Single band-edge states can trap light and function as high-quality optical feedback for microscale lasers and nanolasers. However, access to more than a single band-edge mode for nanolasing has not been possible because of limited cavity designs. Here, we describe how plasmonic superlattices-finite-arrays of nanoparticles (patches) grouped into microscale arrays-can support multiple band-edge modes capable of multi-modal nanolasing at programmed emission wavelengths and with large mode spacings. Different lasing modes show distinct input-output light behaviour and decay dynamics that can be tailored by nanoparticle size. By modelling the superlattice nanolasers with a four-level gain system and a time-domain approach, we reveal that the accumulation of population inversion at plasmonic hot spots can be spatially modulated by the diffractive coupling order of the patches. Moreover, we show that symmetry-broken superlattices can sustain switchable nanolasing between a single mode and multiple modes.

Acceleration and manipulation of electron bunches underlie most electron and X-ray devices used for ultrafast imaging and spectroscopy. New terahertz-driven concepts offer orders-of-magnitude improvements in field strengths, field gradients, laser synchronization and compactness relative to conventional radio-frequency devices, enabling shorter electron bunches and higher resolution with less infrastructure while maintaining high charge capacities (pC), repetition rates (kHz) and stability. We present a segmented terahertz electron accelerator and manipulator (STEAM) capable of performing multiple high-field operations on the 6D-phase-space of ultrashort electron bunches. With this single device, powered by few-micro-Joule, single-cycle, 0.3 THz pulses, we demonstrate record THz-acceleration of >30 keV, streaking with <10 fs resolution, focusing with >2 kT/m strength, compression to ~100 fs as well as real-time switching between these modes of operation. The STEAM device demonstrates the feasibility of THz-based electron accelerators, manipulators and diagnostic tools enabling science beyond current resolution frontiers with transformative impact.

X-ray crystallography is one of the main methods to determine atomic-resolution 3D images of the whole spectrum of molecules ranging from small inorganic clusters to large protein complexes consisting of hundred-thousands of atoms that constitute the macromolecular machinery of life. Life is not static, and unravelling the structure and dynamics of the most important reactions in chemistry and biology is essential to uncover their mechanism. Many of these reactions, including photosynthesis which drives our biosphere, are light induced and occur on ultrafast timescales. These have been studied with high time resolution primarily by optical spectroscopy, enabled by ultrafast laser technology, but they reduce the vast complexity of the process to a few reaction coordinates. In the AXSIS project at CFEL in Hamburg, funded by the European Research Council, we develop the new method of attosecond serial X-ray crystallography and spectroscopy, to give a full description of ultrafast processes atomically resolved in real space and on the electronic energy landscape, from co-measurement of X-ray and optical spectra, and X-ray diffraction. This technique will revolutionize our understanding of structure and function at the atomic and molecular level and thereby unravel fundamental processes in chemistry and biology like energy conversion processes. For that purpose, we develop a compact, fully coherent, THz-driven atto-second X-ray source based on coherent inverse Compton scattering off a free-electron crystal, to outrun radiation damage effects due to the necessary high X-ray irradiance required to acquire diffraction signals. This highly synergistic project starts from a completely clean slate rather than conforming to the specifications of a large free-electron laser (FEL) user facility, to optimize the entire instrumentation towards fundamental measurements of the mechanism of light absorption and excitation energy transfer. A multidisciplinary team formed by laser-, accelerator,- X-ray scientists as well as spectroscopists and biochemists optimizes X-ray pulse parameters, in tandem with sample delivery, crystal size, and advanced X-ray detectors. Ultimately, the new capability, attosecond serial X-ray crystallography and spectroscopy, will be applied to one of the most important problems in structural biology, which is to elucidate the dynamics of light reactions, electron transfer and protein structure in photosynthesis.

This Letter reports the shape-dependent third-order nonlinear optical properties of anisotropic gold nanoparticles. We characterized the nonlinear absorption coefficients of nanorods, nanostars, and nanoshells using femtosecond Z-scan measurements. By comparing nanoparticle solutions with a similar linear extinction at the laser excitation wavelength, we separated shape effects from that of the localized surface plasmon wavelength. We found that the nonlinear response depended on particle shape. Using pump-probe spectroscopy, we measured the ultrafast transient response of nanoparticles, which supported the strong saturable absorption observed in nanorods and weak nonlinear response in nanoshells. We found that the magnitude of saturable absorption as well as the ultrafast spectral responses of nanoparticles were affected by the linear absorption of the nanoparticles.

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This Letter describes how out-of-plane lattice plasmon (OLP) resonances in 2D Au nanoparticle (NP) arrays show dispersive quality factors. These quality factors can be tailored simply by controlling NP height. Numerical calculations of near-field optical properties and band diagrams were performed to understand the measured dispersion effects of the OLPs. The results revealed that delocalized OLPs are a type of surface Bloch mode composed of many Bloch harmonics. As the OLP dispersion evolves from a stationary state to a propagating state, the nonradiative loss decreases because of weak local field confinement, whereas the radiative loss increases because of strong coupling to the leaky zero-order harmonic.

This article describes the angle-dependent optical responses of 2D metal−insulator−metal (MIM) nanocavity arrays. Through a combination of soft nanolithography and template stripping, we fabricated arrays of plasmonic MIM nanostructures with subwavelength spacings over square centimeter areas. We controlled the coupling between the localized surface plasmon and guided modes as well as engineered the optical band structure by tuning the insulator thickness. Rabi splitting of hybridized modes strongly depended on the spatial overlap of the near-fields of the localized and guided modes.

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