2 Few other areas of study have uncovered the secrets of the universe like that of the interaction between light and matter, leading to many revolutionary scientific discoveries. The interaction of light, in particular with semiconducting materials, has enabled us to understand the behaviour of various fundamental phenomena and has laid the foundation of the optoelectronic systems that we rely on today. The majority of such systems necessitate the detection of light which is achieved via the use of photodetector devices. A photodetector converts incident photons into an electrical signal, which in the solid-state, is assembled together with an application-oriented readout integrated circuit (ROIC). Present-day commercially available photodetectors are typically made from gallium phosphide/silicon carbide (GaP)/(SiC), silicon (Si) and indium gallium arsenide/germanium (InGaAs)/(Ge) for detection in the ultraviolet (UV), visible and near-infrared (IR) regimes of the electromagnetic spectrum, respectively. For mid and far IR, lead sulphide (PbS), lead selenide (PbSe), indium antimonide (InSb), indium arsenide (InAs) and mercury cadmium telluride (HgCdTe) based photodetectors are commonly used. Photodetectors based on a photoemissive principle such as photomultiplier tubes (PMTs) are also widely used for ultrasensitive detection in the UV to near-IR spectral regime and are fabricated using alkali metals having a low workfunction. For applications demanding multispectral detection, 'two-colour' detectors are often manufactured with a bi-level structure, for example consisting of an IR transmitting Si photodiode mounted over an IR sensitive PbS photoconductor. Such a device structure has drawbacks that include added cost, increased complexity of device fabrication and associated issues in implementation. Furthermore, a significant majority of applications are based upon UV to near-IR light detection where the indirect bandgap of Si, the InGaAs epitaxial growth process, PMT bulkiness and high bias voltage requirement all present challenges and renders their use with flexible platforms impossible. As a result significant research effort continues to be expended on the development of a singlesystem multispectral photodetector to replace two or more detectors. In the last decade amongst all the candidate materials studied 1 PbS semiconductor nanocrystals (NCs), often referred as 'quantum dots', have emerged as the most promising material for the fabrication of 3 this type of photodetector. Such has been the progress in their development that reported PbS NC based photodetectors have already outperformed conventional state-of-the-art photodetectors in many aspects including low-cost room temperature device fabrication via solution processing, flexible substrate compatibility, broadband spectral sensitivity along with the figures of merit achieved, Fig 1a. In this review article, we present an overview of recent developments in PbS NC based photodetectors. We first provide a brief introduction to PbS NCs and their releva...

Understanding the interactions between photoexcited charge carriers (electrons and holes) with lattice vibrations (phonons) in quantum confined semiconductor nanocrystals (NCs) is of fundamental interest and a prerequisite for their use in fabricating high-performance optoelectronic devices. Such interactions have a significant impact on their optoelectronic properties including their charge carrier mobility and photoluminescence. Here, we investigate these interactions in cesium lead halide (CsPbX 3 , where X is Cl, Br or I) NC perovskites. We show that a wide broadening of the excitonic linewidth in these NCs arises from strong exciton-phonon coupling, which is substantially dominated by longitudinal optical phonons via the Fröhlich interaction. Unlike the behavior of conventional semiconductors these NCs display a general red-shift of their emission energy peak with reducing temperature. Interestingly, the CsPbCl 3 NCs also display an initial blue-shift and undergo at structural phase transition at ~175 K to 200 K. The anomalous red-shift observed is modeled and analyzed using a Bose-Einstein two-oscillator model to interpret the interaction of excitons with acoustic and optical phonons which induce a renormalization of the bandgap. The net renormalization due to zero point motion (T= 0 K) was found to be ~41.6 meV and ~94.9 meV for CsPbBr 3 and CsPbI 3 NCs respectively.

One dimensional single-crystal nanorods of C60 possess unique optoelectronic properties including high electron mobility, high photosensitivity and an excellent electron accepting nature. In addition, their rapid large scale synthesis at room temperature makes these organic semiconducting nanorods highly attractive for advanced optoelectronic device applications. Here, we report low-cost large-area flexible photoconductor devices fabricated using C60 nanorods. We demonstrate that the photosensitivity of the C60 nanorods can be enhanced ~400-fold via an ultralow photodoping mechanism. The photodoped devices offer broadband UV-vis-NIR spectral tuneability, exhibit a detectivitiy >109 Jones, an external quantum efficiency of ~100%, a linear dynamic range of 80 dB, a rise time 60 µs and the ability to measure ac signals up to ~250 kHz. These figures of merit combined are among the highest reported for one dimensional organic and inorganic large-area planar photoconductors and are competitive with commercially available inorganic photoconductors and photoconductive cells. With the additional processing benefits providing compatibility with large-area flexible platforms, these devices represent significant advances and make C60 nanorods a promising candidate for advanced photodetector technologies.

Hybrid PbS nanocrystal/C 60 fullerite photodetectors are fabricated using a simple one-step drop casting procedure onto pre-patterned interdigitated electrodes. The devices exhibit a broad spectral response from the near UV through to the near infrared yielding a detectivity, D * , of above 10 10 Jones from 400 nm to ≈ 1050 nm. The ability to further extend the spectral response to wavelengths ≈ 1350 nm in the near infrared via tuning of the PbS nanocrystal diameter is also demonstrated. The dynamic responses of the devices are presented, exhibiting a fast photocurrent rise time ( < 40 ns) followed by a long bi-exponential decay with characteristic lifetimes of τ 1 = 5.3 μ s ± 0.1 μ s and τ 2 = 37.8 μ s ± 0.7 μ s. These devices, which have a detectivity approaching that of commercial detectors, a broader spectral response, and a fast rise time, offer an attractive low-cost solution for large-area broadband photodetectors.

Visible spectrum photodetector devices fabricated using molecular crystals of carbon C are reported. The devices operate efficiently, extending over and beyond the full visible light spectrum (300-710 nm) with a bias voltage tunable responsivity of 4 mA-0.5 mA W . Across this range of wavelengths, the noise equivalent power of these devices remains below 10 nW Hz , providing a detectivity of 10 Jones. The noise current in these devices is found to have a strong dependence on both bias voltage and frequency, varying by 4 orders of magnitude from 1 nA Hz to 0.1 pA Hz . The devices also display a near-linear dependence of photocurrent on light intensity over 4 orders of magnitude, providing a dynamic range approaching 80 dB. The 3 dB bandwidth of the devices is found to be above 10 Hz, while the 18 dB bandwidth exceeds 1 kHz. The transient photocurrents of the devices have a rise time of ≈50 µs and a long fall time of ≈4 ms. The spectral photocurrent of the devices is found to quench gradually with a reduction in temperature from ≈300 K and is fully quenched at temperatures below T ≈ 100 K. Upon reheating, the device performance is fully recovered.