Colloidal nanocrystals (NCs), especially lead sulfide NCs, are promising candidates for solution-processed next-generation photodetectors with high-speed operation frequencies. However, the intrinsic response time of PbS-NC photodetectors, which is the material-specific physical limit, is still elusive, as the reported response times are typically limited by the device geometry. Here, we use the two-pulse coincidence photoresponse technique to identify the intrinsic response time of 1,2-ethanedithiol-functionalized PbS-NC photodetectors after femtosecond-pulsed 1560 nm excitation. We obtain an intrinsic response time of ∼1 ns, indicating an intrinsic bandwidth of ∼0.55 GHz as the material-specific limit. Examination of the dependence on laser power, gating, bias, temperature, channel length, and environmental conditions suggest that Auger recombination, assisted by NC-surface defects, is the dominant mechanism. Accordingly, the intrinsic response time might further be tuned by specifically controlling the ligand coverage and trap states. Thus, PbS-NC photodetectors are feasible for gigahertz optical communication in the third telecommunication window.

We investigate the time-resolved photocurrent response of CdSe quantum dot (QD) thin films sensitized with zinc β-tetraaminophthalocyanine (Zn4APc) (Kumar et al., ACS Appl. Mater. Interfaces, 2019, 11, 48271-48280) on three different substrates, namely, silicon with 230 nm SiO 2 dielectric, glass, and polyimide. While Si/SiO 2 (230 nm) is not suitable for any transient photocurrent characterization due to an interfering photocurrent response of the buried silicon, we find that polyimide substrates invoke the larger optical bandwidth with 85 kHz vs 67 kHz for the same quantum dot thin film on glass. Upon evaluation of the transient photocurrent, we find that the photoresponse of the CdSe quantum dot films can be described as a combination of carrier recombination and fast trapping within 2.7 ns followed by slower multiple trapping events. The latter are less pronounced on polyimide, which leads to the higher bandwidth. We show that all devices are resistance-capacitance (RC)-time limited and that improvements of photoresistance are the key to further increasing the bandwidth.

We report an optically gated transistor composed of CdSe nanocrystals (NCs), sensitized with the dye zinc β-tetraaminophthalocyanine for operation in the first telecom window. This device shows a high ON/OFF ratio of 6 orders of magnitude in the red spectral region and an unprecedented 4.5 orders of magnitude at 847 nm. By transient absorption spectroscopy, we reveal that this unexpected infrared sensitivity is due to electron transfer from the dye to the CdSe NCs within 5 ps. We show by time-resolved photocurrent measurements that this enables fast rise times during near-infrared optical gating of 47 ± 11 ns. Electronic coupling and accelerated nonradiative recombination of charge carriers at the interface between the dye and the CdSe NCs are further corroborated by steady-state and time-resolved photoluminescence measurements. Field-effect transistor measurements indicate that the increase in photocurrent upon laser illumination is mainly due to the increase in the carrier concentration while the mobility remains unchanged. Our results illustrate that organic dyes as ligands for NCs invoke new optoelectronic functionalities, such as fast optical gating at sub-bandgap optical excitation energies.

We investigate the time-resolved photoelectric response of WSe2 crystals on glass and flexible polyimide substrates to determine the effect of a changed dielectric environment on the speed of the photodetectors....

Photoelectron spectroscopy was used to investigate electronic interface properties and interactions of the organic semiconductors CoPc and CoPcF16 on graphene/nickel based substrates. Additional focus was put on the influence of germanium intercalation of graphene/nickel. The presented results demonstrate that germanium can decouple graphene from nickel and in this manner restore its buffer layer properties. No charge transfer from the substrate to the organic layer is observed in the germanium intercalated case, while interface related peaks in the Co 2p core level spectra indicate such charge transfer on graphene/nickel. Strong interface dipoles are found for CoPcF16 on graphene/nickel and on germanium intercalated graphene/nickel. Fluorine Auger parameters have been measured, and the results provide evidence for polarization and charge transfer screening effects of different amounts at the unlike film-substrate interfaces. The various contributions to the observed shifts are discussed.