Azimul Haque

CH3NH3PbCl3 Single Crystals: Inverse Temperature Crystallization and Visible-Blind UV-Photodetector

Single crystals of hybrid perovskites have shown remarkably improved physical properties compared to their polycrystalline film counterparts, underscoring their importance in the further development of advanced semiconductor devices. Here we present a new method of growing sizable CH3NH3PbCl3 single crystals based on the retrograde solubility behavior of hybrid perovskites. We show, for the first time, the energy band structure, charge recombination, and transport properties of CH3NH3PbCl3 single crystals. These crystals exhibit trap-state density, charge carrier concentration, mobility, and diffusion length comparable with the best quality crystals of methylammonium lead iodide or bromide perovskites reported so far. The high quality of the crystal along with its suitable optical band gap enabled us to build an efficient visible-blind UV-photodetector, demonstrating its potential in optoelectronic applications.

High-Performance Ultraviolet-to-Infrared Broadband Perovskite Photodetectors Achieved via Inter-/Intraband Transitions

A high-performance vertically injected broadband UV-to-IR photodetector based on Gd-doped ZnO nanorods (NRs)/CH3NH3PbI3 perovskite heterojunction was fabricated on metal substrates. Our perovskite-based photodetector is sensitive to a broad spectral range, from ultraviolet to infrared light region (λ = 250-1357 nm). Such structure leads to a high photoresponsivity of 28 and 0.22 A/W, for white light and IR illumination, respectively, with high detectivity values of 1.1 × 1012 and 9.3 × 109 Jones. Optical characterizations demonstrate that the IR detection is due to intraband transition in the perovskite material. Metal substrate boosts carrier injection, resulting in higher responsivity compared to the conventional devices grown on glass, whereas the presence of Gd increases the ZnO NRs performance. For the first time, the perovskite-based photodetector is demonstrated to extend its detection capability to IR (>1000 nm) with high room temperature responsivity across the detected spectrum, leading to a high-performance ingenious cost-effective UV-to-IR broadband photodetector design for large-scale applications.

Effects of High Temperature and Thermal Cycling on the Performance of Perovskite Solar Cells: Acceleration of Charge Recombination and Deterioration of Charge Extraction

In this work, we investigated the effects of high operating temperature and thermal cycling on the photovoltaic (PV) performance of perovskite solar cells (PSCs) with a typical mesostructured (m)-TiO2-CH3NH3PbI3-xClx-spiro-OMeTAD architecture. After temperature-dependent grazing-incidence wide-angle X-ray scattering, in situ X-ray diffraction, and optical absorption experiments were carried out, the thermal durability of PSCs was tested by subjecting the devices to repetitive heating to 70 °C and cooling to room temperature (20 °C). An unexpected regenerative effect was observed after the first thermal cycle; the average power conversion efficiency (PCE) increased by approximately 10% in reference to the as-prepared device. This increase of PCE was attributed to the heating-induced improvement of the crystallinity and p doping in the hole transporter, spiro-OMeTAD, which promotes the efficient extraction of photogenerated carriers. However, further thermal cycles produced a detrimental effect on the PV performance of PSCs, with the short-circuit current and fill factor degrading faster than the open-circuit voltage. Similarly, the PV performance of PSCs degraded at high operation temperatures; both the short-circuit current and open-circuit voltage decreased with increasing temperature, but the temperature-dependent trend of the fill factor was the opposite. Our impedance spectroscopy analysis revealed a monotonous increase of the charge-transfer resistance and a concurrent decrease of the charge-recombination resistance with increasing temperature, indicating a high recombination of charge carriers. Our results revealed that both thermal cycling and high temperatures produce irreversible detrimental effects on the PSC performance because of the deteriorated interfacial photocarrier extraction. The present findings suggest that the development of robust charge transporters and proper interface engineering are critical for the deployment of perovskite PVs in harsh thermal environments.

A Photodetector Based on p-Si/n-ZnO Nanotube Heterojunctions with High Ultraviolet Responsivity

Enhanced ultraviolet (UV) photodetectors (PDs) with high responsivity comparable to that of visible and infrared photodetectors are needed for commercial applications. n-Type ZnO nanotubes (NTs) with high-quality optical, structural, and electrical properties on a p-type Si(100) substrate are successfully fabricated by pulsed laser deposition (PLD) to produce a UV PD with high responsivity, for the first time. We measure the current-voltage characteristics of the device under dark and illuminated conditions and demonstrated the high stability and responsivity (that reaches ∼101.2 A W-1) of the fabricated UV PD. Time-resolved spectroscopy is employed to identify exciton confinement, indicating that the high PD performance is due to optical confinement, the high surface-to-volume ratio, the high structural quality of the NTs, and the high photoinduced carrier density. The superior detectivity and responsivity of our NT-based PD clearly demonstrate that fabrication of high-performance UV detection devices for commercial applications is possible.

Embedding 1D Conducting Channels into 3D Isoporous Polymer Films for High-Performance Humidity Sensing

Isoporous block copolymer (BCP) films have received exponential interest as highly selective membranes, stemming from their unique morphological features, but their applications in functional devices remain to be realized. Now single-walled carbon nanotubes (CNTs) were efficiently incorporated into isoporous block copolymer films for chemiresistive sensing at room temperature. Leveraging the efficient charge extraction ability of CNTs together with nanochannel arrays aligned perpendicular to the surface of the films, an ultrafast response time of 0.3 s was achieved for humidity detection with a sensor response of about 800 on changing humidity from 10 % to 95 %. Furthermore, the sensor also responds to various organic vapors, underscoring its promising detection capability.

Overcoming the Ambient Manufacturability‐Scalability‐Performance Bottleneck in Colloidal Quantum Dot Photovoltaics

Colloidal quantum dot (CQD) solar cells have risen rapidly in performance; however, their low-cost fabrication under realistic ambient conditions remains elusive. This study uncovers that humid environments curtail the power conversion efficiency (PCE) of solar cells by preventing the needed oxygen doping of the hole transporter during ambient fabrication. A simple oxygen-doping step enabling ambient manufacturing irrespective of seasonal humidity variations is devised. Solar cells with PCE > 10% are printed under high humidity at industrially viable speeds. The devices use a tiny fraction of the ink typically needed and are air stable over a year. The humidity-resilient fabrication of efficient CQD solar cells breaks a long-standing compromise, which should accelerate commercialization.