Band 12, Heft 8 - Special Issue: Nanofabrication

Semiconductor lasers play critical roles in many different systems, ranging from optical communications to absorption spectroscopy for environmental monitoring. Despite numerous applications, many semiconductor lasers have problems such as significant beam divergence and polarization instability. External optical elements like objective lenses and polarizers are usually needed to address these issues. This Review will discuss how these issues have recently been dealt with by instead integrating metasurfaces into semiconductor lasers. This necessitates the development of innovative fabrication methods; these will also be the topic of this Review. Metasurfaces can be integrated on the emitting facet of a laser. This can help select the lasing mode or can be used just to modify the output beam properties without affecting the modes. They can also be integrated monolithically with lasers through waveguides, or work in an external cavity configuration. These integrated devices provide novel optical functions, such as direct orbital angular momentum (OAM) mode generation, wavelength tuning and holographic pattern generation. We hope this Review will help extend the use of metasurface-integrated semiconductor lasers to scientific and industrial systems that employ lasers.

Silicon nitride (SiN) has surged into prominence as a material for photonic-integrated circuits (PICs) in the past decade, well regarded for its broadband transparency, compatibility with complementary metal oxide semiconductor (CMOS) fabrication processes and high optical bandgap that avoids two-photon absorption. However, current fabrication methods result in users having to choose between low thermal budgets and low losses, which are suboptimal given that both are necessary to facilitate a wide range of applications. Recently, works have emerged featuring PICs fabricated using deuterated silicon nitride (SiNx:D) – SiNx films grown using deuterated precursors instead of conventional hydrogenated ones. This decreases material absorption near the telecommunications bands at 1.55 µm previously present due to parasitic silicon–hydrogen and nitrogen–hydrogen bonds, attaining low-loss PICs realised using a low temperature, back-end-of-line CMOS-compatible fabrication plasma-enhanced chemical vapour deposition process. These devices have shown promise for both linear and nonlinear applications and the platform has the potential to be instrumental in realising highly efficient chips with co-packaged electronics and photonics devices. This paper reviews recent developments on the SiNx:D platform and provides a glance at future advancements for this highly promising material.

Metasurface-generated holograms have emerged as a unique platform for arbitrarily shaping the reflected/transmitted wavefronts with the advantages of subwavelength large pixel sizes and multiple information channels. However, achieving multiple holographic images with large operation bandwidths is a rather complicated and arduous issue due to the dissimilar dispersion of all meta-atoms involved. In this work, we design and experimentally demonstrate single-celled metasurfaces to realize broadband and spin-multiplexed holograms, whose phase modulation is based only on the geometric phase supplied by a judiciously designed high-performance nanoscale half-wave plate operating in reflection. Four different multiplexing strategies are implemented, and the resulting holograms are systemically assessed and compared with respect to background levels, image fidelities, holograms efficiencies, and polarization conversion ratios. Our work complements the methodologies available for designing multiplexed meta-holograms with versatile functionalities.

Metalenses have potential to replace various bulky conventional optical elements with ultrathin nanostructure arrays. In particular, active metalenses with reconfigurable focusing capability have attracted considerable interest from the academic and industrial communities. However, their tuning range is currently restricted by limited material properties and fabrication difficulties. Here, a hybrid optical system capable of three-dimensional relocation of a focal spot is proposed and experimentally demonstrated. The system comprises a mechanically actuated passive metalens doublet that can be easily fabricated with commonly available materials and processes. An incident laser can be focused to a desired point in three-dimensional space simply by rotating two metalenses or changing their separation. In addition, exploiting the polarization-multiplexing capability of metasurfaces, a hologram is incorporated to the metalenses to guide rotational and positional alignment of two metasurfaces. The ease of fabrication and alignment provided by this approach could widen its application to many practical fields.

Electrical switching of nanophotonic structural color elements is a promising approach towards addressable color switching pixels for next generation reflective displays. However, electrical switching between the primary colors to colorless near-white state remains a challenge. Here, we present a reversible electrical switching approach, relying on the electrocoagulation of Ag nanoparticles between silicon nanostructures that support Mie resonances. The electrodeposited Ag nanoparticles enable the excitation of the hybrid plasmon-Mie resonance as supported on Ag-silicon nanostructures, resulting in a large spectral transformation. Importantly, this process is reversible. This device design outperforms other designs in terms of electrotonic color control since it is highly stable and reliable for use in high-resolution reflective displays, such as colored electronic papers and smart display glass, where the combination is scalable to other nanostructure designs and electrolytic solutions.

We present an electrically switchable, compact metasurface device based on the metallic polymer PEDOT:PSS in combination with a gel polymer electrolyte. Applying square-wave voltages, we can reversibly switch the PEDOT:PSS from dielectric to metallic. Using this concept, we demonstrate a compact, standalone, and CMOS compatible metadevice. It allows for electrically controlled ON and OFF switching of plasmonic resonances in the 2–3 µm wavelength range, as well as electrically controlled beam switching at angles up to 10°. Furthermore, switching frequencies of up to 10 Hz, with oxidation times as fast as 42 ms and reduction times of 57 ms, are demonstrated. Our work provides the basis towards solid state switchable metasurfaces, ultimately leading to submicrometer-pixel spatial light modulators and hence switchable holographic devices.

The ideal single-photon source displaying high brightness and purity, emission on-demand, mature integration, practical communication wavelength (i.e., in the telecom range), and operating at room temperature does not exist yet. In 2018, a new single-photon source was discovered in gallium nitride (GaN) showing high potential thanks to its telecom wavelength emission, record-high brightness, good purity, and operation at room temperature. Despite all these assets, its coupling to photonic structures has not been achieved so far. In this article, we make a first step in this direction. First, we analyze whether stacking faults are indeed a necessary condition for obtaining such emitters in GaN layers. Then, we discuss the challenges associated to a low spatial density and to a spectrally wide distribution of emitters, which necessitate their location to be determined beforehand and the photonic structure resonance to be tuned to their emission wavelength. The design and fabrication of bullseye antennas are thoroughly described. Finally, we fabricate such bullseyes around telecom emitters and demonstrate that the embedded emitters are able to sustain the necessary clean-room process and still operate as single-photon emitters after the fabrication steps, with room-temperature purities up to 99% combined with repetition rates in the order of hundreds of kHz. The findings in this work demonstrate that telecom single-photon emitters in GaN operating at room temperature are well adapted for single-photon applications where brightness and purity are the required figures of merit, but highlight the numerous difficulties that still need to be overcome before they can be exploited in actual quantum photonic applications.

Nonlinear propagation in periodic media has been studied for decades, yielding demonstrations of numerous phenomena including strong temporal compression and slow light generation. Gap solitons, that propagate at frequencies inside the stopband, have been observed in optical fibres but have been elusive in photonic chips. In this manuscript, we investigate nonlinear pulse propagation in a chip-based nonlinear Bragg grating at frequencies inside the stopband and observe clear, unequivocal signatures of gap soliton propagation, including slow light, intensity-dependent transmission, intensity-dependent temporal delay and gap soliton compression. Our experiments which are performed in an on-chip ultra-silicon-rich nitride (USRN) Bragg grating with picosecond time scales, reveal slow light group velocity reduction to 35%–40% of the speed of light in vacuum, change in the temporal delay of 7 ps at low peak powers between 15.7 W–36.6 W, which is accompanied by up to 2.7× temporal compression of input pulses. Theoretical calculations using the nonlinear coupled mode equations confirm the observations of intensity-dependent temporal delay. Of fundamental importance, this demonstration opens up on-chip platforms for novel experimental studies of gap solitons as the basis of all-optical buffers, delay lines and optical storage.

Single-digit-nanometer scale plasmonic nanoantenna platforms are widely used in optical sensors, quantum plasmonics, and other applications. Uniform and reliable fabrications with a single-digit-nanometer resolution are desirable for diverse quantum nanophotonic device applications, but improving the process yield and uniformity of the shape of the nanoantenna over the entire fabrication area remains a challenge. Here we report the guided domino lithography fabrication method for uniform ultra-sharp nanoantenna arrays. We use a collapsing of unstable photoresist nanostructures with a guide structure to uniformly fabricate ultra-sharp bowtie photoresist masks. We directly compare the yields of the conventional and the guided domino lithography under the optimized electron beam exposing and development conditions. Furthermore, we conduct a rigorous analysis to verify the electric field enhancement effect from ultra-sharp bowtie nanoantennas fabricated with different geometry. We believe that guided domino lithography can be a promising solution toward a practical manufacturing method for single-digit-nanometer plasmonic nanoantennas.

Nano-kirigami method enables rich diversity of structural geometries that significantly broaden the functionalities of optical micro/nano-devices. However, the methodologies of various nano-kirigami are still limited and as a result, the chiral nano-kirigami structure has yet been pushed to the limit for operation at visible wavelength region. Here, the merits of the various nano-kirigami strategies are comprehensively explored and bio-inspired nano-cilia metasurface with enhanced circular dichroism at visible wavelengths is demonstrated. The stereo chiral nano-cilia metasurface is designed with three-fold rotational symmetry, which exhibits tuneable chiroptical responses when the nano-cilia are deformed to form strong chiral light–matter interactions. By employing electron-beam lithography (EBL) and focused ion beam (FIB) lithography, on-chip nano-cilia metasurfaces are experimentally realized in near-infrared wavelengths region and at visible wavelengths, respectively, successfully validating the giant circular dichroism revealed in simulations. Our work is useful to broaden the existing platform of micro/nano-scale manufacturing and could provide an effective method for the realization of versatile bioinspired nanostructures with profound chiroptical responses.

Epitaxially grown semiconductor quantum dots (QDs) and quantum rings (QRs) have been demonstrated to be excellent sources of single photons and entangled photon pairs enabling applications within quantum photonics. The emerging field of QD-based nanophotonics requires the deterministic integration of single or multiple QD structures into photonic architectures. However, the natural inhomogeneity and spatial randomness of self-assembled QDs limit their potential, and the reliable formation of homogeneous and ordered QDs during epitaxy still presents a challenge. Here, we demonstrate the fabrication of regular arrays of single III–V QDs and QRs using molecular beam epitaxy assisted by in situ direct laser interference patterning. Both droplet epitaxy (DE) GaAs/AlGaAs QDs and QRs and Stranski–Krastanov (SK) InAs/GaAs QDs are presented. The resulting QD structures exhibit high uniformity and good optical quality, in which a record-narrow photoluminescence linewidth of ∼17 meV from patterned GaAs QD arrays is achieved. Such QD and QR arrays fabricated through this novel optical technique constitute a next-generation platform for functional nanophotonic devices and act as useful building blocks for the future quantum revolution.

Cracks are formed along the photolithographically pre-determined lines with extremely high yield and repeatability, when Cu clusters are introduced between planarized Au thin films sequentially deposited on a PET substrate. These clusters act as nanometer-sized spacers preventing the formation of contiguous metallic bond between the adjacent Au layers which will render prepatterned-cracking impossible. While the effective gap width is initially zero in the optical sense from microwaves all the way to the visible, outer-bending the PET substrate allows the gap width tuning into the 100 nm range, with the stability and controllability in the ranges of 100 s and Angstrom-scale, respectively. It is anticipated that our wafer-scale prepatterned crack technology with an unprecedented mixture of macroscopic length and Angstrom-scale controllability will open-up many applications in optoelectronics, quantum photonics and photocatalysis.

Due to their atomic-scale thickness, handling and processing of two-dimensional (2D) materials often require multistep techniques whose complexity hampers their large-scale integration in modern device applications. Here we demonstrate that the laser-induced forward transfer (LIFT) method can achieve the one-step, nondestructive printing of the prototypical 2D material MoS 2 . By selecting the optimal LIFT experimental conditions, we were able to transfer arrays of MoS 2 pixels from a metal donor substrate to a dielectric receiver substrate. A combination of various characterization techniques has confirmed that the transfer of intact MoS 2 monolayers is not only feasible, but it can also happen without incurring significant defect damage during the process. The successful transfer of MoS 2 shows the broad potential the LIFT technique has in the emerging field of printed electronics, including printed devices based on 2D materials.

Fabrication of nanostructures with a feature size much smaller than the laser wavelength is challenging due to the optical diffraction limit. It’s well known that the irradiation of polarized ultrafast laser generates periodic nanostructures, so called laser-induced periodic surface structures (LIPSS). Owing to the modulated field, the surface is periodically ablated to form specific patterns, which can be used for some photonic applications including surface-enhanced Raman scattering (SERS). In this paper, we investigate the morphologies of LIPSS on ZnO substrates by mask-less ultrafast laser processing. By adjusting the laser processing parameters, including fluence, pulse number, polarization, and pulse duration, the homogenous nanostrip array and nanopillar array are created. Furthermore, by adjusting the laser fluence, a single nanogroove with a width of ∼20 nm and a single nanocavity with a diameter of ∼24 nm are created. The gold nanoparticles are then coated on the ZnO nanopillar array for SERS application. We found that the concentration of defects in ZnO substrate is increased by the laser irradiation, which is beneficial for SERS performances to achieve an enhancement factor of SERS as high as 2.28 × 10 7 .

The fabrication of three-dimensional (3D) nanostructures within optical materials is currently a highly sought-after capability. Achieving nanoscale structuring of media within its inner volume in 3D and with free design flexibility, high accuracy and precision is a development yet to be demonstrated. In this work, a 3D laser nanolithography technique is developed which allows producing mm-long hollow nanopores inside solid-state laser crystals and with a high degree of control of pore cross-sectional aspect ratio and size. We report an in-depth study on the formation of pores both within the non-thermal regime at which temperature is fast dissipated after each laser pulse, and for a thermally controlled regime using pulse-bursts which facilitate the formation of pores with highly circular shapes down to 1.1. We demonstrate this process for a wide range of speeds, pulse repetition rates and pulse energies, thus opening the door to a much more useful nanofabrication technique for nanophotonics. Finally, we also report the change in index of refraction that is produced at the nanoscale obtaining a positive index contrast of ∼3%. The work therefore provides a promising path towards reliable 3D nanostructuring of solid-state laser media for the flexible fabrication of large and complex structures with features sizes from the nanoscale up to the mm-scale. Moreover, due to the embedded, seamless, and monolithic nature of this technology, and since YAG crystals can sustain temperatures of up to 1900 °C and are highly chemically inert and erosion resistant, we anticipate its direct application in harsh environments.

The recent development of light-based 3D printing technologies has marked a turning point in additive manufacturing. Through photopolymerization, liquid resins can be solidified into complex objects. Usually, the polymerization is triggered by exciting a photoinitiator with ultraviolet (UV) or blue light. In two-photon printing (TPP), the excitation is done through the non-linear absorption of two photons; it enables printing 100-nm voxels but requires expensive femtosecond lasers which strongly limit their broad dissemination. Upconversion nanoparticles (UCNPs) have recently been proposed as an alternative to TPP for photopolymerization but using continuous-wave lasers. UCNPs convert near-infrared (NIR) into visible/UV light to initiate the polymerization locally as in TPP. Here we provide a study of this multi-photon mechanism and demonstrate how the non-linearity impacts the printing process. In particular, we report on the possibility of fine-tuning the size of the printed voxel by adjusting the NIR excitation intensity. Using gelatin-based hydrogel, we are able to vary the transverse voxel size from 1.3 to 2.8 μm and the axial size from 7.7 to 59 μm by adjusting the NIR power without changing the degree of polymerization. This work opens up new opportunities to construct 3D structures with micrometer feature size by direct laser writing with continuous wave inexpensive light sources.

The dependence of the polymerization and optical damage thresholds in multi-photon polymerization (MPP) lithography was studied using a broadly-tunable laser system with group delay dispersion (GDD) control. The order of non-linearity and the light–matter interaction mechanisms were investigated using the resolution bridges method for non-photosensitized SZ2080 TM and photosensitized SZ2080 TM + IRG369 prepolymers. Energy deposition, voxel dimension growth, and the size of the dynamic fabrication window (DFW) were measured in the 700–1300 nm wavelength range at three different pulse durations measured at the sample – 100, 200 and 300 fs. Polymerization was observed at all wavelengths and pulse durations without significant differences in the achieved minimal spatial dimension ( < 300 ${< } 300$ nm). This was achieved despite the broad range of excitation wavelengths used which spanned two- and three-photon absorption bands, and the differences in the absorption spectra of the prepolymers. The lateral and longitudinal voxel growth dynamics revealed an abrupt change in the power dependence of polymerization and a significant variation of the DFW – from 1 at 1250 nm to 29 at 700 nm. This result can be interpreted as a consequence of a change in the instantaneous refractive index and a lowering of the polymerization but not the damage threshold. The optimization of energy delivery to the material by a wavelength-tunable laser source with pulse duration control was experimentally validated. These findings are uncovering the complexity of polymerization mechanisms and are useful in further development of MPP technology.

A method for direct fabrication of 3D silver microstructures with high fabrication throughput on virtually any substrate is presented. The method is based on laser-induced photoreduction of silver ions to silver atoms, supported by nucleation, substrate functionalization and a multiple exposure fabrication process. The combination of the novel photosensitive suspension and the novel fabrication scheme enables effective fabrication speeds of up to 1 cm per second, with a minimum structure size of less than 1 μm, a resolution of more than 750 lines/mm and a resistivity of 3.0 · 10 −8  Ωm. With this fabrication speed, it is now possible to produce conductive silver topographies several millimeters in length. Thus, with a single technology, one can fabricate photonic components with characteristic spectral features ranging from mid-to far-infrared.

The continuously increasing interest in flexible and integrated photonics requires new strategies for device manufacturing on arbitrary complex surfaces and with smallest possible size, respectively. Terahertz (THz) technology can particularly benefit from this achievement to make compact systems for emission, detection and on-demand manipulation of THz radiation. Here, we present a novel fabrication method to realize conformable terahertz metasurfaces. The flexible and versatile character of polymeric nanomembranes is combined with direct laser writing via two-photon polymerization to develop free-standing ultra-thin quasi-perfect plasmonic absorbers with an unprecedentedly high level of conformability. Moreover, revealing new flexible dielectric materials presenting low absorption and permittivity in the THz range, this work paves the way for the realization of ultra-thin, conformable hybrid or all-dielectric devices to enhance and enlarge the application of THz technologies, and flexible photonics in general.

The systems for multiphoton 3D nanoprinting are rapidly increasing in print speed for larger throughput and scale, unfortunately without also improvement in resolution. Separately, the process of photoinhibition lithography has been demonstrated to enhance the resolution of multiphoton printing through the introduction of a secondary laser source. The photo-chemical dynamics and interactions for achieving photoinhibition in the various multiphoton photoinitiator systems are complex and still not well understood. Here, we examine the photoinhibition process of the common photoinitiator 7-diethylamino 3-thenoylcoumarin (DETC) with inhibition lasers near or at the multiphoton printing laser wavelength in typical low peak intensity, high repetition rate 3D nanoprinting processes. We demonstrate the clear inhibition of the polymerization process consistent with a triplet absorption deactivation mechanism for a DETC photoresist as well as show inhibition for several other photoresist systems. Additionally, we explore options to recover the photoinhibition process when printing with high intensity, low repetition rate lasers. Finally, we demonstrate photoinhibition in a projection multiphoton printing system. This investigation of photoinhibition lithography with common photoinitiators elucidates the possibility for photoinhibition occurring in many resist systems with typical high repetition rate multiphoton printing lasers as well as for high-speed projection multiphoton printing.

Perfect absorption over the entire visible spectrum can create a dark background for acquiring images with high contrast and improved resolution, which is crucial for various applications such as medical imaging, biological detection, and industrial non-destructive testing. The broadband absorption is desired to be achieved in an ultrathin structure for low noise as well as high integration. Here, we experimentally demonstrate a metasurface broadband perfect absorber with an ultrathin thickness of 148 nm and a large area of ∼10 cm 2 . Such a metasurface, with more than 97% absorption in the wavelength range from 400 to 800 nm, is composed of chromium nanodisk hexagonal array deposited on a chromium substrate with a silica spacer. A self-assembly based colloidal lithography nanofabrication method is developed for the scalable fabrication of the proposed nanostructure. We attribute the broadband absorption to the spectrally overlapped Fabry–Perot resonance, surface plasmon polariton, and localized surface plasmon resonances. Our results offer a novel approach to wafer-scale and low-cost manufacturing of absorption-based devices for applications such as high-contrast imaging and optical modulation.

Recent advances in nanofabrication technologies have enabled new ways to produce structural colors. By combining nanofabrication methods, it is possible to integrate electrochromic materials with the nanostructures, which enable electrical tuning of the colors and thus new types of reflective displays. Previous work has shown high quality colors and high switching contrast in general. However, so far the intensity modulation has always been more limited in the blue. In this work we prepare blue structural colors and synthesize films of an electrochromic polymer (PProDOP) that is optimized for high contrast in this spectral region. A protocol for electropolymerization of PProDOP on gold surfaces is presented. The polymer films are shown to follow Lambert–Beer behavior and can provide up to 75% contrast (difference in transmittivity). On blue nanostructures, the reflectivity can be modulated with a contrast of 50%, which is a considerable improvement in comparison with previous work. The results presented here should be useful for electrochromic or other electro-optical devices operating in the blue spectral region.

Lithium niobate on insulator is being established as a versatile platform for a new generation of photonic integrated devices. Extensive progress has been made in recent years to improve the fabrication of integrated optical circuits from a research platform towards wafer-scale fabrication in commercial foundries, and optical losses have reached remarkably low values approaching material limits. In this context, argon etching of lithium niobate waveguides has been shown to provide the best optical quality, yet the process is still challenging to optimise due to its physical nature. Namely, the micro-masking effects introduced by the material redeposition and a close to one etch mask selectivity for deep etches. We present a workflow to identify the parameter set offering the best etching results independent of the plasma system being used. We show how to reach the redeposition-free regime and propose three methods to achieve redeposition-free lithium niobate etching with good quality sidewalls without need of wet chemistry for cleaning.

Metasurfaces offer a versatile platform for engineering the wavefront of light using nanostructures with subwavelength dimensions and hold great promise for dramatically miniaturizing conventional optical elements due to their small footprint and broad functionality. However, metasurfaces so far have been mainly demonstrated on bulky and planar substrates that are often orders of magnitude thicker than the metasurface itself. Conventional substrates not only nullify the reduced footprint advantage of metasurfaces, but also limit their application scenarios. The bulk substrate also determines the metasurface dielectric environment, with potentially undesired optical effects that undermine the optical performance. Here we develop a universal polymer-assisted transfer technique to tackle this challenge by decoupling the substrate employed on the fabrication of metasurfaces from that used for the target application. As an example, Huygens’ metasurfaces with 120 nm thickness in the visible range (532 nm) are demonstrated to be transferred onto a 100 nm thick freestanding SiN x membrane while maintaining excellent structural integrity and optical performance of diffraction-limited focusing. This transfer method not only enables the thinnest dielectric metalens to the best of our knowledge, but also opens up new opportunities in integrating cascaded and multilayer metasurfaces, as well as the heterogeneous integration with nonconventional substrates and various electronic/photonic devices.