High-quality ultra-thin films of niobium nitride (NbN) are developed by plasma-enhanced atomic layer deposition (PEALD) technique. Superconducting nanowire single-photon detectors (SNSPDs) patterned from this material exhibit high switching currents and saturated internal efficiencies over a broad bias range at 1550 nm telecommunication wavelength. Statistical analyses on hundreds of fabricated devices show near-unity throughput yield due to exceptional homogeneity of the films. The ALD-NbN material represents an ideal superconducting material for fabricating large single-photon detector arrays combining high efficiency, low jitter, low dark counts.Superconducting nanowire single-photon detectors (SNSPDs) 1,2 have gained widespread attention due to their excellent performances, including high efficiency 3-6 , fast speed 7,8 , exceptional timing jitter 9-11 and ultra-low dark count rates 12,13 . In addition, their suitability for on-chip integration with various nanophotonics circuits 14-23 as well as their photon number resolving 24-26 and spectral 27-29 resolving capability render them an ideal choice for applications in quantum optics, quantum communications and quantum information processing [30][31][32] .The SNSPD is typically a narrow nanowire (20 nm -150 nm width) patterned from an ultra-thin superconducting film (3-10 nm thickness) for absorbing incident photons. So far, two main classes of superconducting materials have been utilized to fabricate high-efficiency SNSPDs: (1) poly-crystalline nitride superconductors such as NbN 4,15,33 and NbTiN 5,16,34-36 ;(2) amorphous alloy superconductors, such as WSi 3,37 , MoSi 6,11,21,38,39 and MoGe 40 . Each of these two classes of materials has their advantages and drawbacks in photon detection. The amorphous films have smaller superconducting energy gap and lower electron density, which tends to create larger photon-excited hot spots in the nanowires and thus results in better saturated internal efficiency. The structural homogeneity due to the absence of grain boundaries in these films further enables the fabrication of large-area detector arrays without suffering from serious constrictions 41,42 . The drawback is their relatively lower superconducting transition temperature T c (< 5 K for thin films) which sets their operation temperature below 2.5 K in order to achieve saturated efficiency at 1550 nm wavelength 43 . Poly-crystalline Nb(Ti)N-based detectors, on the other hand, have higher T c , higher critical current, relatively improved jitter performance and more immunity to latching at high operation speed due to their shorter hot spot relaxation time [44][45][46] . Consequently, Nb(Ti)N was exploited in the recent demonstration of GHzcounting-rate detectors 7,8 and sub-3 ps timing jitter 9 .In this Letter, we show our development of high-quality NbN thin films by plasma-enhanced atomic layer deposition (PEALD) and their applications in SNSPDs fabrication. The fabricated detectors demonstrate broad saturated plateaus in the efficiency curves that are compara...