Anti-reflection coating with mullite and Duroid for large-diameter cryogenic sapphire and alumina optics.

We developed a broadband two-layer anti-reflection (AR) coating for use on a sapphire half-wave plate (HWP) and an alumina infrared (IR) filter for the cosmic microwave background (CMB) polarimetry. Measuring the faint CMB B-mode signals requires maximizing the number of photons reaching the detectors and minimizing spurious polarization due to reflection with an off-axis incident angle. Sapphire and alumina have high refractive indices of 3.1 and are highly reflective without an AR coating. This paper presents the design, fabrication, quality control, and measured performance of an AR coating using thermally sprayed mullite and Duroid 5880LZ. This technology enables large optical elements with diameters of 600 mm. We also present a thermography-based nondestructive quality control technique, which is key to assuring good adhesion and preventing delamination when thermal cycling. We demonstrate the average reflectance of about 2.6% (0.9%) for two observing bands centered at 90/150 (220/280) GHz. At room temperature, the average transmittance of a 105 mm square test sample at 220/280 GHz is 83%, and it will increase to 90% at 100 K, attributed to reduced absorption losses. Therefore, our developed layering technique has proved effective for 220/280 GHz applications, particularly in addressing dielectric loss concerns. This AR coating technology has been deployed in the cryogenic HWP and IR filters of the Simons Array and the Simons observatory experiments and applies to future experiments such as CMB-S4.

Laser processing of silicon with GHz burst pumped third harmonics for precise microfabrication.

Femtosecond laser processing has proved to be a valuable tool for various microfabrication applications. In order to further increase the quality and efficiency of femtosecond laser processing, processing with GHz burst mode lasers has gained attention in recent years, where packets of high-repetition rate pulses are used instead of single pulses at the fundamental repetition rate. However, the use of burst-pulses has mainly been limited to the fundamental wavelength of powerful regenerative amplifier systems, often near 1 micrometer wavelength. In this study, we explore the characteristics and potential benefits of further wavelength conversion of burst-pulses emitted at the near-infrared to the ultraviolet region via direct third-harmonic generation. We construct an in-line process evaluation setup with a chromatic confocal sensor, and evaluate the ablation characteristics of the burst-pumped and non-burst processing of silicon. We observe that burst-mode processing has significantly reduced surface roughness and debris, resulting in high-quality laser processing. To demonstrate the utility of such burst-pumped UV processing, we show the successful milling of a spherical structure enabled by in-line surface profile feedback, while similar processing with non-burst conditions did not work. We believe such results show the strong potential of burst laser sources for use in accurate microfabrication of structures with micrometer-scale resolution.

Simulation of nonlinear propagation of femtosecond laser pulses in air for quantitative prediction of the ablation crater shape.

The utilization of sub-100 fs pulses has attracted attention as an approach to further improve the quality and precision of femtosecond laser microfabrication. However, when using such lasers at pulse energies typical for laser processing, nonlinear propagation effects in air are known to distort the beam's temporal and spatial intensity profile. Due to this distortion, it has been difficult to quantitatively predict the final processed crater shape of materials ablated by such lasers. In this study, we developed a method to quantitatively predict the ablation crater shape, utilizing nonlinear propagation simulations. Investigations revealed that the ablation crater diameters derived by our method were in excellent quantitative agreement with experimental results for several metals over a two-orders-of-magnitude range in the pulse energy. We also found a good quantitative correlation between the simulated central fluence and the ablation depth. Such methods should improve the controllability of laser processing with sub-100 fs pulses and contribute to furthering their practical application to processes over a wide pulse-energy range, including conditions with nonlinear-propagating pulses.

Tb3+-doped fluorescent glass for biology.

Optical investigation and manipulation constitute the core of biological experiments. Here, we introduce a new borosilicate glass material that contains the rare-earth ion terbium(III) (Tb3+), which emits green fluorescence upon blue light excitation, similar to green fluorescent protein (GFP), and thus is widely compatible with conventional biological research environments. Micropipettes made of Tb3+-doped glass allowed us to target GFP-labeled cells for single-cell electroporation, single-cell transcriptome analysis (Patch-seq), and patch-clamp recording under real-time fluorescence microscopic control. The glass also exhibited potent third harmonic generation upon infrared laser excitation and was usable for online optical targeting of fluorescently labeled neurons in the in vivo neocortex. Thus, Tb3+-doped glass simplifies many procedures in biological experiments.

Tailoring Single-Cycle Near Field in a Tunnel Junction with Carrier-Envelope Phase-Controlled Terahertz Electric Fields.

Light-field-driven processes occurring under conditions far beyond the diffraction limit of the light can be manipulated by harnessing spatiotemporally tunable near fields. A tailor-made carrier envelope phase in a tunnel junction formed between nanogap electrodes allows precisely controlled manipulation of these processes. In particular, the characterization and active control of near fields in a tunnel junction are essential for advancing elaborate manipulation of light-field-driven processes at the atomic-scale. Here, we demonstrate that desirable phase-controlled near fields can be produced in a tunnel junction via terahertz scanning tunneling microscopy (THz-STM) with a phase shifter. Measurements of the phase-resolved subcycle electron tunneling dynamics revealed an unexpected large carrier-envelope phase shift between far-field and near-field single-cycle THz waveforms. The phase shift stems from the wavelength-scale feature of the tip-sample configuration. By using a dual-phase double-pulse scheme, the electron tunneling was coherently manipulated over the femtosecond time scale. Our new prescription-in situ tailoring of single-cycle THz near fields in a tunnel junction-will offer unprecedented control of electrons for ultrafast atomic-scale electronics and metrology.

Real-time broadband terahertz spectroscopic imaging by using a high-sensitivity terahertz camera.

Terahertz (THz) imaging has a strong potential for applications because many molecules have fingerprint spectra in this frequency region. Spectroscopic imaging in the THz region is a promising technique to fully exploit this characteristic. However, the performance of conventional techniques is restricted by the requirement of multidimensional scanning, which implies an image data acquisition time of several minutes. In this study, we propose and demonstrate a novel broadband THz spectroscopic imaging method that enables real-time image acquisition using a high-sensitivity THz camera. By exploiting the two-dimensionality of the detector, a broadband multi-channel spectrometer near 1 THz was constructed with a reflection type diffraction grating and a high-power THz source. To demonstrate the advantages of the developed technique, we performed molecule-specific imaging and high-speed acquisition of two-dimensional (2D) images. Two different sugar molecules (lactose and D-fructose) were identified with fingerprint spectra, and their distributions in one-dimensional space were obtained at a fast video rate (15 frames per second). Combined with the one-dimensional (1D) mechanical scanning of the sample, two-dimensional molecule-specific images can be obtained only in a few seconds. Our method can be applied in various important fields such as security and biomedicine.

Enantiomeric switching of chiral metamaterial for terahertz polarization modulation employing vertically deformable MEMS spirals.

Active modulation of the polarization states of terahertz light is indispensable for polarization-sensitive spectroscopy, having important applications such as non-contact Hall measurements, vibrational circular dichroism measurements and anisotropy imaging. In the terahertz region, the lack of a polarization modulator similar to a photoelastic modulator in the visible range hampers expansion of such spectroscopy. A terahertz chiral metamaterial has a huge optical activity unavailable in nature; nevertheless, its modulation is still challenging. Here we demonstrate a handedness-switchable chiral metamaterial for polarization modulation employing vertically deformable Micro Electro Mechanical Systems. Vertical deformation of a planar spiral by a pneumatic force creates a three-dimensional spiral. Enantiomeric switching is realized by selecting the deformation direction, where the polarity of the optical activity is altered while maintaining the spectral shape. A polarization rotation as high as 28° is experimentally observed, thus providing a practical and compact polarization modulator for the terahertz range.

Polarization control of quantum dot emission by chiral photonic crystal slabs.

We investigate theoretically the polarization properties of the quantum dot's (QDs) optical emission from chiral photonic crystal structures made of achiral materials in the absence of external magnetic field at room temperature. The mirror symmetry of the local electromagnetic field is broken in this system due to the decreased symmetry of the chiral modulated layer. As a result, the radiation of randomly polarized QDs normal to the structure becomes partially circularly polarized. The sign and degree of circular polarization are determined by the geometry of the chiral modulated structure and depend on the radiation frequency. A degree of circular polarization up to 99% can be achieved for randomly distributed QDs, and can be close to 100% for some single QDs.

Highly precise and accurate terahertz polarization measurements based on electro-optic sampling with polarization modulation of probe pulses.

We have developed an electro-optic (EO) sampling method with polarization modulation of probe pulses; this method allows us to measure the direction of a terahertz (THz) electric-field vector with a precision of 0.1 mrad in a data acquisition time of 660 ms using a 14.0-kHz repetition rate pulsed light source. Through combination with a THz time-domain spectroscopy technique, a time-dependent two-dimensional THz electric field was obtained. We used a photoelastic modulator for probe-polarization modulation and a (111)-oriented zincblende crystal as the EO crystal. Using the tilted pulse front excitation method with stable regeneratively amplified pulses, we prepared stable and intense THz pulses and performed pulse-by-pulse analog-to-digital conversion of the signals. These techniques significantly reduced statistical errors and enabled sub-mrad THz polarization measurements. We examined the performance of this method by measuring a wire-grid polarizer as a sample. The present method will open a new frontier of high-precision THz polarization sensitive measurements.

Generation of broadband terahertz vortex beams.

We propose and demonstrate a method for generating broadband terahertz (THz) vortex beams. We convert a THz radially polarized beam into a THz vortex beam via achromatic polarization optical elements for THz waves and characterize the topological charge of the generated vortex beam by measuring the spatial distribution of the phase of the THz wave at its focal plane. For example, a uniform topological charge of +1 is achieved over a wide frequency range. We also demonstrate that the sign of the topological charge can be easily controlled. By utilizing the orbital angular momentum of the beam, these results open new THz wave technologies for sensing, manipulation, and telecommunication.

All-photoinduced terahertz optical activity.

We proposed and demonstrated active control of terahertz optical activity via chiral patterned photoexcitation in a semiconductor with a spatial light modulator (SLM). Arbitrary patterns can be generated by a SLM, including completely symmetric enantiomer pairs. This technique provides a new route to terahertz polarization modulators.

Polarization-controlled circular second-harmonic generation from metal hole arrays with threefold rotational symmetry.

The discrete rotational symmetry of nanostructures provides a powerful and simple guiding principle for designing the second-harmonic generation process in nonlinear metamaterials. We demonstrate that, in achiral nanostructures with threefold rotational symmetries, a circularly polarized fundamental beam produces a countercircularly polarized second-harmonic beam. In this case, the polarization state of the second harmonic is determined in a very simple manner. We also demonstrate how rotational symmetries in nonlinear metamaterials manifest themselves in SHG selection rules.

Efficient coupling of propagating broadband terahertz radial beams to metal wires.

Bare metal wires have recently been demonstrated as waveguides for transporting terahertz (THz) radiation, where the guiding mode is radially polarized surface Sommerfeld waves. In this study, we demonstrate high-efficiency coupling of a broadband radially polarized THz pulsed beam, which is generated with a polarization-controlled beam by a segmented half-wave-plate mode converter, to bare copper wires. A total coupling efficiency up to 16.8% is observed, and at 0.3 THz, the maximum coupling efficiency is 66.3%. The results of mode-overlap calculation and numerical simulation support the experimental data well.

Surface-plasmon enhanced optical activity in two-dimensional metal chiral networks.

We investigated the optical properties of a novel chiral metamaterial; two-dimensional metal chiral networks formed from metal ribbons deposited on a dielectric substrate. For zeroth-order transmitted light, sharp optical resonances were observed at spectral positions, which are determined by the surface plasmon resonance frequencies of the periodic metal structures. The experimental results are in excellent agreement with numerical calculations.

Terahertz vector beam generation using segmented nonlinear optical crystals with threefold rotational symmetry.

We propose and demonstrate a simple method for cylindrical vector beam generation in the terahertz frequency region using optical rectification in segmented nonlinear crystals with threefold rotational symmetry. We used segmented GaP(111) plates to generate the terahertz cylindrical vector beam, and obtained clear evidence of the beam generation with a terahertz camera. By this method, a broadband terahertz cylindrical vector beam can be generated, and the radial and azimuth modes can be easily switched. We also report on the direct observation of the longitudinal electric field components at the focal point using a terahertz time-domain spectroscopy technique.

Dynamics of photo-induced terahertz optical activity in metal chiral gratings.

We investigated the dynamics of photo-induced optical activity of metal chiral gratings on an Si substrate for terahertz (THz) waves. We employed a new technique that enables optical-pump and THz-probe measurements via broadband THz spectroscopy at the microsecond time scale using a low-repetition-rate pump and a high-repetition-rate probe. We revealed that the THz optical activity decays as a result of the carrier diffusion effect because this optical activity is because of the presence of three-dimensional chiral structures of photo-carriers in the Si substrate.

The vectorial control of magnetization by light.

Application of coherent light-matter interactions has recently been extended to the ultrafast control of magnetization. An important but unrealized technique is the manipulation of magnetization vector motion to make it follow an arbitrarily designed multidimensional trajectory. Here we demonstrate a full manipulation of two-dimensional magnetic oscillations in antiferromagnetic NiO with a pair of polarization-twisted femtosecond laser pulses. We employ Raman-type nonlinear optical processes, wherein magnetic oscillations are impulsively induced with a controlled initial phase. Their azimuthal angle follows well-defined selection rules that have been determined by the symmetries of the materials. We emphasize that the temporal variation of the laser-pulse polarization angle enables us to control the phase and amplitude of the two degenerate modes, independently. These results lead to a new concept of the vectorial control of magnetization by light.

Circularly polarized light emission from semiconductor planar chiral nanostructures.

We demonstrate circularly polarized light emission from InAs quantum dots embedded in the waveguide region of a GaAs-based chiral nanostructure. The observed phenomenon originates due to a strong imbalance between left- and right-circularly polarized components of the vacuum field and results in a degree of polarization as high as 26% at room temperature. A strong circular anisotropy of the vacuum field modes inside the chiral nanostructure is visualized using numerical simulation. The results of the simulation agree well with experimental results.

Light-induced terahertz optical activity.

We propose and demonstrate a simple method to induce optical activity in the terahertz (THz) region using photoexcited carriers in a semiconductor substrate with metal two-dimensional chiral masks, which does not show optical activity without photoexcitation. The three-dimensional chirality induced by the combination of photocarriers and metal mask gives rise to the optical activity. With this simple method, we can develop THz polarization modulation techniques applicable for biology, chemistry, and material sciences.

Mechanism of the large polarization rotation effect in the all-dielectric artificially chiral nanogratings.

The physical mechanism of the large polarization rotation effect in direct transmission of the all-dielectric artificially chiral nanogratings is explored by experiment and numerical analysis. It is shown that the different coupling of right- and left-circularly polarized components of the normally incident light to the leaky guided modes or Fabry-Pérot resonance modes lead to the enhanced circular dichroism, resulting in the giant polarization rotation effect. The mode profile and local field calculations demonstrate intuitive images of the different coupling performance at resonances.