Efficient isolation of multiphoton processes and detection of collective resonances in dilute samples

@article{Bruder2015EfficientIO,
  title={Efficient isolation of multiphoton processes and detection of collective resonances in dilute samples},
  author={Lukas Bruder and Marcel Binz and Frank Stienkemeier},
  journal={Physical Review A},
  year={2015},
  volume={92},
  pages={053412}
}
A novel technique to sensitively and selectively isolate multiple-quantum coherences in a femtosecond pump-probe setup is presented. Detecting incoherent observables and imparting lock-in amplification, even weak signals of highly dilute samples can be acquired. Applying this method, efficient isolation of one- and two-photon transitions in a rubidium-doped helium droplet beam experiment is demonstrated and collective resonances up to fourth order are observed in a potassium vapor for the first… 
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References

SHOWING 1-8 OF 8 REFERENCES

Principles of Nonlinear Optical Spectroscopy

1. Introduction 2. Quantum Dynamics in Hilbert Space 3. The Density Operator and Quantum Dynamics in Liouville Space 4. Quantum Electrodynamics, Optical Polarization, and Nonlinear Spectroscopy 5.…

Phase-modulated electronic wave packet interferometry reveals high resolution spectra of free Rb atoms and Rb*He molecules.

The spectra of atomic Rb electronic states show a vastly enhanced sensitivity and spectral resolution when compared to conventional pump-probe wave packet interferometry and the feasibility of applying coherent multidimensional spectroscopy to dilute cold gas phase samples is demonstrated.

and F

  • Stienkemeier, “Phasemodulated electronic wave-packet interferometry reveals high resolution vibronic spectra of free Rb atoms and Rb*He molecules,”
  • 2015

Physics Reports 497

  • 1
  • 2010

Chemical Reviews 110

  • 6891
  • 2010

Nature 466

  • 1089
  • 2010

For simplicity, we consider only the phase of the signals, since it contains all relevant information

    Science 248

    • 73
    • 1990