Type-tunable optical gain performance of core-seeded CdSe/CdS nanorods is studied via two-photon optical pumping. Controlling the Colloidal semiconductor nanocrystals have recently arisen as promising candidates to be utilized as active gain media for lasing applications. 1,2 With their band gap tunability (via size and shape modications), efficient band edge emission (even at room temperature), discrete band structure, and synthesis through facile wet-chemistry, it is possible to achieve colortunable, low-threshold, temperature insensitive and solution processed lasers from colloidal quantum dots (CQDs). [2][3][4][5][6] However, there are various problems and challenges associated with CQD-based lasers. One way of achieving stimulated emission from the CQDs is through multi-exciton generation. When multiple excitons are formed, the Auger recombination (AR) process becomes more pronounced and inhibits optical gain in CQDs. [7][8][9] In addition, high intensity optical pumping, which is required for stimulated emission, can photo-damage the sample and decrease the stability. 10 To address these issues, CQDs having suppressed AR and exhibiting a higher absorption cross-section, which can increase the stability of CQDs by lowering the optical gain threshold, are strongly required.As a subclass of nanocrystals, core/shell nanorods (NRs) have been extensively considered for lasing applications and optical gain studies to overcome these problems with possibility of engineering their electronic structure for longer gain lifetime and increased absorption cross-section. 11-14 From different varieties of core/shell NRs, core-seeded CdSe/CdS NRs have become quite attractive. With advances in the colloidal synthesis of CdSe/CdS core/shell NRs, it is possible to synthesize highly efficient and crystalline CdSe/CdS core/shell NRs having a narrow size distribution by nely controlling their shape and size. 15,16 Furthermore, due to shallow band offset for electrons in the CdSe/CdS core/shell material system, a partial separation of electron and hole wavefunctions is observed which is known as the quasi type-II electronic structure that contributes to the suppression of Auger recombination, which is highly critical for achieving lasing. 11,[16][17][18] The other advantage of having a lower energy barrier for electrons in CdSe/CdS NRs is that, by simply changing their core and shell sizes, it is possible to tailor the electron and hole wavefunction overlap and tune CdSe/CdS NRs from type-I-like to quasi-type-II-like band alignment, which can be an important design consideration when engineering the gain/loss mechanisms in practical lasing systems. [19][20][21][22][23] Moreover, due to the narrower band gap of CdS with respect to ZnS, the absorption cross-section of CdSe/CdS core/shell NRs is greatly enhanced. 13 With all of these aforementioned promises, in the nanocrystal lasing context, CdSe/CdS NRs have become one of the most heavily studied materials systems. 18,24 Recently, singlemode, single-exciton and tunable laser emis...