Terahertz photonics

Abstract:

The perovskite semiconductor, CsPbI₃, holds excellent promise for solar cell applications due to its suitable bandgap. However, achieving phase-stable CsPbI₃ solar cells with high power conversion efficiency remains a major challenge. Ruddlesden-Popper (RP) defects have been identified in a range of perovskite semiconductors, including CsPbI₃. However, there is limited understanding as to why they form or their impact on stability and photophysical properties. Here, the prevalence of RP defects is increased with increased Cs-excess in vapor-deposited CsPbI₃ thin films while  superior structural stability but inferior photophysical properties are observed. Significantly, using electron microscopy, it is found that the atomic positions at the planar defect are comparable to those of a free surface, revealing their role in phase stabilization. Density functional theory (DFT) calculations reveal the RP planes are electronically benign, however, antisites observed at RP turning points are likely to be malign. Therefore it is proposed that increasing RP planes while reducing RP turning points offers a breakthrough for improving both phase stability and photophysical performance. The formation mechanism revealed here can apply more generally to RP structures in other perovskite systems.

Abstract:

FAPbI₃ has emerged as a promising semiconductor for photovoltaic applications offering a suitable bandgap for single-junction cells and high chemical stability. However, device efficiency is negatively affected by intrinsic quantum confinement (QC) effects that manifest as additional peaks in the absorption spectra. Here, we show that aerosol-assisted crystallization is an effective method to improve crystallinity and suppresses regions exhibiting QC in FAPbI₃. We demonstrate that films with minimized QC effects exhibit markedly enhanced optoelectronic properties, such as higher charge-carrier mobilities and recombination lifetimes. Films crystallized under an aerosol solvent flow of either a mixture of <i>N</i>,<i>N</i>-dimethylformamide and dimethyl sulfoxide or methylammonium thiocyanate vapor displayed reduced charge-carrier recombination losses and improved diffusion lengths compared to those of thermally annealed control films. Our study indicates clear correlations between suppression of QC features in absorption spectra with optimization of crystallinity and mitigation of internal strain, highlighting pathways toward high-performance solar cells.

Abstract:

Nanoscale material systems are central to next-generation optoelectronic and quantum technologies, yet their development remains hindered by limited characterization tools, particularly at terahertz (THz) frequencies. Far-field THz spectroscopy techniques lack the sensitivity for investigating individual nanoscale systems, whereas in near-field THz nanoscopy, surface states, disorder, and sample-tip interactions often mask the response of the entire nanoscale system. Here, we present a THz resonance-amplified near-field spectroscopy technique that can detect subtle conductivity changes in isolated nanoscale systems─such as a single InAs nanowire─under ultrafast photoexcitation. By exploiting the spatial localization and resonant field enhancement in the gap of a bowtie antenna, our approach enables precise measurements of the nanostructures through shifts in the antenna resonant frequency, offering a direct means of extracting the system response, and unlocking investigations of ultrafast charge-carrier dynamics in isolated nanoscale and microscale systems.

Abstract:

In this paper, the study of a plasma diagnostic system based on the THz time domain spectroscopy technique is presented. Such a system could potentially probe a large part of the electromagnetic spectrum currently covered by several other diagnostics in a single measurement. This feature, keeping in mind the basic requirements for plasma diagnostics in nuclear fusion experiments, such as robustness and hard environment applicability, as well as durability and low maintenance, makes the diagnostic of great interest. A conceptual design of the THz-TDS diagnostic has been developed, starting from the well-established classical microwave and far infrared plasma diagnostics landscape. The physical constraints and required instrumental characteristics have been studied and are described in detail here, together with the solutions available for each type of plasma measurement. Specific experimental laboratory tests of the different experimental configurations have been carried out, evaluating the capacity and potential of the novel diagnostic, together with the instrumental constraint, within the diagnostic parameter space.