skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


Title: Wavelength dependence in strong field ionization of water
It has recently been shown that strong field multiple ionization of water depends on the duration and intensity of the laser pulse. While the polarizability of neutral water is isotropic, the polarizability of the molecular ions can be significant and evolve in time. If the molecular ions spend enough time in the field, dynamic alignment can reorient them and modify the yield of dissociating fragments as a function of angle relative to the polarization of the laser. Unbending motion is one way that the polarizability of the molecular ions increases. Here, we study strong field ionization of water in the long pulse regime where dynamic alignment and unbending are known to contribute at 800 nm, and we tune the laser wavelength to modify coupling between the states of the monocation. A resonance between the X and A states at 660 nm should excite the monocation and initiate unbending motion, but our results cannot be explained without considering the dynamics and structure of the dication and trication. To conduct these measurements, we utilize laser pulses with a duration of 40 fs and central wavelengths of 660 nm, 800 nm, and 1330 nm to multiply-ionize an effusive molecular beam of water. The resulting charged fragments are detected using a velocity map imaging apparatus. Our results provide additional clues about the strong field ionization of water. *M.B., G.A.M., A.J.H., N.P., and P.H.B. were supported by the National Science Foundation. A.J.H. was additionally supported under a Stanford Graduate Fellowship as the 2019 Albion Walter Hewlett Fellow. N.P. was additionally supported by the Hertz Foundation. R.F. was supported by the Department of Energy office of Basic Energy Science, Facilities Division.  more » « less
Award ID(s):
1806145
PAR ID:
10250347
Author(s) / Creator(s):
; ; ; ; ;
Date Published:
Journal Name:
52nd Annual Meeting of the APS Division of Atomic, Molecular and Optical Physics
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; (, International Conference on Ultrafast Phenomena 2022)
    Légaré, F.; Tahara, T.; Biegert, J.; Brixner, T.; Dudovich, N. (Ed.)
    We demonstrate an enhancement in the formation of D2O3+ as a consequence of field-free molecular dynamics following the strong-field multiple ionization of deuterated water via 6-fs 800-nm pulse pairs. 
    more » « less
  2. ; ; ; ; ; ; ; ; ; ; et al (, Optics Express)
    Absolute density measurements of low-ionization-degree or low-density plasmas ionized by lasers are very important for understanding strong-field physics, atmospheric propagation of intense laser pulses, Lidar etc. A cross-polarized common-path temporal interferometer using balanced detection was developed for measuring plasma density with a sensitivity of ∼0.6 mrad, equivalent to a plasma density-length product of ∼2.6 × 1013cm−2if using an 800 nm probe laser. By using this interferometer, we have investigated strong-field ionization yield versus intensity for various noble gases (Ar, Kr, and Xe) using 800 nm, 55 fs laser pulses with both linear (LP) and circular (CP) polarization. The experimental results were compared to the theoretical models of Ammosov-Delone-Krainov (ADK) and Perelomov-Popov-Terent’ev (PPT). We find that the measured phase change induced by plasma formation can be explained by the ADK theory in the adiabatic tunneling ionization regime, while PPT model can be applied to all different regimes. We have also measured the photoionization and fractional photodissociation of molecular (MO) hydrogen. By comparing our experimental results with PPT and MO-PPT models, we have determined the likely ionization pathways when using three different pump laser wavelengths of 800 nm, 400 nm, and 267 nm. 
    more » « less
  3. ; ; ; ; ; ; ; (, The Journal of Chemical Physics)
    The ionization of CO, CO+, and CO2+ are quantified in an ultrafast, strong laser field. Measurements were performed over the intensity range from 1014 to 1017 W cm−2. Across this span, the intensity-dependent ionization yields were quantified over eight orders of magnitude in the dynamic range. Both sequential and (e, 2e) nonsequential ionization processes were observed. We calculate the electron states for CO and its molecular ions interacting with a strong laser field using a traditional field-free approach, the single active electron approximation, and present the results for the all-electron interaction of CO with the laser field. By comparing the calculated ionization with the experimental yields, we determined that the electron wave function polarization and Stark shifts were accurately treated with an all-electron Hartree–Fock calculation. The calculated field–molecule interaction included the core electron polarizability, which is not captured using field-free or frozen-core single-electron approximation. 
    more » « less
  4. ; ; ; ; ; ; ; ; ; ; et al (, Communications Chemistry)
    Abstract Filming atomic motion within molecules is an active pursuit of molecular physics and quantum chemistry. A promising method is laser-induced Coulomb Explosion Imaging (CEI) where a laser pulse rapidly ionizes many electrons from a molecule, causing the remaining ions to undergo Coulomb repulsion. The ion momenta are used to reconstruct the molecular geometry which is tracked over time (i.e., filmed) by ionizing at an adjustable delay with respect to the start of interatomic motion. Results are distorted, however, by ultrafast motion during the ionizing pulse. We studied this effect in water and filmed the rapid “slingshot” motion that enhances ionization and distorts CEI results. Our investigation uncovered both the geometry and mechanism of the enhancement which may inform CEI experiments in many other polyatomic molecules. 
    more » « less
  5. ; ; ; ; ; ; (, Physical Chemistry Chemical Physics)
    Laser-induced reduction of metal ions is attracting increasing attention as a sustainable route to ligand-free metal nanoparticles. In this work, we investigate the photochemical reactions involved in reduction of Ag + and [AuCl 4 ] − upon interaction with lasers with nanosecond and femtosecond pulse duration, using strong-field ionization mass spectrometry and spectroscopic assays to identify stable molecular byproducts. Whereas Ag + in aqueous isopropyl alcohol (IPA) is reduced through plasma-mediated mechanisms upon femtosecond laser excitation, low-fluence nanosecond laser excitation induces electron transfer from IPA to Ag + . Both nanosecond and femtosecond laser excitation of aqueous [AuCl 4 ] − produce reactive chlorine species by Au–Cl bond homolysis. Formation of numerous volatile products by IPA decomposition during both femtosecond and nanosecond laser excitation of [AuCl 4 ] − is attributed to enhanced optical breakdown by the Au nanoparticle products of [AuCl 4 ] − reduction. These mechanistic insights can inform the design of laser synthesis procedures to improve control over metal nanoparticle properties and enhance byproduct yields. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email