A general approach is introduced for the efficient simultaneous optimization of pulses that compensate each otherʼs imperfections within the same scan. This is applied to Ramsey-type experiments for a broad range of frequency offsets and scalings of the pulse amplitude, resulting in pulses with significantly shorter duration compared to individually optimized broadband pulses. The advantage of the cooperative pulse approach is demonstrated experimentally for the case of two-dimensional nuclear Overhauser enhancement spectroscopy. In addition to the general approach, a symmetry-adapted analysis of the optimization of Ramsey sequences is presented. Furthermore, the numerical results led to the disovery of a powerful class of pulses with a special symmetry property, which results in excellent performance in Ramsey-type experiments. A significantly different scaling of pulse sequence performance as a function of pulse duration is found for characteristic pulse families, which is explained in terms of the different numbers of available degrees of freedom in the offset dependence of the associated Euler angles.Sequences of coherent and well-defined pulses play an important role in the measurement and control of quantum systems. Applications of control pulses include nuclear magnetic resonance (NMR) and electron spin resonance (ESR) spectroscopy [1,2], magnetic resonance imaging (MRI) [3], metrology [4], quantum information processing [5] and atomic, molecular and optical (AMO) physics in general [7,8]. Typically, pulse sequences are defined in terms of ideal pulses with unlimited amplitude and negligible duration (hard pulse limit). In practice, ideal pulses can often be approximated by rectangular pulses of finite duration, during which the phase is constant and the amplitude is set to the maximum available value. However, simple rectangular pulses are only able to excite spins with relatively small detunings (offset frequencies) that are in the order of the maximum pulse amplitude (expressed in terms of the Rabi frequency of the pulse) [9,10]. For broadband applications, e.g. in NMR, ESR or optical spectroscopy with a large range of offset frequencies or highly inhomogeneous line widths, the performance of simple rectangular pulses is not satisfactory and improved performance can be achieved by using shaped or composite pulses [9,[11][12][13].Depending on the application, experimental limitations and imperfections that need to be taken into account include (a) limited pulse amplitude due to amplifier constraints, (b) limited pulse energy in order to reduce heating effects, which are of particular concern in medical applications [3], (c) scaling of the pulse amplitudes due to errors in pulse calibration or due to the spatial inhomogeneity of the control field [9, 14, 15], (d) amplitude and phase transients [16][17][18] and (e) noise on the control amplitude [19,20]. Many different approaches have been used to optimize robust pulses [9,[11][12][13][21][22][23][24][25][26][27][28][29][30]. In addition to pulse imperfect...