Since 2000, there has been an explosion of activity in the field of plasmon-enhanced Raman spectroscopy (PERS), including surface-enhanced Raman spectroscopy (SERS), tip-enhanced Raman spectroscopy (TERS) and shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS). In this Review, we explore the mechanism of PERS and discuss PERS hotspots — nanoscale regions with a strongly enhanced local electromagnetic field — that allow trace-molecule detection, biomolecule analysis and surface characterization of various materials. In particular, we discuss a new generation of hotspots that are generated from hybrid structures combining PERS-active nanostructures and probe materials, which feature a strong local electromagnetic field on the surface of the probe material. Enhancement of surface Raman signals up to five orders of magnitude can be obtained from materials that are weakly SERS active or SERS inactive. We provide a detailed overview of future research directions in the field of PERS, focusing on new PERS-active nanomaterials and nanostructures and the broad application prospect for materials science and technology. Assisted by rationally designed novel plasmonic nanostructures, surface-enhanced Raman spectroscopy has presented a new generation of analytical tools (that is, tip-enhanced Raman spectroscopy and shell-isolated nanoparticle-enhanced Raman spectroscopy) with an extremely high surface sensitivity, spatial resolution and broad application for materials science and technology.

Nanostructure-based plasmon-enhanced Raman spectroscopy for surface analysis of materials

Ultrafast transmission electron microscopy using a laser-driven field emitter: Femtosecond resolution with a high coherence electron beam.

Non-equilibrium photoinduced plasmons in a high-mobility graphene monolayer are investigated at infrared wavelengths. The success of metal-based plasmonics for manipulating light at the nanoscale has been empowered by imaginative designs and advanced nano-fabrication. However, the fundamental optical and electronic properties of elemental metals, the prevailing plasmonic media, are difficult to alter using external stimuli. This limitation is particularly restrictive in applications that require modification of the plasmonic response at sub-picosecond timescales. This handicap has prompted the search for alternative plasmonic media1,2,3, with graphene emerging as one of the most capable candidates for infrared wavelengths. Here we visualize and elucidate the properties of non-equilibrium photo-induced plasmons in a high-mobility graphene monolayer4. We activate plasmons with femtosecond optical pulses in a specimen of graphene that otherwise lacks infrared plasmonic response at equilibrium. In combination with static nano-imaging results on plasmon propagation, our infrared pump–probe nano-spectroscopy investigation reveals new aspects of carrier relaxation in heterostructures based on high-purity graphene.

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Ultrafast optical switching of infrared plasmon polaritons in high-mobility graphene

Time-domain interferometry and near-field scanning microscopy are used to investigate infrared phonon polaritons exhibiting hyperbolic dispersion. Negative phase velocity and group velocity as small as 0.002c are confirmed. Polaritons with hyperbolic dispersion are key to many emerging photonic technologies, including subdiffraction imaging, sensing and spontaneous emission engineering1,2,3,4,5,6,7,8. Fundamental to their effective application are the lifetimes of the polaritons, as well as their phase and group velocities7,9. Here, we combine time-domain interferometry10 and scattering-type near-field microscopy11 to visualize the propagation of hyperbolic polaritons in space and time, allowing the first direct measurement of all these quantities. In particular, we study infrared phonon polaritons in a thin hexagonal boron nitride8,12,13 waveguide exhibiting hyperbolic dispersion and deep subwavelength-scale field confinement. Our results reveal—in a natural material—negative phase velocity paired with a remarkably slow group velocity of 0.002c and lifetimes in the picosecond range. While these findings show the polariton's potential for mediating strong light–matter interactions and negative refraction, our imaging technique paves the way to explicit nanoimaging of polariton propagation characteristics in other two-dimensional materials, metamaterials and waveguides.

Direct observation of ultraslow hyperbolic polariton propagation with negative phase velocity

Optical metasurfaces are two-dimensional optical elements composed of dense arrays of subwavelength optical antennas and afford on-demand manipulation of the basic properties of light waves. Following the pioneering works on active metasurfaces capable of modulating wave amplitude, there is now a growing interest to dynamically control other fundamental properties of light. Here, we present metasurfaces that facilitate electrical tuning of the reflection phase and polarization properties. To realize these devices, we leverage the properties of actively controlled plasmonic antennas and fundamental insights provided by coupled mode theory. Indium–tin–oxide is embedded into gap-plasmon resonator-antennas as it offers electrically tunable optical properties. By judiciously controlling the resonant properties of the antennas from under- to overcoupling regimes, we experimentally demonstrate tuning of the reflection phase over 180°. This work opens up new design strategies for active metasurfaces for displacem...

Dynamic Reflection Phase and Polarization Control in Metasurfaces

We report low-noise avalanche gain from photodiodes composed of a previously uncharacterized alloy, Al0.7In0.3As0.3Sb0.7, grown on GaSb. The bandgap energy and thus the cutoff wavelength are similar to silicon; however, since the bandgap of Al0.7In0.3As0.3Sb0.7 is direct, its absorption depth is 5 to 10 times shorter than indirect-bandgap silicon, potentially enabling significantly higher operating bandwidths. In addition, unlike other III-V avalanche photodiodes that operate in the visible or near infrared, the excess noise factor is comparable to or below that of silicon, with a k-value of approximately 0.015. Furthermore, the wide array of absorber regions compatible with GaSb substrates enable cutoff wavelengths ranging from 1 μm to 12 μm.

Low-noise AlInAsSb avalanche photodiode

We report on time-resolved mid-infrared (mid-IR) near- field spectroscopy of the narrow bandgap semiconductor InAs. The dominant effect we observed pertains to the dynamics of photoexcited carriers and associated surface plasmons. A novel combination of pump− probe techniques and near-field nanospectroscopy accesses high momentum plasmons and demonstrates efficient, subpicosecond photo- modulation of the surface plasmon dispersion with subsequent tens of picoseconds decay under ambient conditions. The photoinduced change of the probe intensity due to plasmons in InAs is found to exceed that of other mid-IR or near-IR media by 1−2 orders of magnitude. Remarkably, the required control pulse fluence is as low as 60 μJ/cm 2 , much smaller than fluences of ∼1−10 mJ/cm 2 previously utilized in ultrafast control of near-IR plasmonics. These low excitation densities are easily attained with a standard 1.56 μm fiber laser. Thus, InAsa common semiconductor with favorable plasmonic properties such as a low effective masshas the potential to become an important building block of optically controlled plasmonic devices operating at infrared frequencies.

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Ultrafast dynamics of surface plasmons in InAs by time-resolved infrared nanospectroscopy.

AlxIn1–xAsySb1–y digital alloys lattice-matched to GaSb were grown within the miscibility gap by molecular beam epitaxy, with aluminum fractions ranging from 0% to 80%. Photoluminescence spectra from AlxIn1–xAsySb1–y films and from AlxIn1–xAsySb1–y/GaSb type-II superlattices were used to determine the direct bandgap and the band offsets as a function of the aluminum fraction. Varying the aluminum content tuned the direct bandgap from 0.25 eV (0% aluminum) to 1.24 eV (75% aluminum), corresponding to photon wavelengths from 5000 to 1000 nm, with the transition from direct-gap to indirect-gap occurring at ∼1.18 eV (∼72% aluminum), or 1050 nm. This direct-gap tuning range of 0.93 eV is the largest reported for a III–V alloy lattice-matched to a commercially available substrate. The broadly tunable bandgap and type-I band alignments of this lattice-matched quaternary make it attractive for advanced mid-infrared and near-infrared detectors and sources.

Broadly Tunable AlInAsSb Digital Alloys Grown on GaSb

Thermal emission from objects tends to be spectrally broadband, unpolarized, and temporally invariant. These common notions are now challenged with the emergence of new nanophotonic structures and concepts that afford on-demand, active manipulation of the thermal emission process. This opens a myriad of new applications in chemistry, health care, thermal management, imaging, sensing, and spectroscopy. Here, we theoretically propose and experimentally demonstrate a new approach to actively tailor thermal emission with a reflective, plasmonic metasurface in which the active material and reflector element are epitaxially grown, high-carrier-mobility InAs layers. Electrical gating induces changes in the charge carrier density of the active InAs layer that are translated into large changes in the optical absorption and thermal emission from metasurface. We demonstrate polarization-dependent and electrically controlled emissivity changes of 3.6%P (6.5% in relative scale) in the mid-infrared spectral range.

Dynamic thermal emission control with InAs-based plasmonic metasurfaces

Over 30 years ago, Capasso and co-workers [IEEE Trans. Electron Devices 30, 381 (1982)] proposed the staircase avalanche photodetector (APD) as a solid-state analog of the photomultiplier tube. In this structure, electron multiplication occurs deterministically at steps in the conduction band profile, which function as the dynodes of a photomultiplier tube, leading to low excess multiplication noise. Unlike traditional APDs, the origin of staircase gain is band engineering rather than large applied electric fields. Unfortunately, the materials available at the time, principally AlxGa1−xAs/GaAs, did not offer sufficiently large conduction band offsets and energy separations between the direct and indirect valleys to realize the full potential of the staircase gain mechanism. Here, we report a true staircase APD operation using alloys of a rather underexplored material, AlxIn1−xAsySb1−y, lattice-matched to GaSb. Single step “staircase” devices exhibited a constant gain of ∼2×, over a broad range of applied ...

Scott J. Maddox

Papers

Low-noise AlInAsSb avalanche photodiode

Ultrafast dynamics of surface plasmons in InAs by time-resolved infrared nanospectroscopy.

Broadly Tunable AlInAsSb Digital Alloys Grown on GaSb

Dynamic thermal emission control with InAs-based plasmonic metasurfaces

AlInAsSb/GaSb staircase avalanche photodiode