Herein, we report the first solution-processed broadband photodetectors to break the past compromise between sensitivity and speed of response. Specifically, we report photodiodes having normalized detectivity (D*) > 1012 Jones and a 3dB bandwidth of > 2.9 MHz. This finding represents a 170,000 fold improvement in response speed over the most sensitive colloidal quantum dot (CQD) photodetector reported1 and a 100,000 fold improvement in sensitivity over the fastest CQD photodetector reported2. At the outset of this study, sensitive, solution-processed IR photodetectors were severely limited by low response speeds1. Much faster response speeds had been demonstrated by solution-processed photodetectors operating in the visible3, but these devices offered no benefits for extending the spectral sensitivity of silicon. No available solution-processed photodetector combined high sensitivity, high operating speed, and response to illumination across the UV, visible and IR. We developed a fast, sensitive, solution-processed photodetector based on a photodiode formed by a Schottky barrier to a CQD film. Previous attempts to form sensitive photodetectors based on CQD photodiodes had demonstrated low quantum efficiencies that limited sensitivity4,5. Efficient, sensitive semiconductor photodiodes are based on two fundamental characteristics: a large built-in potential that separates photogenerated charge carriers and minimizes internal noise generation, and high semiconductor conductivity for efficient collection of photogenerated charge. Schottky barriers to CQD films were developed to provide high, uniform built-in potentials. A multi-step CQD ligand exchange procedure was developed to allow deposition of tightly packed films of CQDs with high mobility and sufficiently well-passivated surfaces to form high-quality metallurgical junctions. The temporal response of the CQD photodiodes showed separate drift and diffusion components. Combined with detailed measurements of the Schottky barrier, these characteristics provided the physical basis for a numerical model of device operation. Based on this understanding, devices that excluded the slow diffusive component were fabricated, exploiting only the sub-microsecond field-driven transient to achieve MHz response bandwidth. These devices are the first to combine megahertz-bandwidth, high sensitivity, and spectral-tunability in photodetectors based on semiconducting CQDs. Record performance is achieved through advances in materials and device architecture based on a detailed understanding the physical mechanisms underlying the operation of CQD photodiodes.

Herein, we report the first solution-processed broadband photodetectors to break the past compromise between sensitivity and speed of response. Specifically, we report photodiodes having normalized detectivity (D*) > 1012 Jones and a 3dB bandwidth of > 2.9 MHz. This finding represents a 170,000 fold improvement in response speed over the most sensitive colloidal quantum dot (CQD) photodetector reported1 and a 100,000 fold improvement in sensitivity over the fastest CQD photodetector reported2. At the outset of this study, sensitive, solution-processed IR photodetectors were severely limited by low response speeds1. Much faster response speeds had been demonstrated by solution-processed photodetectors operating in the visible3, but these devices offered no benefits for extending the spectral sensitivity of silicon. No available solution-processed photodetector combined high sensitivity, high operating speed, and response to illumination across the UV, visible and IR. We developed a fast, sensitive, solution-processed photodetector based on a photodiode formed by a Schottky barrier to a CQD film. Previous attempts to form sensitive photodetectors based on CQD photodiodes had demonstrated low quantum efficiencies that limited sensitivity4,5. Efficient, sensitive semiconductor photodiodes are based on two fundamental characteristics: a large built-in potential that separates photogenerated charge carriers and minimizes internal noise generation, and high semiconductor conductivity for efficient collection of photogenerated charge. Schottky barriers to CQD films were developed to provide high, uniform built-in potentials. A multi-step CQD ligand exchange procedure was developed to allow deposition of tightly packed films of CQDs with high mobility and sufficiently well-passivated surfaces to form high-quality metallurgical junctions. The temporal response of the CQD photodiodes showed separate drift and diffusion components. Combined with detailed measurements of the Schottky barrier, these characteristics provided the physical basis for a numerical model of device operation. Based on this understanding, devices that excluded the slow diffusive component were fabricated, exploiting only the sub-microsecond field-driven transient to achieve MHz response bandwidth. These devices are the first to combine megahertz-bandwidth, high sensitivity, and spectral-tunability in photodetectors based on semiconducting CQDs. Record performance is achieved through advances in materials and device architecture based on a detailed understanding the physical mechanisms underlying the operation of CQD photodiodes.