Yizhu Zhang

Reconstruction and control of a time-dependent two-electron wave packet

The concerted motion of two or more bound electrons governs atomic and molecular non-equilibrium processes including chemical reactions, and hence there is much interest in developing a detailed understanding of such electron dynamics in the quantum regime. However, there is no exact solution for the quantum three-body problem, and as a result even the minimal system of two active electrons and a nucleus is analytically intractable. This makes experimental measurements of the dynamics of two bound and correlated electrons, as found in the helium atom, an attractive prospect. However, although the motion of single active electrons and holes has been observed with attosecond time resolution, comparable experiments on two-electron motion have so far remained out of reach. Here we show that a correlated two-electron wave packet can be reconstructed from a 1.2-femtosecond quantum beat among low-lying doubly excited states in helium. The beat appears in attosecond transient-absorption spectra measured with unprecedentedly high spectral resolution and in the presence of an intensity-tunable visible laser field. We tune the coupling between the two low-lying quantum states by adjusting the visible laser intensity, and use the Fano resonance as a phase-sensitive quantum interferometer to achieve coherent control of the two correlated electrons. Given the excellent agreement with large-scale quantum-mechanical calculations for the helium atom, we anticipate that multidimensional spectroscopy experiments of the type we report here will provide benchmark data for testing fundamental few-body quantum dynamics theory in more complex systems. They might also provide a route to the site-specific measurement and control of metastable electronic transition states that are at the heart of fundamental chemical reactions.

Fractional high-order harmonic combs and energy tuning by attosecond-precision split-spectrum pulse control

We experimentally control high-order harmonic generation by applying a versatile few-cycle pulse-shape control method: splitting up a single broadband continuous laser spectrum into two sections and applying sub-femtosecond relative time delays. For certain time delays, fractional high-harmonic combs (noninteger harmonics) are generated which we find to result from the controlled interference of two attosecond pulse trains. We also observe time-delay-dependent energy-tunability of the high-order harmonics for an asymmetrically split spectrum consisting of a strong and a weak component. The tuning mechanism is quantitatively understood by the controlled modulation of the instantaneous driver frequency at the peak of the shaped laser pulse.

Elliptically polarized terahertz emission in the forward direction of a femtosecond laser filament in air

Elliptically polarized terahertz emission from a femtosecond laser filament in air in the forward direction was discovered by using a wire grid polarizer and electro-optic sampling technique. The generation mechanism could be through four-wave optical rectification or second-order optical rectification inside the filament zone where the inversion symmetry of air is broken.

Charge and Nuclear Dynamics Induced by Deep Inner-Shell Multiphoton Ionization of CH3I Molecules by Intense X-ray Free-Electron Laser Pulses

In recent years, free-electron lasers operating in the true X-ray regime have opened up access to the femtosecond-scale dynamics induced by deep inner-shell ionization. We have investigated charge creation and transfer dynamics in the context of molecular Coulomb explosion of a single molecule, exposed to sequential deep inner-shell ionization within an ultrashort (10 fs) X-ray pulse. The target molecule was CH3I, methane sensitized to X-rays by halogenization with a heavy element, iodine. Time-of-flight ion spectroscopy and coincident ion analysis was employed to investigate, via the properties of the atomic fragments, single-molecule charge states of up to +22. Experimental findings have been compared with a parametric model of simultaneous Coulomb explosion and charge transfer in the molecule. The study demonstrates that including realistic charge dynamics is imperative when molecular Coulomb explosion experiments using short-pulse facilities are performed.

Passively phase-stable, monolithic, all-reflective two-dimensional electronic spectroscopy based on a four-quadrant mirror.

A design for a passively phase-stable two-dimensional electronic spectroscopy experiment, based on a four-quadrant mirror concept, is introduced. The setup, which is particularly simple and robust, achieves subwavelength stability without the need for active stabilization or diffractive optical elements. Since only reflective optical components are used, the setup is suitable for few-cycle laser pulses and ultrabroad-bandwidth light in the ultraviolet, visible, and near-IR regions, with the capability to be used under grazing incidence for soft x ray or x-ray light at free-electron lasers.

Portraying polarization state of terahertz pulse generated by a two-color laser field in air

By using an electro-optic sampling technique, the instantaneous field vector of the terahertz (THz) pulse generated by mixing a near-IR femtosecond pulse and its second harmonic in air has been studied. The polarization of the investigated THz pulse is found to be predominantly linear and orthogonal to that of the second harmonic, revealing the major role of chi((3))(xyxy) during the four-wave mixing process.

Propagation of terahertz wave inside femtosecond laser filament in air

Terahertz (THz) generation in femtosecond laser filament has recently been found to greatly expand THz applications in atmospheric remote sensing. In this article, by investigating the THz waveform emitted from different length of filaments, the refractive index of the THz wave has been found to be smaller than the unity within the filament region. It indicates that the THz pulse may propagate inside the filament though the diameter of the filament is much smaller than the wavelength of the THz wave. The hypothesis is supported by further numerical simulation, which considers the radially non-uniform plasma density distribution of the filament.

Precise phase determination with the built-in spectral interferometry in two-dimensional electronic spectroscopy.

A new method determining the precise phase of pulse sequences in two-dimensional electronic spectroscopy (2DES) is proposed merely using the already built-in spectral interferometry. The approach is easily implemented without the supplementary instrumental construction, only at the expense of a few additional scanning and data-fitting processes. This method is executed with the sample in place, effectively avoiding the phase ambiguities of the beam propagation in samples, thus calibrating the absolute phase at the exact interaction region. The new proposed method is expected to improve the phasing procedure in 2DES in a more convenient way.

Compact design for two-dimensional electronic spectroscopy

We present a passively phase-stabilized two-dimensional electronic spectroscopy (2DES) with a compact size, and the ease of implementation and maintenance. Our design relies on a mask beam-splitter with four holes to form non-collinear box geometry, and a homebuilt stacked retroreflector, which introduces the phase-locked pulse sequence, remedying the instability of commonly used translation stages. The minimized size of the setup suppresses the influences of optical path-length fluctuations during measurements, improving the phase stability and precise timing of pulse sequences. In our 2DES, only few conventional optical components are used, which make this sophisticated instrumentation convenient to establish and particularly easy to conduct alignment. In data analysis, the self-referencing spectral interferometry (SRSI) method is first introduced to extract the complex-valued signal from spectral interferometry in 2DES. The alternative algorithm achieves the improvement of the signal-to-noise ratio (SNR) and considerable reduction of data acquisition time. The new setup is suitable over a tunable range of spectroscopic wavelength, from ultraviolet (UV) to the near-infrared (NIR) regime, and for ultra-broadband bandwidth, few-cycle laser pulses.

Post-processing phase-correction algorithm in two-dimensional electronic spectroscopy.

In a typical two-dimensional electronic spectroscopy (2DES) experiment, the timing errors of the coherence and emission time when determining the absolute time zeros usually introduce extraneous spectral phase slopes and distort the 2D spectrum. In this work, a phase-correction method that merely relies on the data post-processing algorithm is proposed. The method allows reconstructing the spectrum by simply subtracting the artificial linear spectral-phase slopes from the phase component of the 2D spectrum along both coherence and emission frequency axes. The new method has the advantages of ease of implementation and no need for the supplementary experiments and iterative fitting algorithm as commonly-used phasing methods, which may improve the phasing issue in 2DES and serve as a cross-check of now available phasing methods.