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arXiv:1405.4279 · Physical Review Letters

Anomalous Fano Profiles in External Fields

Alejandro Zielinski, Vinay Pramod Majety, Stefan Nagele, Renate Pazourek, Joachim Burgdörfer, Armin Scrinzi

Published Dec 10, 2015• 20 citations
arXivHTMLPDF

Abstract

We show that the external control of Fano resonances in general leads to complex Fano q parameters. Fano line shapes of photoelectron and transient absorption spectra in the presence of an infrared control field are investigated. Computed transient absorption spectra are compared with a model proposed for a recent experiment [C. Ott et al., Science 340, 716 (2013)]. Control mechanisms for photoelectron spectra are exposed: control pulses applied during excitation modify the line shapes by momentum boosts of the continuum electrons. Pulses arriving after excitation generate interference fringes due to infrared two-photon transitions.

DOI
10.1103/physrevlett.115.243001

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We show that the external control of Fano resonances in general leads to complex Fano q parameters. Fano line shapes of photoelectron and transient absorption spectra in the presence of an infrared control field are investigated. Computed transient absorption spectra are compared with a model proposed for a recent experiment [C. Ott et al., Science 340, 716 (2013)]. Control mechanisms for photoelectron spectra are exposed: control pulses applied during excitation modify the line shapes by momentum boosts of the continuum electrons. Pulses arriving after excitation generate interference fringes due to infrared two-photon transitions.
Line shapes observed in attosecond transient absorption spectra (ATAS) encode information on the phase of the optical dipole response. Understanding and controlling the phase evolution of interference fringes is among the fundamental goals of exploring coherent interaction. Here, we simulate the attosecond transient absorption in the near-infrared (NIR) dressing field by considering a three-level model in the adiabatic approximation. We find that the absorption line shape can be changed from Lorentzian to Fano to inverted Lorentzian and back again at two-photon dressed energy levels “ω ± 2ωι”, and line shapes evolve in half-cycle periodicity (T/2). Moreover, the direction of phase evolution of “ω ± 2ωι” is opposite, while the phases of “ω ± 2ωι” are roughly the same at certain delays with an interval of approximately a quarter-cycle periodicity (T/4). These results demonstrate that absorbance of two-photon dressed energy levels “ω ± 2ωι” can qualitatively map the AC Stark shift. These observations provide new insights into the control of spectral line shapes and open the way for the modulation of quantum optical interference in the laser-driven atom.
Photon absorption spectroscopy is a powerful tool for uncovering the structure of atoms, molecules, and solids. Symmetric Lorentzian and asymmetric Fano line shapes are fundamental spectroscopic signatures related to the structural and dynamical properties. Recently, Ott et al. [Science 340, 716 (2013)] successfully transferred Fano profile into Lorentzian line shape using an intense infrared laser, after excitation of autoionizing states in helium by attosecond XUV pulse. This is a very important step forward in quantum phase control. However, here we show experimentally that an autoionizing state can have both Fano and Lorentzian behavior naturally, depending on the process involved. This study utilized the inverse process of photon absorption ionization, i.e., electron ion recombination with photon emission, making sure the resonant autoionizing state is not modified or decorated by the laser fields. Our result implies that excitation of the state through different paths---for example, one photon versus multiphoton excitation, or even one step versus multistep excitation---can lead to different Fano profiles for the same resonant state. We also report an experimental determination of the energy shifts in the recombination photon-intensity peaks due to the interference between the resonant and nonresonant processes.
We know that the Fano profile is obtained for single-photon absorption to the ionization continuum in the presence of an autoionizing state. We have shown that, in the case of (1+1)-photon absorption to an autoionizing state embedded in the ionization continuum, the absorption profile changes radically to a mirror image of the Fano profile for the value of q=\ifmmode\pm\else\textpm\fi{}1, q being the Fano q parameter. Moreover, for higher values of q, the (1+1)-photon absorption profile exhibits a broad minimum, while a distinct interference pattern is obtained in the profile of single-photon absorption. The absorption line shape has been found to oscillate between the Fano and a modified Fano profile for the autoionization through odd and even number of steps, respectively, via resonances.
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 Fano line shape arises from the interference of two excitation pathways to reach a continuum. Its generality has resulted in a tremendous success in explaining the line shapes of many one-dimensional spectroscopies---absorption, emission, scattering, conductance, photofragmentation---applied to very varied systems---atoms, molecules, semiconductors, and metals. Unraveling a spectroscopy into a second dimension reveals the relationship between states in addition to decongesting the spectra. Femtosecond-resolved two-dimensional electronic spectroscopy (2DES) is a four-wave mixing technique that measures the time evolution of the populations and coherences of excited states. It has been applied extensively to the dynamics of photosynthetic units, and more recently to materials with extended band structures. In this paper, we solve the full time-dependent third-order response, measured in 2DES, of a Fano model and give the system parameters that become accessible.