The rapid relaxation of above-band-gap “hot” carriers (HCs) imposes the key efficiency limit in lead-halide perovskite (LHP) solar cells. Recent studies have indicated that HC cooling in these systems may be sensitive to materials composition, as well as the energy and density of excited states. However, the key parameters underpinning the cooling mechanism are currently under debate. Here we use a sequence of ultrafast optical pulses (visible pump–infrared push–infrared probe) to directly compare the intraband cooling dynamics in five common LHPs: FAPbI3, FAPbBr3, MAPbI3, MAPbBr3, and CsPbBr3. We observe ∼100–900 fs cooling times, with slower cooling at higher HC densities. This effect is strongest in the all-inorganic Cs-based system, compared to the hybrid analogues with organic cations. These observations, together with band structure calculations, allow us to quantify the origin of the “hot-phonon bottleneck” in LHPs and assert the thermodynamic contribution of a symmetry-breaking organic cation toward rapid HC cooling.
Photoconductive antennas are promising sources of terahertz radiation that is widely used for spectroscopy, characterization, and imaging of biological objects, deep space studies, scanning of surfaces, and detection of potentially hazardous substances. These antennas are compact and allow for generation of both ultrabroadband pulses and tunable continuous wave terahertz signals at room temperatures, with no need for high‐power optical sources. However, such antennas have relatively low energy conversion efficiency of femtosecond laser pulses or two close pump wavelengths (photomixers) into the pulsed and continuous terahertz radiation, correspondingly. Recently, an approach to solving this problem that involves known methods of nanophotonics applied to terahertz photoconductive antennas and photomixers has been proposed. This approach comprises the use of optical nanoantennas for enhancing the absorption of pump laser radiation in the antenna gap, reducing the lifetime of photoexcited carriers, and improving the antenna thermal efficiency. This Review is intended to systematize the main results obtained by researchers in this promising field of hybrid optical‐to‐terahertz photoconductive antennas and photomixers. We summarize the main results on hybrid THz antennas, compare the approaches to their implementation, and offer further perspectives of their development including an application of all‐dielectric nanoantennas instead of plasmonic ones.
Carrier cooling is of widespread interest in the field of semiconductor science. It is linked to carrier-carrier and carrier-phonon coupling, and has profound implications for the photovoltaic performance of materials. Recent transient optical studies have shown that a high carrier density in lead-halide perovskites (LHPs) can reduce the cooling rate through a "phonon bottleneck".However, the role of carrier-carrier interactions, and the material properties that control cooling in LHPs, are still disputed. To address these factors, we utilize ultrafast "pump-push-probe" spectroscopy on LHP nanocrystal (NC) films. We find that the addition of cold carriers to LHP NCs increases the cooling rate, competing with the phonon bottleneck. By comparing different NCs and bulk samples, we deduce that the cooling behavior is intrinsic to the LHP composition, and independent of the NC size or surface. This can be contrasted with other colloidal nanomaterials, where confinement and trapping considerably influence the cooling dynamics.
Compact and tunable semiconductor terahertz sources providing direct electrical control, efficient operation at room temperatures and device integration opportunities are of great interest at the present time. One of the most well-established techniques for terahertz generation utilises photoconductive antennas driven by ultrafast pulsed or dualwavelength continuous wave laser systems, though some limitations, such as confined optical wavelength pumping range and thermal breakdown, still exist. The use of quantum dotbased semiconductor materials, having unique carrier dynamics and material properties, can help to overcome limitations and enable efficient optical-to-terahertz signal conversion at room temperatures. Here we discuss the construction of novel and versatile terahertz transceiver systems based on quantum dot semiconductor devices. Configurable, energy-dependent optical and electronic characteristics of quantum-dot-based semiconductors are described, and the resonant response to optical pump wavelength is revealed. Terahertz signal generation and detection at energies that resonantly excite only the implanted quantum dots opens the potential for using compact quantum dot-based semiconductor lasers as pump sources. Proof-ofconcept experiments are demonstrated here that show quantum dot-based samples to have higher optical pump damage thresholds and reduced carrier lifetime with increasing pump power.
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