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. © 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreement