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International Conference on Ultrafast Phenomena

Coherent Control In Ultrafast Photon Echo Spectroscopy: Liouville-Space Pathways Interference

Maxim S. Pshenichnikov, Wim P. de Boeij, Douwe A. Wiersma

Published Jan 1, 1996• 0 citations
Publisher

Abstract

Dephasing-induced resonances, arising from interference between different excitation pathways, are well-known in frequency-domain spectroscopy.[1] It is generally thought that the time-domain analog of this phenomena is difficult to achieve due to the explicit time ordering of the interaction fields.[2,3] In this contribution we report on the observation of time-domain interference in phase-locked stimulated photon echo. We also show how complete control over the interference effect can be exercised.

DOI
10.1364/up.1996.fe.29

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Optics Express•Mar 25, 2011•6 citations
Dephasing-induced resonances, arising from interference between different excitation pathways, are well-known in frequency-domain spectroscopy.[1] It is generally thought that the time-domain analog of this phenomena is difficult to achieve due to the explicit time ordering of the interaction fields.[2,3] In this contribution we report on the observation of time-domain interference in phase-locked stimulated photon echo. We also show how complete control over the interference effect can be exercised.
We demonstrate coherent control over interference between different Liouville-space pathways that describe the generation of the nonlinear optical polarization in a stimulated photon echo. This control was exercised by phase-locking of the excitation pulses and observed in the heterodyne detected echo signal. A theoretical analysis of the effect is presented and found to be in good agreement with the obtained results. The relation between this novel time-domain interference effect and the pressure-induced extra resonance in four-wave mixing spectroscopy is discussed.
A novel interference effect in transient four-wave mixing is demonstrated. The phenomenon is based on phase-controlled Liouville-space pathways interference and observed in the heterodyne-detected stimulated photon echo. Changing the phase difference between the first two excitation pulses from $\ensuremath{\pi}/2$ to 0 leads from no signal to maximum echo signal. A Brownian oscillator dynamical model is successfully used to analyze the effect and simulate the experimental data. The relation between this time-domain interference effect and dephasing-induced resonance in four-wave mixing spectroscopy is elaborated.
We extend a recently formulated coherence spectroscopy of dissipative media [J. Chem. Phys. 122, 084502 (2005)] from the stationary excitation limit to the time domain. Our results are based on analytical and numerical solutions of the quantum Liouville equation within the Bloch framework. It is shown that the short pulse introduces a new, controllable time scale that allows better insight into the relation between the coherence signal and the phase properties of the material system. We point to the relation between the time-domain coherence spectroscopy and the method of interferometric two-photon photoemission spectroscopy, and propose a variant of the latter method, where the two time-delayed excitation pathways are distinguishable, rather than identical. In particular, we show that distinguishability of the two excitation pathways introduces the new possibility of disentangling decoherence from population relaxation.
Weak-field coherent phase control of atomic non-resonant multiphoton excitation induced by shaped femtosecond pulses is studied theoretically in the single-cycle regime. The carrier-envelope phase (CEP) of the pulse, which in the multi-cycle regime does not play any control role, is shown here to be a new effective control parameter that its effect is highly sensitive to the spectral position of the ultrabroad spectrum. Rationally chosen position of the ultrabroadband spectrum coherently induces several groups of multiphoton transitions from the ground state to the excited state of the system: transitions involving only absorbed photons as well as Raman transitions involving both absorbed and emitted photons. The intra-group interference is controlled by the relative spectral phase of the different frequency components of the pulse, while the inter-group interference is controlled jointly by the CEP and the relative spectral phase. Specifically, non-resonant two- and three-photon excitation is studied in a simple model system within the perturbative frequency-domain framework. The developed intuition is then applied to weak-field multiphoton excitation of atomic cesium (Cs), where the simplified model is verified by non-perturbative numerical solution of the time-dependent Schrödinger equation. We expect this work to serve as a basis for a new line of femtosecond coherent control experiments.