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

  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},
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… 

Figures from this paper

Coherent multidimensional spectroscopy in the gas phase

Recent work applying multidimentional coherent electronic spectroscopy at dilute samples in the gas phase is reviewed. The development of refined phase cycling approaches with improved sensitivity

Two-dimensional spectroscopy beyond the perturbative limit: The influence of finite pulses and detection modes.

This work employs non-perturbative time evolution to investigate the effects of finite pulse width and amplitude on 2DES signals and identifies key differences in the response of HD and FD detection schemes, as well as the regions of parameter space where the signal is obscured by unwanted artifacts in either technique.

Extending lock-in methods: term isolation detection of nonlinear signals.

It is shown that components of a nonlinear signal can be measured using phase-sensitive detection at unconventional demodulation frequencies, allowing the isolation of individual autocorrelation terms from the signal.

Coherent two-dimensional electronic mass spectrometry

This work introduces coherent 2D electronic mass spectrometry that allows 2D measurements on effusive molecular beams and thus on quantum systems with minimum system–bath interaction and employs this to identify the major ionization pathway of 3d Rydberg states in NO2.

Stable interferometric platform for phase modulation of seeded free-electron lasers.

We present a compact phase modulation setup designed for high laser intensities sufficient to drive highly nonlinear processes, such as high-gain harmonic generation in seeded free-electron lasers.

Advances in nonlinear spectroscopy using phase modulated light fields: prospective applications in perturbative and non-perturbative regimes

ABSTRACT Since its first implementation in 2006, in fluorescence detected Fourier transform excitation spectroscopy of rubidium atoms, phase modulation is being increasingly used in nonlinear

Incoherent population mixing contributions to phase-modulation two-dimensional coherent excitation spectra.

It is demonstrated that an incoherent contribution to the measured line shape, arising from nonlinear population dynamics over the entire photoexcitation lifetime, generates a similar line shape to the expected 2D coherent spectra in condensed-phase systems.

Rapid multiple-quantum three-dimensional fluorescence spectroscopy disentangles quantum pathways

3D population-based three-dimensional electronic spectroscopy is introduced and the extraction of all fourth- and multiple sixth-order nonlinear signal contributions are extracted by employing 125-fold phase cycling of a four-pulse sequence.

Communication: The origin of many-particle signals in nonlinear optical spectroscopy of non-interacting particles.

  • S. Mukamel
  • Physics
    The Journal of chemical physics
  • 2016
It is shown that signals that scale with higher powers of N are generated by the joint detection of several particles that can be accomplished by phase sensitive detection such as phase cycling, photo-acoustic modulation, or by Hanbury-Brown Twiss photon coincidence.

Frequency-Comb Based Double-Quantum Two-Dimensional Spectrum Identifies Collective Hyperfine Resonances in Atomic Vapor Induced by Dipole-Dipole Interactions.

This work uses double-quantum multidimensional coherent spectroscopy to reveal collective hyperfine resonances in rubidium vapor at 100 °C induced by dipole-dipole interactions.



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