Inspired by the formulation of quantum-electrodynamical time-dependent density functional theory (QED-TDDFT) by Rubio and co-workers [Flick et al., ACS Photonics 6, 2757-2778 (2019)], we propose an implementation that uses dimensionless amplitudes for describing the photonic contributions to QED-TDDFT electron–photon eigenstates. This leads to a Hermitian QED-TDDFT coupling matrix that is expected to facilitate the future development of analytic derivatives. Through a Gaussian atomic basis implementation of the QED-TDDFT method, we examined the effect of dipole self-energy, rotating-wave approximation, and the Tamm–Dancoff approximation on the QED-TDDFT eigenstates of model compounds (ethene, formaldehyde, and benzaldehyde) in an optical cavity. We highlight, in the strong coupling regime, the role of higher-energy and off-resonance excited states with large transition dipole moments in the direction of the photonic field, which are automatically accounted for in our QED-TDDFT calculations and might substantially affect the energies and compositions of polaritons associated with lower-energy electronic states.

For nearly a century, oxygen has been widely accepted as the key element that triggers photoresponse in polycrystalline PbSe photoconductive detectors. Our photoluminescence and responsivity studies on PbSe samples, however, suggest that oxygen only serves as an effective sensitization improver and it is iodine rather than oxygen that plays the key role in triggering the photo-response. These studies shed light on the sensitization process for detector applications and ways to passivate defects in IV-VI semiconductors. As a result, high peak detectivity of 2.8 Â 10 10 cm Á Hz 1/2 Á W À1 was achieved at room temperature. V

n-CdS/p-PbSe heterojunction is investigated. A thin CdS film is deposited by chemical bath deposition on top of epitaxial PbSe film by molecular beam epitaxy on Silicon. Current-voltage measurements demonstrate very good junction characteristics with rectifying ratio of $178 and ideality factor of 1.79 at 300 K. Detectors made with such structure exhibit mid-infrared spectral photoresponse at room temperature. The peak responsivity R k and specific detectivity D * are 0.055 A/W and 5.482 Â 10 8 cmÁHz 1/2 /W at k ¼ 4.7 lm under zero-bias photovoltaic mode. Temperature-dependent photoresponse measurements show abnormal intensity variation below $200 K. Possible reasons for this phenomenon are also discussed. V

The CaF 2 nano-structures grown by thermal vapor deposition are presented. Significant responsivity improvement (>200%) of mid-infrared PbSe detectors incorporating a 200 nm nano-structured CaF 2 coating was observed. The detector provides a detectivity of 4.2 Â 10 10 cm Á Hz 1/2 /W at 3.8 lm, which outperforms all the reported un-cooled PbSe detectors. Structural investigations show that the coating is constructed by tapered-shape nanostructures, which creates a gradient refractive-index profile. Analogy to moth-eye antireflective mechanism, the gradient refractive-index nanostructures play the major roles for this antireflection effect. Some other possible mechanisms that help enhance the device performance are also discussed in the work.

Following the formulation of cavity quantum-electrodynamical time-dependent density functional theory (cQED-TDDFT) models [Flick et al., ACS Photonics 6, 2757–2778 (2019) and Yang et al., J. Chem. Phys. 155, 064107 (2021)], here, we report the derivation and implementation of the analytic energy gradient for polaritonic states of a single photochrome within the cQED-TDDFT models. Such gradient evaluation is also applicable to a complex of explicitly specified photochromes or, with proper scaling, a set of parallel-oriented, identical-geometry, and non-interacting molecules in the microcavity.