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.
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.
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.
Ultrafast laser pulses with broad bandwidth can simultaneously excite multiple quantum states, forming coherent superpositions. The phases of the associated optical transitions evolve in time, giving rise to spectral line profiles that range from symmetric Lorentzian to asymmetric Fano-like forms. Yet, the line shape relations between different transitions within such superpositions remain largely unexplored. Here, we use transient absorption spectroscopy to probe transitions from coherent superpositions. While each transition’s line profile evolves over time, the relative line shape relations between different transitions remain fixed. We identify 4 fundamental types of line shape relations, each producing distinct spectral signatures. These relations naturally arise from second-order perturbation processes and can be actively tuned via the laser–matter interaction strength. Our findings establish a pathway for line shape-engineered control across atomic and molecular systems.
Ott et al. (Science (340, 716 (2013)) successfully transferred Fano profile into Lorentzian lineshape using an intense infrared laser, after excitation of autoionizing states in helium by attosecond XUV pulse. This is a very important step forward of 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 perturbed by the laser fields. Our result implies that excitation of the state through different paths can lead to different Fano profiles for the same resonant state. This allows more options for the combination of laser fields and lead to more opportunities for quantum phase control. Our result also indicates the breakdown of the classical two step picture for dielectronic recombination.
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.
Based on the laser-induced-phase model, periodic quantum phase modulation of the dipole response in atomic He is studied theoretically. The two-level system of the transition 1s2→1s2p with a delay width of 1.8 × 109 s-1 and an energy difference of 21.2 eV between the excited state and the ground state is used in the calculation. The system is excited by attosecond laser pulse from high harmonic generator, and the spectral response of the system is of single isolated symmetric Lorentzian absorption line. After the excitation, near infrared (NIR) femtosecond laser pulse train with a repetition rate of 5 GHz, central frequency 780 nm, and pulse duration of 100 fs, is utilized to periodically modify the spontaneous decay of the excited 1s2p level. The incremental phase step Δφ depends on the intensity of the NIR laser pulse, while the initial offset phase φ can be controlled independently by partially overlapping the first NIR pulse with the excitation. Simulated results show that the Lorentzian absorption line is transformed into comb-like spectral structure with equal gap depending on the repetition rate of the NIR pulse train. The line shape of each comb tooth is symmetric Lorentzian line by setting φ = Δφ/2 = π/2, while it is Fano line by setting φ = Δφ = π. The location of the comb structure is mainly dependent on the energy difference between the excited state and the ground state, while it can be slightly tuned by controlling the incremental phase step Δφ. We develop an analytic description of the comb-like spectral structure by Fourier analysis, depending on both the atomic and the phase-control properties. The analytical expressions can be readily used to estimate the exact experimental parameters. The universality of this mechanism allows the spectral modulation in arbitrary atomic system at arbitrary frequency, including the hard X-ray regime, by using reference transitions in highly charged ions. The generalization of this approach should thus not only enable relative frequency measurement and relevant applications at extremely high frequencies, but also open the way for pulse shaping at arbitrary frequencies.
The attosecond pump-femtosecond probe technique is widely used in electron dynamics research, with temporal resolution reaching tens of attoseconds. Here, we propose a scheme for controlling the Fano line shapes of helium doubly excited states by replacing the pump source with a pair of time-delayed attosecond pulses. We show that the interference induced by this delay provides an additional, highly effective means of controlling electron dynamics, enabling temporal resolution on the zeptosecond scale. We demonstrate that the corresponding line shapes in transient absorption spectra can shift dramatically within a time-delay variation of just a few hundred zeptoseconds. This extreme spectral modulation occurs under two key conditions: (i) when the time delay aligns with the spectral minimum of the coherently combined attosecond pulses in the frequency domain, and (ii) when the delay between the infrared probe pulse and the first attosecond pulse is held constant. This approach opens a new pathway to zeptosecond-scale control in quantum systems and demonstrates the powerful synergy between phase manipulation in both light and electron waves for achieving ultrafast spectral transformations.