Colloidal semiconductor nanocrystals, also known as colloidal quantum dots (QDs), have been proven scientifically and technologically important enough to win the Nobel Prize in Chemistry. Their light absorption and emission wavelengths or energies can be tuned by tailoring their sizes. The colloidal phase of QDs allows their solution processability and deposition on various substrates, allowing the fabrication of thin-film devices such as field effect transistors (FETs) and integrated circuits, photodetectors, and light emitting diodes (LEDs). II-VI and IV-VI QDs, such as Cd chalcogenides and Pb and Hg chalcogenides, have been well-studied for visible and infrared applications, respectively. Still, the toxicity of their heavy metal cations has limited their use in consumer electronics due to the Restrictions of Hazardous Substances (RoHS) directive. III-V colloidal QDs have emerged as an alternative composition to the Cd, Pb, and Hg containing QDs, and InP QDs are integrated and commercialized in Samsung QLED TVs. The covalent bond between the group III and V elements makes III-V QDs less susceptible to degradation in polar environments than more ionic II-VI and IV-VI QDs. III-V QDs are particularly interesting since large QDs absorb and emit light in the short-wavelength infrared (SWIR) beyond the bandgap of Si. To practically leverage the properties of III-V QDs for devices, the growth mechanism, surface chemistry, and photophysics of III-V QDs must be uncovered. In this thesis, we first study the size- and shape-dependent growth of large tetrahedral colloidal InAs QDs, that absorb SWIR radiation, and investigate the effects of chemical modification of the QD surface in assemblies. We employ large InAs QDs as the absorber layers of proof-of-concept SWIR photodetectors. These core-only InAs QDs have negligible photoluminescence at room temperature (RT). Thus, we investigate shelling of the InAs QDs by ZnSe or InP and then ZnSe to yield RT SWIR-emitting InAs/ZnSe and InAs/InP/ZnSe core-shell QDs with petal-like and uniform ZnSe shells. The photophysics of the core-shell QDs is examined to analyze the effect of the InP buffer layer in relieving the lattice strain between InAs and ZnSe and forming electronically passivating shells. Finally, the InAs QDs are deposited and chemically modified on p-Si substrates to show the viability of p-Si/n-InAs QD heterojunction SWIR photodiodes, compatible with integration on current Si semiconductor technology and circuits.