Both singlesource and dual-source precursor approaches (SSPA and DSPA) to binary semiconductors have been documented. [9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24][25][26][27] Such materials consist of elements from two groups such as IIB and VIA. The single-source precursors (SSPs) consist of the metallic and nonmetallic elements of the semiconductor constituents in a single molecule. [9][10][11][12][13][14] DSPA uses separated metallic-element and nonmetallic-element precursors, which commonly involve metal carboxylates (M(OOCR) n such as M = Zn, Cd, Pb, Cu, In) and phosphine chalcogenides (such as E = PHR 2 where E = S, Se, Te), [15][16][17][18][19][20][21][22][23][24][25][26][27] respectively. Despite the large number of recipes developed for the various colloidal semiconductor nanocrystals (NCs) in the past 20 years, there is still little understanding of their formation mechanisms. To realize the full potential of semiconductor materials, there is an urgent need to advance our mechanistic understanding. Filling this gap in our knowledge should have practical implications such as lowering the high temperature currently employed for syntheses and offering new avenues to optimize the design of low-temperature approaches to novel semiconductor nanomaterials.Recent evidence suggests that the formation of various binary semiconductor NCs by SSPAs and DSPAs may share analogous mechanisms. A DSPA to CdS quantumm dots (QDs) at 160 8C in tetradecane (CH 3 (CH 2 ) 12 CH 3 ) was reported from the reaction of cadmium stearate (Cd(OOCC 17 H 35 ) 2 ) and diphenylphosphine sulfide (S= PHPh 2 ). [25] DSAPs to E-based semiconductor QDs have become popular with metal carboxylates as cation precursors and diphenylphosphine chalcogenides E = PHPh 2 as anion precursors. [15][16][17][18][19][20][21][22][23][24][25][26][27] Astonishingly, the lack of a common formation mechanism is actually accompanied by the same 31 P NMR identification of RCOO-PPh 2 (R = C 17 H 33 99 ppm (3 in Scheme 1) or C 6 H 5 102 ppm) and Ph 2 P-PPh 2 (À14 ppm, 4) for the various DSPAs to PbSe, [18] CdSe, [19][20][21][22] ZnSe, [23,24] ZnS, [24] and ZnSeS, [24] together with C 17 H 33 COO-P(Se)Ph 2 (77 ppm, 5) for the Se-based NCs. [18,[21][22][23][24] Furthermore, the conversion of Se = PHPh 2 to diphenyldiselenophosphinate derivatives (ÀSeSePPh 2 ) has been documented. [18,19,22] For instance, [22] the formation of RCOOCdSeSePPh 2 (c) was proposed from a Cd(OA) 2 + Se=PHPh 2 reaction after the release of oleic acid (C 17 H 33 COOH or RCOOH, R = C 17 H 33 ) from (RCOO) 2 Cd(Se = PHPh 2 ) 2 (b) followed by diphenylphosphine (HPPh 2 or DPP) from RCOOCd(Se À PPh 2 )-(Se = PHPh 2 ) (d) through cleavage of the Se = P bond of the Se=PHPh 2 coordination arm.