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EPJ Web of Conferences

Temporal and spectral evolution of an interrupted virtual single-photon transition: creation of optical gain and loss

Jens Herrmann, M. Weger, Reto Locher, Mazyar Sabbar, P. Rivière, Ulf Saalmann, Jan Michael Rost, L. Gallmann, Ursula Keller

Published Jan 1, 2013• 0 citations
Publisher

Abstract

We examine the optical response of a virtual dipole transition of a quantum mechanical two-level system (TLS). In the case of off-resonant excitation the time-integrated dipole response (TIDR) is expected to be zero, which corresponds to transparency of the system with respect to the exciting pulse. Our new time-frequency representation reveals that even for a zero TIDR there are positive and negative contributions included in the response. Furthermore, we present a way to access these contributions by using a second electromagnetic field, which interrupts the temporal evolution of the dipole response. The theoretical results are confirmed by attosecond transient absorption spectroscopy in helium (He).

DOI
10.1051/epjconf/20134102024

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Physical Review Letters•Oct 26, 2018•51 citations
We examine the optical response of a virtual dipole transition of a quantum mechanical two-level system (TLS). In the case of off-resonant excitation the time-integrated dipole response (TIDR) is expected to be zero, which corresponds to transparency of the system with respect to the exciting pulse. Our new time-frequency representation reveals that even for a zero TIDR there are positive and negative contributions included in the response. Furthermore, we present a way to access these contributions by using a second electromagnetic field, which interrupts the temporal evolution of the dipole response. The theoretical results are confirmed by attosecond transient absorption spectroscopy in helium (He).
The temporal evolution of the dipole response of a system excited by an electromagnetic field usually is not accessible with traditional spectroscopy. Only the time-integrated dipole response (TIDR) is detected. Here, we investigate the case of the off-resonant excitation of a quantum-mechanical two-level system (TLS) where the TIDR is expected to be zero. Our time-frequency representation of the dipole response reveals that even in this case positive and negative contributions are present during its temporal evolution. The zero TIDR is a result of the exact balance of positive and negative contributions, which cancel out. We present a way to create and control optical gain and loss by interrupting the evolution of the dipole in time. In this way, we make these nonzero contributions accessible for spectroscopy.
The response of matter to an optical excitation consists essentially of absorption and emission. Traditional spectroscopy accesses the frequency-resolved and time-integrated response, while the temporal evolution stays concealed. However, we will demonstrate here that the temporal evolution of a virtual single-photon transition can be mapped out by a second pulsed electromagnetic field. The resulting optical signal shows optical gain and loss, which can be gated and controlled via the relative delay of the electromagnetic fields.
Abstract This work is dedicated to the generalization of the spectroscopic correspondence principle to the time dependence of the evolution of a dipole-allowed quantum transition in a two-level system (TLS) under the action of an electromagnetic pulse (EMP). The formulas for the time dependence of the absorbed EMP energy for excitation of a classical oscillator and an oscillator of a transition in a TLS are derived within the framework of the first order of perturbation theory. It is shown that in the case of zero width of a transition line (or in case of zero damping constant γ for a classical oscillator) classical and quantum approaches give the same results for arbitrary EMP parameters (duration and carrier frequency). A noticeable distinction between the time dependences of the absorbed energy for a classical oscillator and a quantum TLS with a Lorentz spectral profile is observed for sufficiently long pulses.
In this work, the strong-field-modified dipole response at the ionization threshold of helium is studied. The dipole response is induced by an attosecond pulse in the extreme ultraviolet spectral range and is manipulated by an ultrashort and strong femtosecond pulse in the near-infrared. To probe the response, the transient absorption spectrum of helium is recorded for different time delays between both pulses and different intensities of the femtosecond pulse. From the spectra, the dipole response of the ionization threshold is reconstructed, which is linked to the dynamics of excited electrons with energies in the transition region from bound to free. To identify the underlying processes of light-matter interaction leading to the observed structures in the time and spectral domain, different quantum-mechanical model simulations are conducted. As a result, the measured dipole response reveals light-induced energy shifts of the photoelectron’s kinetic energy close to the parent ion, signatures for field-driven recollisions of a photoelectron into the parent ion, and a temporal amplitude and phase gating mechanism. With the latter, the build-up dynamics of complex spectral structures are temporally resolved, which are the time-dependent separation and line-shape modification of the doubly excited Rydberg series as well as the temporal build-up of the ionization threshold.
The reconstruction of the full temporal dipole response of a strongly driven time-dependent system from a single absorption spectrum is demonstrated, only requiring that a sufficiently short pulse is employed to initialize the coherent excitation of the system. We apply this finding to the time-domain observation of Rabi cycling between doubly excited atomic states in the few-femtosecond regime. This allows us to pinpoint the breakdown of few-level quantum dynamics at the critical laser intensity near 2 TW/cm^{2} in doubly excited helium. The present approach unlocks single-shot real-time-resolved signal reconstruction across timescales down to attoseconds for nonequilibrium states of matter. In contrast to conventional pump-probe schemes, there is no need for scanning time delays in order to access real-time information. The potential future applications of this technique range from testing fundamental quantum dynamics in strong fields to measuring and controlling ultrafast chemical and biological reaction processes when applied to traditional transient-absorption spectroscopy.