Related papers: High-harmonic probing of electronic coherence in d…
The detection of electron motion and electronic wavepacket dynamics is one of the core goals of attosecond science. Recently, choosing the nitric oxide (NO) molecule as an example, we have introduced and demonstrated a new experimental…
Exposing a molecule to intense light pulses may bring this molecule to a nonstationary quantum state, thus launching correlated dynamics of electronic and nuclear subsystems. Although much had been achieved in the understanding of…
The existence of electronic coherence can fundamentally change the scenario of nonlinear interaction of light with quantum systems such as atoms and molecules, which, however, has escaped from observation in the investigations of strong…
We explore long lived electronic coherences in molecules using shaped ultrafast laser pulses to launch and probe entangled nuclear-electronic wave packets. We find that under certain conditions, the electronic phase remains well defined…
We theoretically propose a multidimensional high-harmonic echo spectroscopy technique which utilizes strong optical fields to resolve coherent electron dynamics spanning an energy range of multiple electron Volts. Using our recently…
We study the ultrafast dynamics initiated by a coherent superposition of core-excited states of nitrous oxide molecule. Using high-level \textit{ab-initio} methods, we show that the decoherence caused by the electronic decay and the nuclear…
Nonstationary molecular states which contain electronic coherences can be impulsively created and manipulated by using recently-developed ultrashort optical and X-ray pulses via photoexcitation, photoionization and Auger processes. We…
Tracking the coupled motion of electrons and nuclei on their intrinsic timescales is essential to understanding and controlling photochemical transformations. While attosecond techniques have provided unprecedented insight into electronic…
We use extreme-ultraviolet interferometry to measure the phase of high-order harmonic generation from transiently aligned CO2 molecules. We unambiguously observe a reversal in phase of the high order harmonic emission for higher harmonic…
We present momentum resolved covariance measurements of entangled electronic-nuclear wave packets created and probed with octave spanning phaselocked ultrafast pulses. We launch vibrational wave packets on multiple electronic states via…
Electronic coherences are key to understanding and controlling photo-induced molecular transformations. We identify a crucial quantum-mechanical feature of electron-nuclear correlation, the projected nuclear quantum momenta, essential to…
Asymmetric molecules look different when viewed from one side or the other. This difference influences the electronic structure of the valence electrons, thereby giving stereo sensitivity to chemistry and biology. We show that attosecond…
This tutorial presents the most important aspects of the molecular self-probing paradigm, which views the process of high harmonic generation as "a molecule being probed by one of its own electrons". Since the properties of the electron…
High harmonic emissions from crystalline solids contain rich information on the dynamics of electrons driven by intense infrared laser fields and have been intensively studied owing to their potential use as a probe of microscopic…
We study high-order harmonic generation in aligned molecules close to the ionization threshold. Two distinct contributions to the harmonic signal are observed, which show very different responses to molecular alignment and ellipticity of…
We propose an approach to probe coherent spin-state dynamics of molecules using circularly polarized hard x-ray pulses. For the dynamically aligned nitric oxide molecules in a coherent superposition spin-orbit coupled electronic state that…
High-harmonic spectroscopy driven by circularly-polarized laser pulses and their counter-rotating second harmonic is a new branch of attosecond science which currently lacks quantitative interpretations. We extend this technique to the…
We characterize both entanglement and quantum coherence in a molecular system by connecting the linear entropy of electronic-nuclear entanglement with Wigner-Yanase skew information measuring vibronic coherence and local quantum uncertainty…
We present the experimental and theoretical details of our recent published letter [Phys. Rev. Lett. 115. 123002] on synchronized high-harmonic and terahertz-wave spectroscopy (HATS) from nonadiabatically aligned nitrogen molecules in…
We study theoretically and experimentally the electronic relaxation of NO2 molecules excited by absorption of one ~400 nm pump photon. Semi-classical simulations based on trajectory surface hopping calculations are performed. They predict…