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Physical Review Letters

Resonant Perfect Absorption Yielded by Zero-Area Pulses

Yu He, Zuoye Liu, Christian Ott, Adrian Nikolaus Pfeiffer, Shaohua Sun, Mette B. Gaarde, Thomas Pfeifer, Bitao Hu

Published Dec 28, 2022• 15 citations
Publisher

Abstract

We propose and study the manipulation of the macroscopic transient absorption of an ensemble of open two-level systems via temporal engineering. The key idea is to impose an ultrashort temporal gate on the polarization decay of the system by transient absorption spectroscopy, thus confining its free evolution and the natural reshaping of the excitation pulse. The numerical and analytical results demonstrate that even at moderate optical depths, the resonant absorption of light can be reduced or significantly enhanced by more than 5 orders of magnitude relative to that without laser manipulation. The achievement of the quasicomplete extinction of light at the resonant frequency, here referred to as resonant perfect absorption, arises from the full destructive interference between the excitation pulse and its subpulses developed and tailored during propagation, and is revealed to be connected with the formation of zero-area pulses in the time domain.

DOI
10.1103/physrevlett.129.273201

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We propose and study the manipulation of the macroscopic transient absorption of an ensemble of open two-level systems via temporal engineering. The key idea is to impose an ultrashort temporal gate on the polarization decay of the system by transient absorption spectroscopy, thus confining its free evolution and the natural reshaping of the excitation pulse. The numerical and analytical results demonstrate that even at moderate optical depths, the resonant absorption of light can be reduced or significantly enhanced by more than 5 orders of magnitude relative to that without laser manipulation. The achievement of the quasicomplete extinction of light at the resonant frequency, here referred to as resonant perfect absorption, arises from the full destructive interference between the excitation pulse and its subpulses developed and tailored during propagation, and is revealed to be connected with the formation of zero-area pulses in the time domain.
The concept of resonant perfect absorption, enabled by the combined action of pulse propagation and an auxiliary gate pulse, was recently proposed and demonstrated in a group of two-level systems [Y. He , ]. Here we exploit this method in a more realistic scenario by solving the coupled time-dependent Schrödinger equation and the Maxwell wave equation in helium. Through emptying the population of the 1s2p excited state after its excitation, we explore the evolution of the spectral profile with time delay and propagation distance and link the observations to the controlled interference between the original field and the gated new field. We find that resonant absorption for higher-lying states can also be strongly enhanced, in spite of the congestion of multiple resonances and the presence of complex laser-induced couplings. Our results show that interferometric control of absorption using intense laser fields can be applied selectively in both the temporal and spatial domains. Published by the American Physical Society 2024
An ultrashort strong nonresonant pulse induces transient phenomena in an optically thick medium consisting of an ensemble of nondegenerate two-level atoms (nonadiabatic transitions, transient light-shifts,\dots{}). A weak resonant pulse propagates in the system and we study theoretically and numerically the temporal and spectral modifications that are induced. Moreover, we show that the atomic media, modified by a strong pulse can act as a ``pulse-shaper'' device that can modify, in a controlled way, the shape of the weak pulse. It maps out the transient light shift induced by the strong pulse and reduces efficiently the long time dispersion tail of the weak pulse. We study and discuss the physical phenomena that allow such shaping effects and the necessary conditions to satisfy in order to observe them.
We report theoretical and experimental studies of the propagation of a square-modulated laser pulse through a laser-cooled atomic ensemble of two-level absorbers, as well as through a three-level system with electromagnetically induced transparency. We find that the transmission characteristics over a wide range of optical depth can be fully accounted for as optical coherent transients excited by the wide spectral content of the square-modulated optical pulse. We show that both time-domain atom-field coupled equations and frequency-domain linear dispersion theory give precisely the same description of the optical transients at a weak power limit. At low optical depth with moderate absorption, resonant excitation dominates and free-induction decay (FID) contributes mostly to the transient field. At high optical depth when absorption and propagation effects become significant, lossless optical precursors start to dominate the transient response. By varying the optical depth from 0 to 45, we observe that optical transients evolve gradually from FID to optical precursors. We thus show that FID and optical precursors, which have been considered as two different optical transients for many decades, can be unified within a single theoretical frame and they are the manifestations of the same physical process in two different regimes.
We explore the connection between adiabatic rapid passage, a technique that allows for robust complete population transfer (CPT) in a resonant absorber, and self-induced transparency solitons. We employ the auxiliary differential equation finite-difference time-domain method to fully resolve the dynamics of femtosecond light pulses propagating through an absorbing two-level medium. Using the example of linearly chirped Gaussian pulses we find that the pulses achieving robust CPT for a single two-level system are also pulses that will transform into solitary waves when incident on a resonantly absorbing medium. At the entrance into the absorber strongly chirped, adiabatic pulses completely transfer the electronic population from the ground to the upper state. As the pulses suffer absorption they undergo a dynamic transition and quickly split into an off-resonant radiation part and one or several unchirped solitary pulses that may carry away some of the initially achieved population inversion. This spectral and temporal transformation process limits the spatial depths of the region of CPT in a dense absorber regardless of the initial pulse amplitude. We also show that the frequency-domain pulse area, defined as the spectral amplitude at the resonance frequency, allows for a better distinction between the regimes of $2\ensuremath{\pi}$-pulse and $0\ensuremath{\pi}$-pulse formation than time-domain measurements.
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).
Propagation and amplification of an ultrashort laser pulse in a two-level medium is numerically investigated with the use of the finite-difference time-domain (FDTD) procedure simultaneously solving Maxwell and Schrodinger equations with no assumptions characteristic of slowly varying envelope approximation. Comparison of the results of FDTD numerical simulations with the predictions of the pulse area theorem has demonstrated that the developed numerical procedure provides an adequate description of pulse evolution in a two-level medium. Amplification of ultrashort light pulses in a two-level medium is analyzed. Two methods of improving the gain of ultrashort pulses in a two-level medium by modulating the spatial distribution of dipole moments of resonant transitions and using initially chirped frequency-detuned pulses are explored.