Influence of Surface Basic Sites and Oxygen Vacancies on the Performance of Metal-Modified Rod-Like Ceria Catalysts for Low-Temperature Hydrolysis of Carbonyl Sulfide.

This study utilized a hydrothermal method to synthesize various metal-modified rod-like ceria catalysts (Fe, Co, Cu, Ni, La), achieving efficient COS removal at low temperatures. The research identified surface oxygen vacancies and basic sites as critical factors that influence the catalytic performance of COS hydrolysis. The addition of different metals to pristine ceria rods increased the specific surface area, oxygen vacancy content (Ov), and basicity, which enhanced the catalysts' sulfur resistance and stability. Among all the catalysts tested, 10La-CeO2 demonstrated the highest COS removal rate. This is because La doping significantly augmented Ov, providing more H2O adsorption and activation sites. Furthermore, 10La-CeO2 showed enhanced Lewis basicity, making it easier for COS to adsorb and promote hydrolysis. The in situ DRIFTS results confirmed that appropriate oxygen vacancies and basic sites favored the formation of intermediates such as HCO3 - and HSCO2 -, promoting the decomposition of COS into H2S and CO2.

Wide-field mid-infrared hyperspectral imaging beyond video rate.

Mid-infrared hyperspectral imaging has become an indispensable tool to spatially resolve chemical information in a wide variety of samples. However, acquiring three-dimensional data cubes is typically time-consuming due to the limited speed of raster scanning or wavelength tuning, which impedes real-time visualization with high spatial definition across broad spectral bands. Here, we devise and implement a high-speed, wide-field mid-infrared hyperspectral imaging system relying on broadband parametric upconversion of high-brightness supercontinuum illumination at the Fourier plane. The upconverted replica is spectrally decomposed by a rapid acousto-optic tunable filter, which records high-definition monochromatic images at a frame rate of 10 kHz based on a megapixel silicon camera. Consequently, the hyperspectral imager allows us to acquire 100 spectral bands over 2600-4085 cm-1 in 10 ms, corresponding to a refreshing rate of 100 Hz. Moreover, the angular dependence of phase matching in the image upconversion is leveraged to realize snapshot operation with spatial multiplexing for multiple spectral channels, which may further boost the spectral imaging rate. The high acquisition rate, wide-field operation, and broadband spectral coverage could open new possibilities for high-throughput characterization of transient processes in material and life sciences.

Giant enhancement of fluorescence resonance energy transfer based on nanoporous gold with small amount of residual silver.

Fluorescence resonance energy transfer (FRET) was found strongly enhanced by plasmon resonance. In this work, Nanoporous Gold with small amount of residual silver was used to form nanoporous gold/organic molecular layer compound with PSS and PAH. The ratio of its specific gold and silver content is achieved by controlling the time of its dealloying. Layered films of polyelectrolyte multilayers were assembled between the donor-acceptor pairs and NPG films to control distance. The maximum of FRET enhancement of 80-fold on the fluorescence intensity between the donor-acceptor pairs (CFP-YFP) is observed at a distance of ∼10.5 nm from the NPG film. This Nanoporous Gold with small amount of residual silver not only enhanced FRET 4-fold more than nanoporous gold of only gold content almost, but also effectively realized the regulation of FRET enhancement. The ability to precisely measure and regulate the enhancement of FRET enables the rational selection of plasmonic nanotransducer dimensions for the particular biosensing application.

Enhanced sequestration of CO2 from simulated electrolytic aluminum flue gas by modified red mud.

The aluminum industry is facing severe economic and environmental problems due to increasing carbon emissions and growing stockpiles of red mud (RM). RM is a strongly alkaline, high-emission solid waste from the alumina industry with potential for CO2 sequestration. However, the effectiveness of RM carbon sequestration is poor, and the mechanism behind it is not well understood. In this study, the effect of microwave and tube furnace activation of RM on CO2 sequestration in alumina was first investigated at different temperatures. The result showed that the CO2 sequestration capacity of unmodified RM (URM) was only 14.35 mg/g at ambient temperature and pressure, and the CO2 sequestration capacity could be increased to 52.89 mg/g after high-temperature activation and modification. Besides, high-temperature activation and modification will effectively improve the carbon sequestration capacity of RM. The carbonized RM was characterized by FT-IR, SEM, XRD, laser particle size, TG-DSC, and pH measurements. In addition, the mechanism of RM capturing CO2 was also proposed, which shows that CO2 was finally sequestered in the RM as CaCO3. The change in particle size distribution and the mineral phase in the RM indicated that high-temperature activation modification positively affects the application of RM to the sequestration of CO2. This study can provide a promising technology for the low-carbon and green development of the aluminum industry, as well as achieving the waste treatment and utilization objective.

Dual-comb optomechanical spectroscopy.

Optical cavities are essential for enhancing the sensitivity of molecular absorption spectroscopy, which finds widespread high-sensitivity gas sensing applications. However, the use of high-finesse cavities confines the wavelength range of operation and prevents broader applications. Here, we take a different approach to ultrasensitive molecular spectroscopy, namely dual-comb optomechanical spectroscopy (DCOS), by integrating the high-resolution multiplexing capabilities of dual-comb spectroscopy with cavity optomechanics through photoacoustic coupling. By exciting the molecules photoacoustically with dual-frequency combs and sensing the molecular-vibration-induced ultrasound waves with a cavity-coupled mechanical resonator, we measure high-resolution broadband ( > 2 THz) overtone spectra for acetylene gas and obtain a normalized noise equivalent absorption coefficient of 1.71 × 10-11 cm-1·W·Hz-1/2 with 30 GHz simultaneous spectral bandwidth. Importantly, the optomechanical resonator allows broadband dual-comb excitation. Our approach not only enriches the practical applications of the emerging cavity optomechanics technology but also offers intriguing possibilities for multi-species trace gas detection.

Mid-infrared single-photon 3D imaging.

Active mid-infrared (MIR) imagers capable of retrieving three-dimensional (3D) structure and reflectivity information are highly attractive in a wide range of biomedical and industrial applications. However, infrared 3D imaging at low-light levels is still challenging due to the deficiency of sensitive and fast MIR sensors. Here we propose and implement a MIR time-of-flight imaging system that operates at single-photon sensitivity and femtosecond timing resolution. Specifically, back-scattered infrared photons from a scene are optically gated by delay-controlled ultrashort pump pulses through nonlinear frequency upconversion. The upconverted images with time stamps are then recorded by a silicon camera to facilitate the 3D reconstruction with high lateral and depth resolutions. Moreover, an effective numerical denoiser based on spatiotemporal correlation allows us to reveal the object profile and reflectivity under photon-starving conditions with a detected flux below 0.05 photons/pixel/second. The presented MIR 3D imager features high detection sensitivity, precise timing resolution, and wide-field operation, which may open new possibilities in life and material sciences.

Volume plasma grating by noncollinear interaction of femtosecond filament arrays.

Stable propagation of multifilament arrays in transparent bulk media with adjustable separation distances between adjacent child filaments has always been desired for advanced manufacturing. Here, we report on the generation of an ionization-induced volume plasma grating (VPG) by the interaction of two batches of noncollinearly propagating arrays of multiple filaments (AMF). The VPG can externally arrange the propagation of the pulses along regular plasma waveguides via spatial reconstruction of electrical fields, which is compared with the self-formation of randomly distributed multiple filamentation originated from noises. The separation distances of filaments in VPG are controllable by readily changing the crossing angle of the excitation beams. In addition, an innovative method to efficiently fabricate multidimensional grating structures in transparent bulk media through laser modification using VPG was demonstrated.

Free-Running Single-Photon Detection via GHz Gated InGaAs/InP APD for High Time Resolution and Count Rate up to 500 Mcount/s.

Free-running InGaAs/InP single-photon avalanche photodiodes (SPADs) typically operate in the active-quenching mode, facing the problems of long dead time and large timing jitter. In this paper, we demonstrate a 1-GHz gated InGaAs/InP SPAD with the sinusoidal gating signals asynchronous to the incident pulsed laser, enabling free-running single-photon detection. The photon-induced avalanche signals are quenched within 1 ns, efficiently reducing the SPAD's dead time and achieving a count rate of up to 500 Mcount/s. However, the timing jitter is measured to be ~168 ps, much larger than that of the SPAD with synchronous gates. We adjust the delay between the gating signals and the incident pulsed laser to simulate the random arrival of the photons, and record the timing jitter, respectively, to figure out the cause of the jitter deterioration. In addition, the effects of the incident laser power and working temperature of the APD on the time resolution have been investigated, broadening the applications of the GHz gated free-running SPAD in laser ranging and imaging, fluorescence spectroscopy detection and optical time-domain reflectometry.

Mid-infrared single-pixel imaging at the single-photon level.

Single-pixel cameras have recently emerged as promising alternatives to multi-pixel sensors due to reduced costs and superior durability, which are particularly attractive for mid-infrared (MIR) imaging pertinent to applications including industry inspection and biomedical diagnosis. To date, MIR single-pixel photon-sparse imaging has yet been realized, which urgently calls for high-sensitivity optical detectors and high-fidelity spatial modulators. Here, we demonstrate a MIR single-photon computational imaging with a single-element silicon detector. The underlying methodology relies on nonlinear structured detection, where encoded time-varying pump patterns are optically imprinted onto a MIR object image through sum-frequency generation. Simultaneously, the MIR radiation is spectrally translated into the visible region, thus permitting infrared single-photon upconversion detection. Then, the use of advanced algorithms of compressed sensing and deep learning allows us to reconstruct MIR images under sub-Nyquist sampling and photon-starving illumination. The presented paradigm of single-pixel upconversion imaging is featured with single-pixel simplicity, single-photon sensitivity, and room-temperature operation, which would establish a new path for sensitive imaging at longer infrared wavelengths or terahertz frequencies, where high-sensitivity photon counters and high-fidelity spatial modulators are typically hard to access.

Terahertz Time-of-Flight Ranging with Adaptive Clock Asynchronous Optical Sampling.

We propose and implement a terahertz time-of-flight ranging system based on adaptive clock asynchronous optical sampling, where the timing jitter is corrected in real time to recover the depth information in the acquired interferograms after compensating for laser instabilities using electronic signal processing. Consequently, the involved measurement uncertainties caused by the timing jitter during the terahertz sampling process and the noise intensity of the terahertz electric field have been reduced by the utilization of the adaptive clock. The achieved uncertainty range is about 2.5 µm at a 5 cm distance after averaging the acquisition time of 1876 ms 5000 times, showing a significant improvement compared with the asynchronous optical sampling using a constant clock. The implemented terahertz ranging system only uses free-running mode-locked lasers without any phase-locked electronics, and this favors simple and robust operations for subsequent applications that extend beyond the laboratory conditions.

Synchronization, Desynchronization, and Intermediate Regime of Breathing Solitons and Soliton Molecules in a Laser Cavity.

We report on the experimental and numerical observations of synchronization and desynchronization of bound states of multiple breathing solitons (breathing soliton molecules) in an ultrafast fiber laser. In the desynchronization regime, although the breather molecules as wholes are not synchronized to the cavity, the individual breathers within a molecule are synchronized to each other with a delay (lag synchronization). An intermediate regime between the synchronization and desynchronization phases is also observed, featuring self-modulation of the synchronized state. This regime may also occur in other systems displaying synchronization. Breathing soliton molecules in a laser cavity open new avenues for the study of nonlinear synchronization dynamics.

Farey tree and devil's staircase of frequency-locked breathers in ultrafast lasers.

Nonlinear systems with two competing frequencies show locking or resonances. In lasers, the two interacting frequencies can be the cavity repetition rate and a frequency externally applied to the system. Conversely, the excitation of breather oscillations in lasers naturally triggers a second characteristic frequency in the system, therefore showing competition between the cavity repetition rate and the breathing frequency. Yet, the link between breathing solitons and frequency locking is missing. Here we demonstrate frequency locking at Farey fractions of a breather laser. The winding numbers exhibit the hierarchy of the Farey tree and the structure of a devil's staircase. Numerical simulations of a discrete laser model confirm the experimental findings. The breather laser may therefore serve as a simple test bed to explore ubiquitous synchronization dynamics of nonlinear systems. The locked breathing frequencies feature a high signal-to-noise ratio and can give rise to dense radio-frequency combs, which are attractive for applications.

Ultra-rapid dual-comb ranging with an extended non-ambiguity range.

In this Letter, we report a scheme that combines time-of-flight (ToF) ranging detection of multi-repetition-rate pulses with asymmetric dual-comb ranging (DCR) measurement. Notably, this combination extends the non-ambiguity range (NAR) of the DCR method without sacrificing its refresh rate and distance precision. With this scheme, we demonstrate absolute distance measurement of moving targets with an NAR of 1.5 km, which is 5× larger than that allowed solely by the DCR method for a given refresh rate at 500 kHz. The ranging precision in a single measurement of 2 µs reaches 10 µm at an effective distance of 571 m (down to 60 nm in 0.1 s). This combined scheme benefits remote sensing of high-speed objects.

Dual-comb quartz-enhanced photoacoustic spectroscopy.

Photoacoustic spectroscopy (PAS) using two optical combs is a new-born technique, offering appealing features, including broad optical bandwidths, high resolutions, fast acquisition speeds, and wavelength-independent photoacoustic detection, for chemical sensing. However, its further application to, e.g., trace detection, is jeopardized due to the fundamentally and technically limited sensitivity and specificity. Here, we take a different route to comb-enabled PAS with acoustically enhanced sensitivity and nonlinear spectral hole-burning defined resolution. We demonstrate dual-comb quartz-enhanced PAS with two near-infrared electro-optic combs and a quartz tuning fork. Comb-line-resolved multiplexed spectra are acquired for acetylene with a single-pass detection limit at the parts-per-billion level. The technique is further extended to the mid-infrared (for methane), enabling improved sensitivity. More importantly, we measure nonlinear dual-comb photoacoustic spectra for the 12C2H2 ν1 + ν3 band P(17) transition with sub-Doppler pressure-broadening dominated homogeneous linewidths (e.g., 45.8 MHz), hence opening up new opportunities for Doppler-free photoacoustic gas sensing.

Optical Bistability in a Tunable Gourd-Shaped Silicon Ring Resonator.

In this study, a tunable gourd-shaped ring resonator is demonstrated to generate optical bistability. The system consists of two sub-rings for a gourd shape configuration with a U-shaped wave guiding pathway. The transfer matrix method and FDTD simulation are used to acquire the spectral characteristics of the system. For the fabricated device, the spectra profile and extinction ratio can be effectively tuned by the microheater above the U-shaped waveguide, which matches with the theoretical results. Due to the gourd structure of the resonator, the light waves in two rings can be cross-coupled with each other, and the optical bistability could come out effectively with the change in the input optical power around 6 mW. The presented optical bistability devices have great application potential in optical information processing such as optical storage, switch and logic operation.

Special Issue: State-of-the-Art Nanophotonic and Optical Nanomaterials in China.

In recent years, the fields of nanophotonics and nano-optics have been greatly fueled by rapid advancements in photonic science and technology, especially by the emergence of novel optical nanomaterials and new functional nanostructures [...].

Carbon-Assistant Nanoporous Gold for Surface-Enhanced Raman Scattering.

Surface-enhanced Raman scattering (SERS) technology can amplify the Raman signal due to excited localized surface plasmon (LSP) from SERS substrates, and the properties of the substrate play a decisive role for SERS sensing. Several methods have been developed to improve the performance of the substrate by surface modification. Here, we reported a surface modification method to construct carbon-coated nanoporous gold (C@NPG) SERS substrate. With surface carbon-assistant, the SERS ability of nanoporous gold (NPG) seriously improved, and the detection limit of the dye molecule (crystal violet) can reach 10-13 M. Additionally, the existence of carbon can avoid the deformation of the adsorbed molecule caused by direct contact with the NPG. The method that was used to improve the SERS ability of the NPG can be expanded to other metal structures, which is a convenient way to approach a high-performance SERS substrate.

Wide-field mid-infrared single-photon upconversion imaging.

Frequency upconversion technique, where the infrared signal is nonlinearly translated into the visible band to leverage the silicon sensors, offers a promising alternation for the mid-infrared (MIR) imaging. However, the intrinsic field of view (FOV) is typically limited by the phase-matching condition, thus imposing a remaining challenge to promote subsequent applications. Here, we demonstrate a wide-field upconversion imaging based on the aperiodic quasi-phase-matching configuration. The acceptance angle is significantly expanded to about 30°, over tenfold larger than that with the periodical poling crystal. The extended FOV is realized in one shot without the need of parameter scanning or post-processing. Consequently, a fast snapshot allows to facilitate high-speed imaging at a frame rate up to 216 kHz. Alternatively, single-photon imaging at room temperature is permitted due to the substantially suppressed background noise by the spectro-temporal filtering. Furthermore, we have implemented high-resolution time-of-flight 3D imaging based on the picosecond optical gating. These presented MIR imaging features with wide field, fast speed, and high sensitivity might stimulate immediate applications, such as non-destructive defect inspection, in-vivo biomedical examination, and high-speed volumetric tomography.

Passive repetition-rate stabilization for a mode-locked fiber laser by electro-optic modulation.

We report a passive stabilization of the repetition rate for a mode-locked fiber laser by using an electro-optic modulator in a phase-biased nonlinear amplifying loop mirror. The underlying mechanism, in contrast to active feedback operations, lies in the cross-phase modulation between electrical and optical pulses within an electro-optic crystal. The resulting spectral shift can automatically compensate for the cavity-length drift via the group velocity dispersion. Consequently, the artificial actuator enables a capture range up to 2.3 mm, much longer than that achieved by index changes of the modulator. A robust and tight locking for the repetition rate is then realized with a standard deviation as low as 9 µHz with a 1-s sample time over 11 hours, corresponding to a fractional instability of 4.3 × 10-13. Furthermore, a dynamic optical sampling by repetition-rate tuning has been manifested with a fast refresh rate at 100 kHz and a broad scanning range over 305 ps. The demonstrated passive servo action may provide a simple yet effective way to stabilize the repetition rate with high precision, large bandwidth, and wide tunability.

Hydrogenated Amorphous Titania with Engineered Surface Oxygen Vacancy for Efficient Formaldehyde and Dye Removals under Visible-Light Irradiation.

Hydrogenated crystalized TiO2-x with oxygen vacant (OV) doping has attracted considerable attraction, owing to its impressive photoactivity. However, amorphous TiO2, as a common allotrope of titania, is ignored as a hydrogenated templet. In this work, hydrogenated amorphous TiO2-x (HAm-TiO2-x) with engineered surface OV and high surface area (176.7 cm2 g-1) was first prepared using a unique liquid plasma hydrogenation strategy. In HAm-TiO2-x, we found that OV was energetically retained in the subsurface region; in particular, the subsurface OV-induced energy level preferred to remain under the conduction band (0.5 eV) to form a conduction band tail and deep trap states, resulting in a narrow bandgap (2.36 eV). With the benefits of abundant light absorption and efficient photocarrier transportation, HAm-TiO2-x coated glass has demonstrated superior visible-light-driven self-cleaning performances. To investigate its formaldehyde photodegradation under harsh indoor conditions, HAm-TiO2-x was used to decompose low-concentration formaldehyde (~0.6 ppm) with weak-visible light (λ = 600 nm, power density = 0.136 mW/cm2). Thus, HAm-TiO2-x achieved high quantum efficiency of 3 × 10-6 molecules/photon and photoactivity of 92.6%. The adsorption capabilities of O2 (-1.42 eV) and HCHO (-1.58 eV) in HAm-TiO2-x are both largely promoted in the presence of subsurface OV. The surface reaction pathway and formaldehyde decomposition mechanism over HAm-TiO2-x were finally clarified. This work opened a promising way to fabricate hydrogenated amorphous photocatalysts, which could contribute to visible-light-driven photocatalytic environmental applications.