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Optics Communications

Tuning optical spectrum between Fano and Lorentzian line shapes with phase control

Keyu Xia, Jian‐Qi Zhang

Published May 26, 2015• 6 citations
Publisher
DOI
10.1016/j.optcom.2015.05.042

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Symmetric Lorentzian and asymmetric Fano line shapes are fundamental spectroscopic signatures that quantify the structural and dynamical properties of nuclei, atoms, molecules, and solids. This study introduces a universal temporal-phase formalism, mapping the Fano asymmetry parameter q to a phase φ of the time-dependent dipole response function. The formalism is confirmed experimentally by laser-transforming Fano absorption lines of autoionizing helium into Lorentzian lines after attosecond-pulsed excitation. We also demonstrate the inverse, the transformation of a naturally Lorentzian line into a Fano profile. A further application of this formalism uses quantum-phase control to amplify extreme-ultraviolet light resonantly interacting with He atoms. The quantum phase of excited states and its response to interactions can thus be extracted from line-shape analysis, with applications in many branches of spectroscopy.
Spectroscopic signatures associated with symmetric Lorentzian and asymmetric Fano line shapes are ubiquitous. Distinct features of Fano resonances in contrast with conventional symmetric resonances have found several applications in photonics such as optical switching, sensing, lasing, and nonlinear and slow-light devices. It is therefore important to effectively generate and control these resonances. In this work, we show through ab initio simulations of coupled light–matter systems that Fano interference phenomena can be realized in a multimode photonic environment by strong coupling to the electromagnetic continuum. Specifically, we show that by effectively enhancing the light–matter coupling strength to the photon continuum in an experimentally feasible way, we can achieve a transition from Lorentzian to Fano lines shapes for both electronic and polaritonic excitations. An important outcome of switching between these spectral signatures is the possibility to control the Purcell enhancement of spontaneous emission alongside electromagnetically induced transparency, which is a special case of Fano resonances. Switching from Fano back to a Lorentzian profile can be achieved by physically reducing the coupling strength to the continuum of modes. Our results hold potential for realizing tunable Fano resonances of molecules and materials interacting with the electromagnetic continuum within multimode photonic environments.
The absorption spectrum of a bound state with a finite lifetime gives rise to the well-known Lorentzian line shape. This fundamental mechanism breaks down at high intensities. Here we demonstrate how even a single intense multicycle excitation pulse can result in Fano absorption profiles in the frequency domain. The intensity-dependent line shapes indicate the dipole responses are phase modulated by the single excitation pulse itself. Further, as the atomic density increases, we observe broader Fano-like shapes and the appearance of novel substructures in absorption lines. These are clear signatures of propagation effects in which collective interactions need to be taken into account. An analytical model is applied, which describes both effects observed in the experiment. Understanding the transition from optically dilute to dense medium is crucial to distinguish between single-atom and macroscopic effects.