Wetc hemical screening reveals the very high reactivity of Mo(NMe 2 ) 4 with H 2 Sf or the low-temperature synthesis of MoS 2 .This observation motivated an investigation of Mo(NMe 2 ) 4 as av olatile precursor for the atomic layer deposition (ALD) of MoS 2 thin films.H erein we report that Mo(NMe 2 ) 4 enables MoS 2 film growth at recordl ow temperatures-as lowas608 8C. The as-deposited films are amorphous but can be readily crystallized by annealing.I mportantly,t he low ALD growth temperature is compatible with photolithographic and lift-off patterning for the straightforwardfabrication of diverse device structures.Stimulated by the landmark discovery of two-dimensional (2D) monolayer graphene [1] and the vast body of subsequent work delineating the rich physical phenomena associated with the electronic structure of graphene, [2] interest has expanded to the exploration of inorganic graphene-analogous 2D materials. [3] Central to this family of materials are 2D layered transition metal dichalcogenides,MX 2 (M = Mo,W;X= S, Se, Te ), [4] themost notable of which is MoS 2 .Whereas graphene is az ero-band-gap-energy conductor,M oS 2 is al ayered semiconductor with athickness-dependent optical band gap in the range of 1.2-1.8 eV. [5] Mono-and few-layer MoS 2 have been demonstrated to possess properties [6] suitable for awide range of electronic [7] and optoelectronic [8] applications,a nd more recently for valleytronics [9] and spintronics. [10] Additionally, 2D MoS 2 has been utilized for battery, [11] gas, [12] and biosensor applications, [13] and extensively for catalytic hydrodesulfurization [14] and hydrogen evolution processes. [15,16] It is thus not surprising that MoS 2 has in recent years become one of the most intensely studied subjects in materials chemistry and materials science. [17] To date,awide range of synthetic approaches to monoand few-layer MoS 2 have been reported;t hese include hydrothermal [18] and electrochemical synthesis, [19] thermolysis of Mo-and S-containing species, [20] sulfurization of Mo-containing seed layers, [12,21] micromechanical [7b, 22] and liquid exfoliation of bulk MoS 2 , [23] as well as physical [24] and chemical vapor deposition [25] (PVD and CVD,r espectively). [26] The most commonly employed methods,e xfoliation and CVD, have,h owever, significant limitations.T op-down methods such as exfoliation can suffer from solvent contamination and ultimately yield collections of discrete flakes rather than continuous films.Bottom-up approaches such as CVD,while promising for MoS 2 film growth on solid supports,o ften require high volatilization/reaction temperatures which limit substrate scope and patterning techniques such as photolithography. [26] Thep recise,l arge-scale growth of mono-or few-layer MoS 2 on insulating substrates would enable the scalable fabrication of atomically thin high-performance transistors,p hotodetectors,a nd other desirable products on at echnologically relevant scale;t his currently represents asignificant challenge. [4,25c] Atomic layer d...