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Commensurate two-quantum coherences induced by time-delayed THz fields.

Sharly Fleischer1, Robert W Field, Keith A Nelson

  • 1Department of Chemistry, Massachusetts Institute of Technology, Cambridge, 02139, USA.

Physical Review Letters
|September 26, 2012
PubMed
Summary

Two time-delayed terahertz (THz) pulses significantly enhance molecular rotational coherences in carbonyl sulfide gas. This effect, observed experimentally and theoretically, can also occur with a single THz pulse if multiple molecular species are present.

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Area of Science:

  • Physical Chemistry
  • Molecular Spectroscopy
  • Quantum Dynamics

Background:

  • Molecular rotational coherences are fundamental to understanding molecular dynamics.
  • Terahertz (THz) pulse interactions with molecules offer unique insights into rotational energy levels.
  • Controlling molecular coherences is key for advanced spectroscopic techniques.

Purpose of the Study:

  • To investigate the induction and enhancement of two-quantum rotational coherences in carbonyl sulfide (COS) using time-delayed THz pulses.
  • To explore the role of pulse delay and molecular species in coherence enhancement.
  • To demonstrate a general mechanism for coherence generation applicable to complex molecular systems.

Main Methods:

  • Experimental application of two time-delayed, single-cycle THz pulses to carbonyl sulfide gas.
  • Theoretical modeling to analyze the induced two-quantum rotational coherences.
  • Spectroscopic observation of free induction decay (FID) from atmospheric water vapor as a secondary interaction source.

Main Results:

  • Two time-delayed THz pulses significantly enhance two-quantum rotational coherences compared to a single pulse.
  • The degree of enhancement is dependent on the relative delay between the two THz pulses.
  • The phenomenon was shown to be general, occurring with a single THz pulse when multiple molecular species are present, utilizing FID from one species to interact with another.

Conclusions:

  • Time-delayed THz pulse sequences provide a powerful method for enhancing molecular rotational coherences.
  • The findings offer a new pathway for controlling and probing molecular quantum dynamics.
  • The demonstrated generality of the phenomenon opens possibilities for advanced spectroscopy of complex gas mixtures.