Ankun Yang

Real-time tunable lasing from plasmonic nanocavity arrays.

Plasmon lasers can support ultrasmall mode confinement and ultrafast dynamics with device feature sizes below the diffraction limit. However, most plasmon-based nanolasers rely on solid gain materials (inorganic semiconducting nanowire or organic dye in a solid matrix) that preclude the possibility of dynamic tuning. Here we report an approach to achieve real-time, tunable lattice plasmon lasing based on arrays of gold nanoparticles and liquid gain materials. Optically pumped arrays of gold nanoparticles surrounded by liquid dye molecules exhibit lasing emission that can be tuned as a function of the dielectric environment. Wavelength-dependent time-resolved experiments show distinct lifetime characteristics below and above the lasing threshold. By integrating gold nanoparticle arrays within microfluidic channels and flowing in liquid gain materials with different refractive indices, we achieve dynamic tuning of the plasmon lasing wavelength. Tunable lattice plasmon lasers offer prospects to enhance and detect weak physical and chemical processes on the nanoscale in real time.

Unidirectional Lasing from Template-Stripped Two-Dimensional Plasmonic Crystals.

Plasmon lasers support cavity structures with sizes below that of the diffraction limit. However, most plasmon-based lasers show bidirectional lasing emission or emission with limited far-field directionality and large radiative losses. Here, we report unidirectional lasing from ultrasmooth, template-stripped two-dimensional (2D) plasmonic crystals. Optically pumped 2D plasmonic crystals (Au or Ag) surrounded by dye molecules exhibited lasing in a single emission direction and their lasing wavelength could be tuned by modulating the dielectric environment. We found that 2D plasmonic crystals were an ideal architecture to screen how nanocavity unit-cell structure, metal material, and gain media affected the lasing response. We discovered that template-stripped strong plasmonic materials with cylindrical posts were an optimal cavity design for a unidirectional laser operating at room temperature.

Deterministic Coupling of Quantum Emitters in 2D Materials to Plasmonic Nanocavity Arrays

Quantum emitters in two-dimensional materials are promising candidates for studies of light-matter interaction and next generation, integrated on-chip quantum nanophotonics. However, the realization of integrated nanophotonic systems requires the coupling of emitters to optical cavities and resonators. In this work, we demonstrate hybrid systems in which quantum emitters in 2D hexagonal boron nitride (hBN) are deterministically coupled to high-quality plasmonic nanocavity arrays. The plasmonic nanoparticle arrays offer a high-quality, low-loss cavity in the same spectral range as the quantum emitters in hBN. The coupled emitters exhibit enhanced emission rates and reduced fluorescence lifetimes, consistent with Purcell enhancement in the weak coupling regime. Our results provide the foundation for a versatile approach for achieving scalable, integrated hybrid systems based on low-loss plasmonic nanoparticle arrays and 2D materials.

Band-edge engineering for controlled multi-modal nanolasing in plasmonic superlattices

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.

Programmable and reversible plasmon mode engineering

Significance Plasmonic nanostructures that can amplify localized optical fields and support ultranarrow resonances are critical for applications ranging from ultrasensitive molecular sensing to nanoscale lasing. However, the active engineering and maintaining of narrow resonances over a broad range of wavelengths, within a single system, is a grand challenge. In this paper, we introduce a platform that can overcome the limitations of as-fabricated nanoparticle arrays as well as toggle between different lattice plasmon mode orders (dipolar or quadrupolar) by mechanical manipulation of the sample along different symmetry directions. Dynamic tuning of narrow lattice plasmons (<5 nm) was possible over the entire visible wavelength range, which now opens possibilities in real-time optical systems and flexible electronics. Plasmonic nanostructures with enhanced localized optical fields as well as narrow linewidths have driven advances in numerous applications. However, the active engineering of ultranarrow resonances across the visible regime—and within a single system—has not yet been demonstrated. This paper describes how aluminum nanoparticle arrays embedded in an elastomeric slab may exhibit high-quality resonances with linewidths as narrow as 3 nm at wavelengths not accessible by conventional plasmonic materials. We exploited stretching to improve and tune simultaneously the optical response of as-fabricated nanoparticle arrays by shifting the diffraction mode relative to single-particle dipolar or quadrupolar resonances. This dynamic modulation of particle–particle spacing enabled either dipolar or quadrupolar lattice modes to be selectively accessed and individually optimized. Programmable plasmon modes offer a robust way to achieve real-time tunable materials for plasmon-enhanced molecular sensing and plasmonic nanolasers and opens new possibilities for integrating with flexible electronics.

Breakthroughs in Photonics 2014: Advances in Plasmonic Nanolasers

Plasmonic nanolasers are promising as nanoscale coherent sources of optical fields because they support ultrasmall sizes and show ultrafast dynamics. Major advances over the last several years have focused on nanocavity design, materials improvements in quality of both the plasmonic materials and gain media, and room-temperature operation. In 2014, the most significant results focused on tunable nanolasing emission and strategies to time-resolve the dynamics.

Coherent Light Sources at the Nanoscale

This review focuses on coherent light sources at the nanoscale, and specifically on lasers exploiting plasmonic cavities that can beat the diffraction limit of light. Conventional lasers exhibit coherent, intense, and directional emission with cavity sizes much larger than their operating wavelength. Plasmon lasers show ultrasmall mode confinement, support strong light-matter interactions, and represent a class of devices with extremely small sizes. We discuss the differences between plasmon lasers and traditional ones, and we highlight advances in directionality and tunability through innovative cavity designs and new materials. Challenges and future prospects are also discussed.

Correlating Nanoscopic Energy Transfer and Far-Field Emission to Unravel Lasing Dynamics in Plasmonic Nanocavity Arrays

Excited-state interactions between nanoscale cavities and photoactive molecules are critical in plasmonic nanolasing, although the underlying details are less-resolved. This paper reports direct visualization of the energy-transfer dynamics between two-dimensional arrays of plasmonic gold bowtie nanocavities and dye molecules. Transient absorption microscopy measurements of single bowties within the array surrounded by gain molecules showed fast excited-state quenching (2.6 ± 1 ps) characteristic of individual nanocavities. Upon optical pumping at powers above threshold, lasing action emerged depending on the spacing of the array. By correlating ultrafast microscopy and far-field light emission characteristics, we found that bowtie nanoparticles acted as isolated cavities when the diffractive modes of the array did not couple to the plasmonic gap mode. These results demonstrate how ultrafast microscopy can provide insight into energy relaxation pathways and, specifically, how nanocavities in arrays can show single-unit nanolaser properties.

Millimeter-Scale Spatial Coherence from a Plasmon Laser

Coherent light sources have been demonstrated based on a wide range of nanostructures, however, little effort has been devoted to probing their underlying coherence properties. Here, we report long-range spatial coherence of lattice plasmon lasers constructed from a periodic array of gold nanoparticles and a liquid gain medium at room temperature. By combining spatial and temporal interferometry, we demonstrate millimeter-scale (∼1 mm) spatial coherence and picosecond (∼2 ps) temporal coherence. The long-range spatial coherence occurs even without the presence of strong coupling with the lattice plasmon mode extending over macroscopic distances in the lasing regime. This plasmonic lasing system thus provides a platform for understanding the emergence of long-range coherence from collections of nanoscale resonators and points toward novel types of distributed lasing sources.