Publication database
A primary radiation standard based on quantum nonlinear optics
The black body remains the most prominent source of light for absolute radiometry. Its main alternative, synchrotron radiation, requires costly and large facilities. Quantum optics offers a new radiometric source: parametric down-conversion (PDC), a nonlinear optical process, in which pairwise photon correlations enable absolute calibration of photodetectors. Since the emission rate crucially depends on the brightness of the electromagnetic field, quantum-mechanical fluctuations of the vacuum can be seen as a seed of spontaneous PDC, and their amplitude is a natural radiometric standard. Thus, they allow for the calibration of the spectral radiance of light sources by measuring the ratio between seeded and unseeded PDC. Here, we directly use the frequency spectrum of the electromagnetic vacuum to trigger spontaneous PDC and employ the generated light to infer the spectral response of a spectrometer over a broad spectral range. Then, we deduce the absolute quantum efficiency from the spectral shape of PDC in the high-gain regime, without relying on a seed or reference detector. Our results compare well with the ones obtained with a reference lamp, demonstrating a promising primary radiation standard.
Aggregation states of poly (4-methylpentene-1) at a solid interface
A thin film of poly(4-methylpentene-1) (P4MP1) was prepared on a quartz substrate, which was a model system of an interface in filler-reinforced semicrystalline polymer composites. Grazing-incidence wide-angle X-ray diffraction measurements revealed that P4MP1 in the thin film after isothermal crystallization formed a Form I crystal polymorph composed of a tetragonal unit cell with a 72 helix, in which the chain axis was oriented along the direction parallel to the quartz interface. Combining sum-frequency generation vibrational spectroscopy with molecular dynamics simulation enabled us to gain access to the local conformation of P4MP1 chains at the quartz interface and the changes that occurred with isothermal crystallization. Finally, the way in which the initial chain orientation at the substrate interface impacted the crystalline structure in the thin film was discussed.
Black phosphorene as a hole extraction layer boosting solar water splitting of oxygen evolution catalysts
As the development of oxygen evolution co-catalysts (OECs) is being actively undertaken, the tailored integration of those OECs with photoanodes is expected to be a plausible avenue for achieving highly efficient solar-assisted water splitting. Here, we demonstrate that a black phosphorene (BP) layer, inserted between the OEC and BiVO4 can improve the photoelectrochemical performance of pre-optimized OEC/BiVO4 (OEC: NiOOH, MnOx, and CoOOH) systems by 1.2∼1.6-fold, while the OEC overlayer, in turn, can suppress BP self-oxidation to achieve a high durability. A photocurrent density of 4.48 mA·cm−2 at 1.23 V vs reversible hydrogen electrode (RHE) is achieved by the NiOOH/BP/BiVO4 photoanode. It is found that the intrinsic p-type BP can boost hole extraction from BiVO4 and prolong holes trapping lifetime on BiVO4 surface. This work sheds light on the design of BP-based devices for application in solar to fuel conversion, and also suggests a promising nexus between semiconductor and electrocatalyst.
Considerable matrix shift in the electronic transitions of helium-solvated cesium dimer cation Cs2He+n
We investigate the photodissociation of helium-solvated cesium dimer cations using action spectroscopy and quantum chemical calculations. The spectrum of Cs2He+ shows three distinct absorption bands into both bound and dissociative states. Upon solvation with further helium atoms, considerable shifts of the absorption bands are observed, exceeding 0.1 eV (850 cm−1) already for Cs2He10+, along with significant broadening. The shifts are highly sensitive to the character of the excited state. Our calculations show that helium atoms adsorb on the ends of Cs2+. The shifts are particularly pronounced if the excited state orbitals extend to the area occupied by the helium atoms. In this case, Pauli repulsion leads to a deformation of the excited state orbitals, resulting in the observed blue shift of the transition. Since the position of the weakly bound helium atoms is ill defined, Pauli repulsion also explains the broadening.
Contrast agent enhanced multimodal photoacoustic microscopy and optical coherence tomography for imaging of rabbit choroidal and retinal vessels in vivo
Multimodal imaging with photoacoustic microscopy (PAM) and optical coherence tomography (OCT) can be an effective method to evaluate the choroidal and retinal microvasculature. To improve the efficiency for visualizing capillaries, colloidal gold nanoparticles (AuNPs) have been applied as a multimodal contrast agent for both OCT and PAM imaging by taking advantage of the strong optical scattering and the strong optical absorption of AuNPs due to their surface plasmon resonance. Ultra-pure AuNPs were fabricated by femtosecond laser ablation, capped with polyethylene glycol (PEG), and administered to 13 New Zealand white rabbits and 3 Dutch Belted pigmented rabbits. The synthesized PEG-AuNPs (20.0 ± 1.5 nm) were demonstrated to be excellent contrast agents for PAM and OCT, and do not demonstrate cytotoxicity to bovine retinal endothelial cells in cell studies. The image signal from the retinal and choroidal vessels in living rabbits was enhanced by up to 82% for PAM and up to 45% for OCT, respectively, by the administered PEG-AuNPs, which enables detection of individual blood vessels by both imaging modalities. The biodistribution study demonstrated the AuNP accumulated primarily in the liver and spleen. Histology and TUNEL staining did not indicate cell injury or death in the lung, liver, kidney, spleen, heart, or eyes up to seven days after AuNP administration. PEG-AuNPs offer an efficient and safe contrast agent for multimodal ocular imaging to achieve improved characterization of microvasculature.
Electronic spectroscopy and nanocalorimetry of hydrated magnesium ions [Mg(H2O)n]+, n = 20–70: spontaneous formation of a hydrated electron?
Hydrated singly charged magnesium ions [Mg(H2O)n]+ are thought to consist of an Mg2+ ion and a hydrated electron for n > 15. This idea is based on mass spectra, which exhibit a transition from [MgOH(H2O)n−1]+ to [Mg(H2O)n]+ around n = 15–22, black-body infrared radiative dissociation, and quantum chemical calculations. Here, we present photodissociation spectra of size-selected [Mg(H2O)n]+ in the range of n = 20–70 measured for photon energies of 1.0–5.0 eV. The spectra exhibit a broad absorption from 1.4 to 3.2 eV, with two local maxima around 1.7–1.8 eV and 2.1–2.5 eV, depending on cluster size. The spectra shift slowly from n = 20 to n = 50, but no significant change is observed for n = 50–70. Quantum chemical modeling of the spectra yields several candidates for the observed absorptions, including five- and six-fold coordinated Mg2+ with a hydrated electron in its immediate vicinity, as well as a solvent-separated Mg2+/e− pair. The photochemical behavior resembles that of the hydrated electron, with barrierless interconversion into the ground state following the excitation.
Engineering electrochemical sensors using nanosecond laser treatment of thin gold film on ITO glass
Direct generation of gold nanoparticles on ITO glass using a nanosecond laser is presented and the electrochemical properties of the gold modified ITO electrodes for detection of the ascorbic acid are analyzed. Gold nanoparticles were generated by nanosecond laser pulse irradiation of thin, 3–30 nm thick, gold films. It was found that diameters and the number of generated nanoparticles per unit area strongly depends on the thickness of the gold film when it is less than 10 nm. Furthermore, experiments have shown that the influence of laser processing parameters (the laser pulse energy and pulse number) to the size, the distribution and the area density of generated gold nanoparticles on ITO glass is negligible. Characterization of the electrochemical properties of the gold modified ITO electrodes by nanosecond laser showed that the fabricated electrodes could be employed in electrochemical sensing. Therefore, the demonstrated generation of gold nanoparticles on ITO by using the nanosecond laser approach opens new opportunities for the development of highly sensitive and low-cost electrochemical sensors.
Glass dicing with elliptical Bessel beam
In this paper the possibility to optimize the glass dicing process by controlling the axicon-generated Bessel beam ellipticity is presented. Single-shot intra-volume modifications in soda-lime glass followed by dicing experiments of 1 mm-thick samples are performed. The Bessel beam ellipticity is essential for glass dicing process. Such beam generates intra-volume modifications with transverse crack propagation in dominant direction. Orientation of these modifications parallel to the dicing direction gives significant advantages in terms of processing speed, glass breaking force and cutting quality.
High-efficiency laser fabrication of drag reducing riblet surfaces on pre-heated Teflon
Bio-inspired surfaces are able to decrease friction with fluids and gases. The most recognizable are shark-skin-like riblet surface structures. Such bio-inspired surfaces can be formed by the laser ablation technique. In this work, bio-inspired riblet surfaces with grooves were formed using picosecond ultraviolet laser ablation on pre-heated polytetrafluoroethylene (PTFE) at various sample temperatures. The ablation of hot PTFE was found to be 30% more efficient than the conventional laser structuring at the room temperature. The friction of structured PTFE surfaces with the flowing air was investigated by using drag a measurement setup. Results show the decrease of friction force by 6% with dimensionless riblet spacing around 14–20.
High-performance all-organic DFB and DBR waveguide laser with various grating height fabricated by a two-photon absorption DLW method
Organic solid-state lasers (OSSLs) with distributed feedback (DFB) structures or distributed Bragg reflectors (DBRs) are promising for potential application in bio-sensing and hazardous materials detection. Here, the laser performances of the all-organic DFB waveguide lasers with various grating heights ranging from 0.4 to 4.7 μm were investigated. The grating structures used as the lasing cavity were fabricated using a two-photon absorption (TPA) direct laser writing (DLW) method with an SU-8 negative photoresist. The laser active layer consisted of a rhodamine 6G (R6G) laser dye and a cellulose acetate (CA) matrix. The R6G/CA solution was spin-coated onto the quartz substrate with the cavity (grating) structures to fabricate the DFB waveguide laser devices. The diffraction order of lasing ranged from m = 4 to 7. As the grating height was increased to 1.9 μm, the slope efficiency increased for all diffraction orders and the threshold decreases for each diffraction order. The dependence of the cavity (grating) length on the laser performances was investigated. The slope efficiency increased as the cavity length increased to 300 μm. The effect of the cavity (grating) position on the slope efficiency and the threshold position of the cavity (grating) was also studied. A maximum slope efficiency of 10.2% was achieved for the DFB waveguide laser device with a cavity (grating) length of 300 μm, a cavity position at 6 mm from the emission edge of the waveguide, and an aspect ratio ≈3 between the grating height of 1.74 μm and the grating width of 0.6 μm for the diffraction order m = 6 for lasing.