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Optics Express

Selective ultrafast control of multi-level quantum systems by subcycle and unipolar pulses

Rostislav M. Arkhipov, A. V. Pakhomov, Mikhail V. Arkhipov, Ayhan Demircan, Uwe Morgner, Nikolay N. Rosanov, Ihar Babushkin

Published Apr 22, 2020• 72 citations
Publisher

Abstract

The most typical way to optically control population of atomic and molecular systems is to illuminate them with radiation, resonant to the relevant transitions. Here we consider a possibility to control populations with the subcycle and even unipolar pulses, containing less than one oscillation of electric field. Despite the spectrum of such pulses covers several levels at once, we show that it is possible to selectively excite the levels of our choice by varying the driving pulse shape, duration or time delay between consecutive pulses. The pulses which are not unipolar, but have a peak of electric field of one polarity much higher (and shorter) than of the opposite one, are also capable for such control.

DOI
10.1364/oe.393142

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The most typical way to optically control population of atomic and molecular systems is to illuminate them with radiation, resonant to the relevant transitions. Here we consider a possibility to control populations with the subcycle and even unipolar pulses, containing less than one oscillation of electric field. Despite the spectrum of such pulses covers several levels at once, we show that it is possible to selectively excite the levels of our choice by varying the driving pulse shape, duration or time delay between consecutive pulses. The pulses which are not unipolar, but have a peak of electric field of one polarity much higher (and shorter) than of the opposite one, are also capable for such control.
Based on an approximate solution of the Schrödinger equation, the effect that a pair of extremely short small-amplitude subcycle pulses has on a quantum system is studied. It is shown that, if the pulses are shorter than the inverse frequencies of atomic transitions, the probability of transitions between levels is determined by the electric area of the pulses and the time delay between them. As a consequence, a unipolar pulse can more efficiently affect the system than a bipolar one, while a sequence of pulses realizes a selective action on quantum objects, despite a nonresonant character of the interaction.
We theoretically demonstrate the possibility of coherent control of the response of a multilevel resonant medium by means of half-cycle unipolar or quasi-unipolar attosecond pulses. We show that despite the ultrabroad spectrum of half-cycle pulses the induced medium polarization can be efficiently steered through the proper choice of the parameters for the excitation pulses. Besides, we found that the response of a multilevel medium for the amplitude of driving subcycle pulses below a certain threshold can be quantitatively well approximated by the two-level model.
Abstract The possibility of selective population of the energy levels of quantum systems using a single unipolar subcycle pulse and a pair of pulses has been studied. The possibility of selective population of quantum levels has been clearly illustrated based on the numerical solution of a system of equations for the density matrix of a three-level medium that interacts with a pair of subcycle attosecond and terahertz pulses. The possibility of creating a population inversion in a three-level medium using a pair of such pulses has been shown. The dynamics of population gratings in a three-level medium exposed to the action of a pair of Gaussian pulses of large amplitude on the system is studied. Whereas the shape of the gratings in a weak field is harmonic, according to analytical calculations performed by the perturbation theory, in the case of a strong field, the spatial profile of the gratings may differ from the sinusoidal profile and may have a complex structure of peaks.
We theoretically demonstrate the possibility to tune the temporal waveform of optical unipolar pulses upon their coherent interaction with a multi-level resonant medium. This is achieved through the coherent control of the response of a multi-level resonant medium by means of half-cycle unipolar pulses. We show that despite the ultrabroad spectrum of half-cycle pulses one can efficiently steer the induced medium polarization through the proper choice of the parameters of the excitation pulses. As the result, producing of unipolar optical pulses of varying profile, like rectangular or triangular ones, from an extended layer of a multi-layer medium was obtained when excited by a pair of half-cycle pulses. Besides, we find out that the response of a multi-level medium for the amplitude of the driving pulses below a certain threshold can be quantitatively well approximated by the two-level model.
We study theoretically a possibility of creation and ultrafast control (erasing, spatial frequency multiplication) of population density gratings in a multi-level resonant medium having a resonance transition frequency in the THz range. These gratings are produced by subcycle THz pulses coherently interacting with a nonlinear medium, without any need for pulses to overlap, thereby utilizing an indirect pulse interaction via an induced coherent polarization grating. High values of dipole moments of the transitions in the THz range facilitate low field strength of the needed THz excitation. Our results clearly show this possibility in multi-level resonant media. Our theoretical approach is based on an approximate analytical solution of time-dependent Schrödinger equation (TDSE) using perturbation theory. Remarkably, as we show here, quasi-unipolar subcycle pulses allow more efficient excitation of higher quantum levels, leading to gratings with a stronger modulation depth. Numerical simulations, performed for THz resonances of the [Formula: see text] molecule using Bloch equations for density matrix elements, are in agreement with analytical results in the perturbative regime. In the strong-field non-perturbative regime, the spatial shape of the gratings becomes non-harmonic. A possibility of THz radiation control using such gratings is discussed. The predicted phenomena open novel avenues in THz spectroscopy of molecules with unipolar and quasi-unipolar THz light bursts and allow for better control of ultra-short THz pulses.