Ultrafast Hole Deformation Revealed by Molecular Attosecond Interferometry

Abstract

Understanding the evolution of molecular electronic structures is the key to explore and control photochemical reactions and photobiological processes. Subjected to strong laser fields, electronic holes are formed upon ionization and evolve in the attosecond timescale. It is crucial to probe the electronic dynamics in real time with attosecond-temporal and atomic-spatial precision. Here, we present molecular attosecond interferometry that enables the in situ manipulation of holes in carbon dioxide molecules via the interferometry of the phase-locked electrons (propagating in opposite directions) of a laser-triggered rotational wave packet. The joint measurement on high-harmonic and terahertz spectroscopy (HATS) provides a unique tool for understanding electron dynamics from picoseconds to attoseconds. The optimum phases of two-color pulses for controlling the electron wave packet are precisely determined owing to the robust reference provided with the terahertz pulse generation. It is noteworthy that the contribution of HOMO-1 and HOMO-2 increases reflecting the deformation of the hole as the harmonic order increases. Our method can be applied to study hole dynamics of complex molecules and electron correlations during the strong-field process. The threefold control through molecular alignment, laser polarization, and the two-color pulse phase delay allows the precise manipulation of the transient hole paving the way for new advances in attochemistry.

PbSe Nanosheets for High‐Performance Harmonic Mode Locking

“…At the same time, this work also associates harmonic mode soliton with soliton molecules, that is not very common in previous reports. [ 43–49 ] This strongly demonstrates the excellent performance of PbSe as nonlinear optical devices in the field of ultrafast optics.…”

Ultraviolet supercontinuum generation driven by ionic coherence in a strong laser field

“…On the other hand, the mechanism is not only applicable to molecular nitrogen ions but also to a range of other molecular ions. The multi-level quantum platform prepared by ultrafast lasers provides an unprecedented opportunity to investigate ionic quantum optics in the strong-field regime such as multi-electron dynamics [36][37][38] , electron-nucleus correlation 39 and quantum coherent control 40 .…”

Light-Induced Ultrafast Molecular Dynamics: From Photochemistry to Optochemistry

“…Tracking transient charge localization upon electron removal is however a difficult task because it involves a mixture of many one-hole configurations. , The observation of ultrafast charge migration has been realized in, for example, phenylalanine and C 2 HI molecules , (see Figure ) as a result of the development of attosecond technology. The unprecedented time resolution provided by attosecond pulses enables the measurement of the electron motion and its degree of coherence in molecular systems, offering powerful tools to detect and control the chemical reactions from the most fundamental perspective.…”