Inadequate knowledge of the phase state of atmospheric particles represents a source of uncertainty in global climate and air quality models. Hygroscopic aqueous inorganic particles are often assumed to remain liquid throughout their atmospheric lifetime or only (re)crystallize at low relative humidity (RH) due to the kinetic limitations of efflorescence (salt crystal nucleation and growth from an aqueous solution). Here we present experimental observations of a previously unexplored heterogeneous nucleation pathway that we have termed "contact efflorescence," which describes efflorescence initiated by an externally located solid particle coming into contact with the surface of a metastable aqueous microdroplet. This study demonstrates that upon a single collision, contact efflorescence is a pathway for crystallization of atmospherically relevant aqueous particles at high ambient RH (≤80%). Soluble inorganic crystalline particles were used as contact nuclei to induce efflorescence of aqueous ammonium sulfate [(NH 4 ) 2 SO 4 ], sodium chloride (NaCl), and ammonium nitrate (NH 4 NO 3 ), with efflorescence being observed in several cases close to their deliquescence RH values (80%, 75%, and 62%, respectively). To our knowledge, these observations represent the highest reported efflorescence RH values for microdroplets of these salts. These results are particularly important for considering the phase state of NH 4 NO 3 , where the contact efflorescence RH (∼20-60%) is in stark contrast to the observation that NH 4 NO 3 microdroplets do not homogeneously effloresce, even when exposed to extremely arid conditions (<1% RH). Considering the occurrence of particle collisions in the atmosphere (i.e., coagulation), these observations of contact efflorescence challenge many assumptions made about the phase state of inorganic aerosol.efflorescence | coagulation | aerosol | climate | air quality N ucleation of the solid phase from a liquid solution (crystallization) is an important process in pharmaceuticals, manufacturing, and atmospheric science (1). In the atmosphere, the phase state and water content of particulate matter influences both heterogeneous chemistry and the aerosol direct and indirect effect on climate (2-6). Despite its importance, there is no comprehensive understanding of the phase state of atmospheric particulate, and the aerosol radiative forcing remains one of the largest uncertainties in climate predictions (6).A significant fraction of aqueous atmospheric aerosol contains soluble inorganics such as chlorides, sulfates, and nitrates that can undergo efflorescence, i.e., the process of salt crystallization and water evaporation. Efflorescence often occurs at a significantly lower relative humidity (RH) than the reverse process of deliquescence (2, 7-12). A potent example of this hydration hysteresis is demonstrated with ammonium nitrate (NH 4 NO 3 ), a hygroscopic component of atmospheric aerosol (9-11). NH 4 NO 3(s) crystals will deliquesce to form an aqueous droplet at ∼62% RH (T = 295 K) (13). However...