the processes to be observed. Here we introduce the concept of noise-enhanced pump-probe spectroscopy, allowing the measurement of dynamics significantly shorter than the average pulse duration by exploiting randomly varying, partially coherent light fields consisting of bunched colored noise. These fields are shown to be superior by more than a factor of 10 to frequency-stabilized fields, with important implications for time-resolved experiments at x-ray free-electron lasers and, in general, for measurements at the frontiers of temporal resolution (e.g., attosecond spectroscopy). As an example application, the concept is used to explain the recent experimental observation of vibrational wave-packet motion in D(2)(+) on time scales shorter than the average pulse duration.