Enhancement of and interference among higher order multipole transitions in molecules near a plasmonic nanoantenna

Spontaneous emission of quantum emitters can be modified by engineering their optical environment. This allows a resonant nanoantenna to significantly modify the radiative properties of a quantum emitter. In this article, we go beyond the common electric dipole approximation for the molecular electronic transition and take light-matter coupling through higher order multipoles into account. We investigate, by means of theory and numerical simulations, a strong enhancement of the magnetic dipole and electric quadrupole emission channels of a molecule adjacent to a plasmonic patch nanoantenna. While this on its own had been considered, the assumption in prior work usually has been that each molecular transition is dominated only by one of those multipolar emission channels. This leads naturally to the notion of discussing the modified emission in terms of a modified local density of states defined for each specific multipolar transition. In reality, this restricts the applicability of the approach, since specific molecular transitions occur via multiple multipolar pathways that have to be considered all at once. Here, we introduce a framework to study interference effects between higher order transitions in molecules by (a) a rigorous quantum-chemical calculation of their multipolar moments and (b) by a consecutive investigation of the transition rate upon coupling to an arbitrarily shaped nanoantenna. Based on that formalism we predict interference effects between these transition channels. This allows for a strong suppression of radiation by exploiting destructive interference. Our work suggests that placing a suitably chosen molecule at a well defined position and at a well defined orientation relative to a nanoantenna can fully suppress the transition probability.Comment: 30 pages, 8 figure

Effective pruning of web-scale datasets based on complexity of concept clusters

Utilizing massive web-scale datasets has led to unprecedented performance gains in machine learning models, but also imposes outlandish compute requirements for their training. In order to improve training and data efficiency, we here push the limits of pruning large-scale multimodal datasets for training CLIP-style models. Today's most effective pruning method on ImageNet clusters data samples into separate concepts according to their embedding and prunes away the most prototypical samples. We scale this approach to LAION and improve it by noting that the pruning rate should be concept-specific and adapted to the complexity of the concept. Using a simple and intuitive complexity measure, we are able to reduce the training cost to a quarter of regular training. By filtering from the LAION dataset, we find that training on a smaller set of high-quality data can lead to higher performance with significantly lower training costs. More specifically, we are able to outperform the LAION-trained OpenCLIP-ViT-B32 model on ImageNet zero-shot accuracy by 1.1p.p. while only using 27.7% of the data and training compute. Despite a strong reduction in training cost, we also see improvements on ImageNet dist. shifts, retrieval tasks and VTAB. On the DataComp Medium benchmark, we achieve a new state-of-the-art Imagehttps://info.arxiv.org/help/prep#commentsNet zero-shot accuracy and a competitive average zero-shot accuracy on 38 evaluation tasks.Comment: Accepted at ICLR 2024, code available at https://github.com/amro-kamal/effective_prunin

If your data distribution shifts, use self-learning

We demonstrate that self-learning techniques like entropy minimization and pseudo-labeling are simple and effective at improving performance of a deployed computer vision model under systematic domain shifts. We conduct a wide range of large-scale experiments and show consistent improvements irrespective of the model architecture, the pre-training technique or the type of distribution shift. At the same time, self-learning is simple to use in practice because it does not require knowledge or access to the original training data or scheme, is robust to hyperparameter choices, is straight-forward to implement and requires only a few adaptation epochs. This makes self-learning techniques highly attractive for any practitioner who applies machine learning algorithms in the real world. We present state-of-the-art adaptation results on CIFAR10-C (8.5% error), ImageNet-C (22.0% mCE), ImageNet-R (17.4% error) and ImageNet-A (14.8% error), theoretically study the dynamics of self-supervised adaptation methods and propose a new classification dataset (ImageNet-D) which is challenging even with adaptation.Comment: Web: https://domainadaptation.org/selflearnin

Hybrid nanoantennas for directional emission enhancement

Plasmonic and dielectric nanoparticles offer complementary strengths regarding their use as optical antenna elements. While plasmonic nanoparticles are well-known to provide strong decay rate enhancement for localized emitters, all-dielectric nanoparticles can enable high directivity combined with low losses. Here, we suggest a hybrid metal-dielectric nanoantenna consisting of a gold nanorod and a silicon nanodisk, which combines all these advantages. Our numerical analysis reveals a giant enhancement of directional emission together with simultaneously high radiation efficiency (exceeding 70%). The suggested hybrid nanoantenna has a subwavelength footprint, and all parameters and materials are chosen to be compatible with fabrication by two-step electron-beam lithography.The authors acknowledge a support from the Australian Research Council

Manipulation of photoluminescence of two-dimensional MoSe₂ by gold nanoantennas

Monolayer molybdenum diselenide (MoSe₂), a member of the TMDCs family, is an appealing candidate for coupling to gold plasmonic nanostructures as it has smaller bandgap and higher electron mobility in comparison to frequently studied molybdenum disulfide (MoS₂). The PL of MoSe₂ occurs in the near-infrared spectral range where the emissive properties do not suffer from the enhanced dissipation in the gold due to inter-band transitions. Here, we study the interaction between monolayer MoSe₂ and plasmonic dipolar antennas in resonance with the PL emission of MoSe₂. By varying the thickness of the spacer between the MoSe₂ layer and nanoantenna, we demonstrate manipulation of the PL intensity from nearly fourfold quenching to approximately threefold enhancement. Furthermore, we show that the coupled TMDC-nanoantenna system exhibits strong polarization-dependent PL, thus offering the possibility of polarization-based emission control. Our experimental results are supported by numerical simulations as well. To the best of our knowledge, this is the first study of Au-MoSe₂ plasmonic hybrid structures realizing flexible PL manipulation

Manipulation of Magnetic Dipole Emission from Eu 3+ with Mie-Resonant Dielectric Metasurfaces

Mie-resonant high-index dielectric nanoparticles and metasurfaces have been suggested as a viable platform for enhancing both electric and magnetic dipole transitions of fluorescent emitters. While the enhancement of the electric dipole transitions by such dielectric nanoparticles has been demonstrated experimentally, the case of magnetic-dipole transitions remains largely unexplored. Here, we study the enhancement of spontaneous emission of Eu3+ ions, featuring both electric and magnetic-dominated dipole transitions, by dielectric metasurfaces composed of Mie-resonant silicon nanocylinders. By coating the metasurfaces with a layer of an Eu3+ doped polymer, we observe an enhancement of the Eu3+ emission associated with the electric (at 610 nm) and magnetic-dominated (at 590 nm) dipole transitions. The enhancement factor depends systematically on the spectral proximity of the atomic transitions to the Mie resonances as well as their multipolar order, both controlled by the nanocylinder size. Importantly, the branching ratio of emission via the electric or magnetic transition channel can be modified by carefully designing the metasurface, where the magnetic dipole transition is enhanced more than the electric transition for cylinders with radii of about 130 nm. We confirm our observations by numerical simulations based on the reciprocity principle. Our results open new opportunities for bright nanoscale light sources based on magnetic transitions.Financial support by the Thuringian State Government within its ProExcellence initiative (ACP2020) and the German Research Foundation (STA 1426/2-1) is gratefully acknowledged. K.E.C., D.N.N., and Y.S.K. acknowledge the support by the Australian Research Council (DP150103733). Y.S.K. acknowledges a support from the Alexander von Humboldt Foundation. S.N. acknowledges financial support by the Karlsruhe School of Optics and Photonics and by the DFG Priority Programm 1839 Tailored Disorder. The authors also acknowledge their participation in the Erasmus Mundus NANOPHI project, contract number 2013 5659/002- 001. N.N., M.A.N., and S.M. would like to acknowledge the support by NSF EiR grant # 1830886