Pulse design is critical for impulse radio communications, as it determines the transmission efficiency with respect to regulation spectral limits. In this paper, we propose the design of several novel pulse shapes relying on combinations of Gaussian derivatives with the target of improving the spectral efficiency. A general model for maximizing the efficiency of dual and triplet couplings is presented, employing the interior point global optimization algorithm. Then, the spectrum peak frequency is derived in closed form for any combination of two Gaussians with consecutive orders of derivation. The parameters controlling the time properties of the generated waveforms have been adequately adjusted to reach the best compliance with the spectral mask. Novel pulses have been investigated providing a high efficiency using simple generation mechanisms, which can be practically implemented via analog circuits. Results demonstrated the advantage of the proposed pulse shapes in terms of the bit error rate performance for 2 Gbps OOK and 1 Gbps PPM in AWGN and multipath channels.