Transition quadrupole moments, Qt, of two ultrahigh-spin, collective structures in 154Er have been measured for the first time using the Doppler Shift Attenuation Method (DSAM). Data were acquired at the ATLAS accelerator facility of Argonne National Laboratory, using the Gammasphere detector array. A thick, gold-backed 110Pd foil was bombarded by a beam of 48Ti ions at 215 MeV. The Qt for each band was determined from the Doppler shift of gamma rays emitted by the resulting recoil nuclei. The extracted transition quadrupole moments are significantly different in magnitude, suggesting the two structures in 154Er represent distinct exotic nuclear shapes, namely axial superdeformed (SD) with Q t 20 eb, and triaxial strongly deformed (TSD) with Qt ≈ 11 eb. Indeed, the results calibrate the quadrupole moments of TSD bands recently measured in light erbium nuclei, 157,158Er
