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Related Concept Videos

¹H NMR of Conformationally Flexible Molecules: Temporal Resolution00:52

¹H NMR of Conformationally Flexible Molecules: Temporal Resolution

At room temperature, the chair conformer of cyclohexane undergoes rapid ring flipping between two equivalent chair conformers at a rate of approximately 105 times per second. These two chair conformers are in equilibrium. The rapid ring flipping results in the interconversion of the axial proton to an equatorial proton and an equatorial to the axial proton. Such interconversions are too rapid and cannot be detected on the NMR timescale. Hence, the NMR spectrometer cannot distinguish between the...
¹H NMR of Labile Protons: Temporal Resolution01:10

¹H NMR of Labile Protons: Temporal Resolution

Protons bonded to heteroatoms such as nitrogen and oxygen exhibit a range of chemical shift values. This is due to the varying degree of hydrogen bonding between the proton and the heteroatom in other molecules. The extent of hydrogen bonding affects the electron density around the proton, thereby giving different chemical shift values for the protons in the proton NMR spectrum.
The –OH proton in alcohols typically appears in the range of δ 2 to 5 ppm but can vary depending on the specific...
Double Resonance Techniques: Overview01:12

Double Resonance Techniques: Overview

Double resonance techniques in Nuclear Magnetic Resonance (NMR) spectroscopy involve the simultaneous application of two different frequencies or radiofrequency pulses to manipulate and observe two distinct nuclear spins. One important application of double resonance is spin decoupling, which selectively suppresses coupling with one type of nucleus while observing the NMR signal from another nucleus, simplifying the spectrum and enhancing resolution.
Spin decoupling is usually achieved by...
NMR Spectrometers: Radiofrequency Pulses and Pulse Sequences01:17

NMR Spectrometers: Radiofrequency Pulses and Pulse Sequences

A pulse is a short burst of radio waves distributed over a range of frequencies that simultaneously excites all the nuclei in the sample. Upon passing a radio frequency pulse along the x-axis, the nuclei absorb energy corresponding to their Larmor frequencies and achieve resonance. This shifts the net magnetization vector from the z-axis toward the transverse plane. This angle of rotation of the magnetization vector, or the flip angle, is proportional to the duration and intensity of the pulse.
Two-Dimensional (2D) NMR: Overview01:12

Two-Dimensional (2D) NMR: Overview

The 1D NMR spectrum of large and complex molecules like natural products has complicated splitting patterns and overlapping signals, which can be easily interpreted using 2-dimensional (2D) NMR. Unlike 1D NMR, 2D NMR has two frequency axes that provide the coupling information between the nucleus A and nucleus B in a molecule. The process from which 2D spectra are obtained has four steps.
The first step is the preparation period, during which nucleus A is excited with a radiofrequency pulse.
2D NMR: Overview of Heteronuclear Correlation Techniques01:18

2D NMR: Overview of Heteronuclear Correlation Techniques

Heteronuclear correlation spectroscopy is an analytical technique that investigates the coupling between different types of nuclei, often a proton and an X-nucleus, such as carbon-13 or nitrogen-15. This method is commonly used in nuclear magnetic resonance (NMR) spectroscopy to gain insights into complex chemical compounds' structural and compositional aspects. A typical heteronuclear correlation spectrum displays X-nucleus chemical shifts on one axis and a proton spectrum on the other axis.

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Updated: Jun 28, 2026

Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization
08:22

Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization

Published on: August 6, 2018

Time-resolved dynamics in N2O4 probed using high harmonic generation.

Wen Li1, Xibin Zhou, Robynne Lock

  • 1JILA and Department of Physics, University of Colorado and National Institute of Standards and Technology, Boulder, CO 80309-0440, USA. wli@jila.colorado.edu

Science (New York, N.Y.)
|November 1, 2008
PubMed
Summary
This summary is machine-generated.

High harmonic generation reveals coupled electronic and nuclear dynamics in molecules. Vibrations in dinitrogen tetraoxide cause electron state-switching, leading to distinct light emission patterns.

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Area of Science:

  • Physical Chemistry
  • Quantum Dynamics
  • Molecular Spectroscopy

Background:

  • High harmonic generation (HHG) probes ultrafast electron dynamics in atoms and small molecules.
  • Understanding HHG in complex polyatomic molecules requires considering coupled electronic and nuclear motion.
  • Previous studies focused on simpler systems, leaving polyatomic molecular dynamics under intense fields less explored.

Purpose of the Study:

  • To investigate coupled electronic and nuclear dynamics in polyatomic molecules using high harmonic generation.
  • To elucidate the role of molecular vibrations in modulating electron recollision dynamics and HHG spectra.
  • To explore the involvement of multiple molecular orbitals in strong-field ionization and HHG of polyatomic molecules.

Main Methods:

  • Excitation of large amplitude vibrations in dinitrogen tetraoxide (N2O4) molecules.
  • High harmonic generation measurements to probe electron recollision dynamics.
  • Theoretical calculations to interpret the observed spectral modulations and electronic state populations.

Main Results:

  • Demonstrated that HHG can reveal coupled electronic and nuclear dynamics in polyatomic molecules.
  • Observed a vibrational state-switching mechanism in N2O4: tunnel ionization accesses the ground ionic state at outer turning points and the first excited state at inner turning points.
  • Identified bursts of HHG predominantly emitted at the outer turning point, attributed to suppressed emission from the excited ionic state.

Conclusions:

  • High harmonic generation is a powerful tool for studying ultrafast coupled electronic and nuclear dynamics in polyatomic molecules.
  • Molecular vibrations significantly influence electron recollision pathways and HHG emission characteristics.
  • Strong-field ionization and HHG in conformationally dynamic molecules involve the participation of multiple molecular orbitals.