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Physical review. B, Condensed matter

Signatures of Fano resonances in four-wave-mixing experiments

T. Meier, A. Schulze, P. Thomas, H. Vaupel, K. Maschke

Published May 15, 1995• 23 citations
Publisher

Abstract

Optical transitions into discrete levels coupled to an optically active continuum lead to asymmetrical Fano lines in the linear absorption spectra, reflecting interference between the excitation channels. We investigate the corresponding four-wave-mixing spectra for the nonlinear optical response within a model of noninteracting electrons. Our results show that four-wave-mixing experiments provide a useful tool to identify Fano resonances.

DOI
10.1103/physrevb.51.13977

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Optical transitions into discrete levels coupled to an optically active continuum lead to asymmetrical Fano lines in the linear absorption spectra, reflecting interference between the excitation channels. We investigate the corresponding four-wave-mixing spectra for the nonlinear optical response within a model of noninteracting electrons. Our results show that four-wave-mixing experiments provide a useful tool to identify Fano resonances.
Fano resonance is a well-celebrated weak-coupling phenomenon whereby a small interaction between a discrete and a continuum of excited states leads to an interference between the respective two transition amplitudes, resulting in an asymmetric line shape in the excitation spectra. We present the strong-coupling phase of the Fano's model where the interaction is localized in a region $\ensuremath{\xi}$ that is smaller than the collective coupling between the discrete state and the continuum. We explore the behavior of the excitation probability $\ensuremath{\sigma}$ as a function of $\ensuremath{\xi}$, the ratio of the bare transition amplitudes, and the energy of the discrete state. In the strong-coupling phase, the spectral function of the discrete state splits up and produces up to three complete destructive interferences or zeros of $\ensuremath{\sigma}$ along with ultrasharp features. We also find that the discrete state does not have to lie within the continuum to produce the well-known weak-coupling profiles of $\ensuremath{\sigma}$ as long as the collective coupling is strong enough. In addition, we consider a broadened state instead of a continuum and present a method that exactly treats such cases by explicitly including the source of the broadening---a weak coupling to the continuum of environment states---in the model.
Summary form only given.Fano resonances arise due to quantum mechanical coupling of a discrete state to a degenerate continuum. The line shape in optical absorption spectra is characterized by an intrinsic broadening of the line, strong asymmetry, and a reduced absorption at one side of the peak falling well below the pure continuum level. Intensive theoretical investigations predicted Fano resonances as a general feature of a large variety of low-dimensional semiconductors. We present the observation of Fano resonances in semiconductor superlattices (SL). In SL, discrete excitonic states of the Wannier-Stark ladder are in resonance with subband continua of lower ladder states. The coupling between discrete and continuous states is mediated by Coulomb interaction, which is also responsible for the formation of the discrete excitonic states. As a unique feature of Fano resonances in SL, the Fano coupling strength can be continuously changed in the experiment by tuning the applied electric field. We have also performed time-integrated four-wave-mixing experiments to investigate the influence of Fano coupling on the polarization decay of a Wannier-Stark exciton. We have been able to resolve the polarization decay of a Fano resonance in the time-integrated signal and to follow its changes with field.
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.
The scattering amplitude from a set of discrete states coupled to a continuum became known as the Fano profile, characteristic for its asymmetric line shape and originally investigated in the context of photoionization. The generality of the model and the proliferation of engineered nanostructures with confined states gives immense success to the Fano line shape, which is invoked whenever an asymmetric line shape is encountered. However, many of these systems do not conform to the initial model worked out by Fano in that (i) they are subject to dissipative processes and (ii) the observables are not entirely analogous to the ones measured in the original photoionization experiments. In this Letter, we work out the full optical response of a Fano model with dissipation. We find that the exact result for the excited population, Raman, Rayleigh, and fluorescence emission is a modified Fano profile where the typical line shape has an additional Lorentzian contribution. Expressions to extract model parameters from a set of relevant observables are given.
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.
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.