The magneto-optical polarization rotation effect has prolific applications in various research areas spanning the scientific spectrum including space and interstellar research, nano-technology and material science, biomedical imaging, and sub-atomic particle research. In nonlinear magnetooptical rotation (NMOR), the intensity of a linearly-polarized probe field affects the rotation of its own polarization plane while propagating in a magnetized medium. However, typical NMOR signals of conventional single-beam Λ−scheme atomic magnetometers are peculiarly small, requiring sophisticated magnetic shielding under complex operational conditions. Here, we show the presence of an energy-symmetry blockade that undermines the NMOR effect in conventional single-beam Λ−scheme atomic magnetometers. We further demonstrate, both experimentally and theoretically, an inelastic wave-mixing technique that breaks this NMOR blockade, resulting in more than five orders of magnitude (>300,000-fold) NMOR optical signal power spectral density enhancement never before seen with conventional single-beam Λ−scheme atomic magnetometers. This new technique, demonstrated with substantially reduced light intensities, may lead to many applications, especially in the field of bio-magnetism and high-resolution low-field magnetic imaging.Magneto-optical effects arise when the different polarized components of an electrical field resonantly coupling to magnetic transitions of an atom experience different magnetic dichriosm [1][2][3]. When the effects become dependent on the intensity of the electric field itself, the resulting rotation of the polarization plane of the field is referred to as nonlinear magneto-optical rotation (NMOR). All polarimetry-based alkali metal vapor atomic magnetometers employ this principle for extremely weak magnetic field detection. Using spin relaxation management techniques [4][5][6][7][8][9][10][11][12][13], together with state-of-the-art magnetic shieldings and phase-locking detection electronics, atomic magnetometers have demonstrated extremely high sensitivities [8,[10][11][12][13][14][15] approaching the benchmark performance of superconducting quantum interference devices [16].The core element of polarimetry-based alkali vapor atomic magnetometers is a three-state atomic system [ Fig. 1(a)] coupling to a linearly polarized probe field [17][18][19][20][21][22]. Although the NMOR signal is enhanced by the probe intensity in this simple Λ-scheme, the NMOR optical signal-to-noise ratio (SNR) is generally low, requiring complex magnetic shielding and sophisticated electronics in addition to long data-acquisition times. Here, we introduce an optical inelastic wave-mixing (WM) process via a second light field counter-propagating with * Corresponding author:lu.deng@nist.gov respect to the probe field. This inelastic WM process opens a multi-excitation channel by sharing two fullyoccupied intermediate states [23][24][25] with the probe field. Consequently, it significantly modifies the ground-state Zeeman coherence and the ...