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We present a new design of a robust cavity-enhanced frequency comb-based spectrometer operating under the continuous-filtering Vernier principle. The spectrometer is based on a compact femtosecond Er-doped fiber laser, a medium finesse cavity, a diffraction grating, a custom-made moving aperture, and two photodetectors. The new design removes the requirement for high-bandwidth active stabilization present in the previous implementations of the technique, and allows scan rates up to 100 Hz. We demonstrate the spectrometer performance over a wide spectral range by detecting CO2 around 1575 nm (1.7 THz bandwidth and 6 GHz resolution) and CH4 around 1650 nm (2.7 THz bandwidth and 13 GHz resolution). We achieve absorption sensitivity of 5 × 10−9 cm-1 Hz-1/2 at 1575 nm, and 1 × 10−7 cm-1 Hz-1/2 cm-1 at 1650 nm. We discuss the influence of the scanning speed above the adiabatic limit on the amplitude of the absorption signal.

The mutual neutralisation of O+ with O- has been studied in a double ion-beam storage ring with combined merged-beams, imaging and timing techniques. Branching ratios were measured at the collision energies of 55, 75 and 170 (+/- 15) meV, and found to be in good agreement with previous single-pass merged-beams experimental results at 7 meV collision energy. Several previously unidentified spectral features were found to correspond to mutual neutralisation channels of the first metastable state of the cation (O+(D-2(o)), tau approximate to 3.6 hours), while no contributions from the second metastable state (O+(P-2(o)), tau approximate to 5 seconds) were observed. Theoretical calculations were performed using the multi-channel Landau-Zener model combined with the anion centered asymptotic method, and gave good agreement with several experimentally observed channels, but could not describe well observed contributions from the O+(D-2(o)) metastable state as well as channels involving the O(3s S-5(o)) state.

A transportable refractometer for assessment of kPa pressures with ppm level precision is presented. It is based on the GAs MOdulation Refractometry (GAMOR) methodology, making it resistant to fluctuations and drifts. At the National Metrology Institute at RISE, Sweden, the system assessed pressures in the 4.3 - 8.7 kPa range with sub-ppm precision (0.5 - 0.9 ppm). The system was thereafter disassembled, packed, and transported 1040 km to Umea University, where it, after unpacking and reassembling, demonstrated a similar precision (0.8 - 2.1 ppm). This shows that the system can be disassembled, packed, transported, unpacked, and reassembled with virtually unchanged performance.

We present experimental results of fluctuation-enhanced gas sensing by low-cost resistive sensors made of a mixture of graphene flakes and TiO2 nanoparticles. Both components are photocatalytic and activated by UV light. Two UV LEDs of different wavelengths (362 and 394 nm) were applied to modulate the gas sensing of the layers. Resistance noise was recorded at low frequencies, between 8 Hz and 10 kHz. The sensors’ response was observed in an ambient atmosphere of synthetic air and toxic NO2 at selected concentrations (5, 10, and 15 ppm). We observed that flicker noise changed its frequency dependence at different UV light wavelengths, thereby providing additional information about the ambient atmosphere. The power spectral density changed by a few times as a result of UV light irradiation. The sensors were operated at 60 and 120°C, and the effect of UV light on gas sensing was most apparent at low operating temperature. We conclude that UV light activates the gas-sensing layer and improves gas detection at low concentrations of NO2. This result is desirable for the detection of the components of gas mixtures, and the modulated sensor can replace an array of independent resistive sensors which would consume much more energy for heating. We also suggest that a more advanced technology for preparing the gas-sensing layer, by use of spin coating, will produce corresponding layers with thickness of about a few μm, which is about ten times less than that for the tested samples. The effects induced by the applied UV light, having a penetration depth of only a few μm, would then be amplified.

A multipurpose and ultra-compact nanoplasmonic wavelength filter based on stub structure in a metal-insulator-metal (MIM) waveguide is suggested and numerically investigated. A novel approach of connecting two stepped-like apertures to both input and output ports is applied to form Fabry-Perot (FP) cavities, which enabled the structure to act as a dual band-pass filter at wavelengths 1310 nm and 1550 nm. It is shown that the variation in cavities' length allows to realize a long-wavelength cutoff filter, and cutoff wavelength can be easily tuned by adjusting the length of the cavities. Furthermore, it is revealed that increasing the gap between the stepped-like apertures and the cavities provides a triple band-pass at telecom wavelengths, e.g., 1267.5 nm, 1414.19 nm, and 1644.7 nm. The tunable broadband high-pass wavelength filter is then achieved while the lengths of stepped-like apertures and stub resonators are set to be identical. Finally, a tunable nearly perfect absorber can be obtained by varying the width of stub resonators. Therefore, because of functionality, size, as well as efficiency the proposed plasmonic filter may greatly contribute to miniaturization of next generation of photonic integrated circuits (PICs), and find applications in on-chip integration and wavelength-division multiplexing (WDM) in optical communication systems.

Approximately 90% of cancers have their origins in epithelial tissues and this leads to epithelial thickening, but the ultrastructural changes and underlying architecture is less well known. Depth resolved label free visualization of nanoscale tissue morphology is required to reveal the extent and distribution of ultrastructural changes in underlying tissue, but is difficult to achieve with existing imaging modalities. We developed a nanosensitive optical coherence tomography (nsOCT) approach to provide such imaging based on dominant axial structure with a few nanometre detection accuracy. nsOCT maps the distribution of axial structural sizes an order of magnitude smaller than the axial resolution of the system. We validated nsOCT methodology by detecting synthetic axial structure via numerical simulations. Subsequently, we validated the nsOCT technique experimentally by detecting known structures from a commercially fabricated sample. nsOCT reveals scaling with different depth of dominant submicron structural changes associated with carcinoma which may inform the origins of the disease, its progression and improve diagnosis., 7 pages, 4 figures

We present ultrabroadband two-beam femtosecond/picosecond coherent Raman spectroscopy on the ro-vibrational spectra of CO2 and O2, applied for multispecies thermometry and relative concentration measurements in a standard laminar premixed hydrocarbon flame. The experimental system employs fs-laser-induced filamentation to generate the compressed supercontinuum in-situ, resulting in a ∼24 fs full-width-at-half-maximum pump/Stokes pulse with sufficient bandwidth to excite all the ro-vibrational Raman transitions up to 1600 cm-1. We report the simultaneous recording of the ro-vibrational CO2 Q-branch and the ro-vibrational O2 O-, Q- and S-branch coherent Stokes Raman spectra (CSRS) on the basis of a single-laser-shot. The use of filamentation as the supercontinuum generation mechanism has the advantage of greatly simplifying the experimental setup, as it avoids the use of hollow-core fibres and chirped mirrors to deliver a near-transform-limited ultrabroadband pulse at the measurement location. Time-domain models for the ro-vibrational Q-branch spectrum of CO2 and the ro-vibrational O-, Q- and S-branch spectra of O2 were developed. The modelling of the CO2 Q-branch spectrum accounts for up to 180 vibrational bands and for their interaction in Fermi polyads, and is based on recently available, comprehensive calculations of the vibrational transition dipole moments of the CO2 molecule: the availability of spectroscopic data for these many vibrational bands is crucial to model the high-temperature spectra acquired in the flue gases of hydrocarbon flames, where the temperature can exceed 2000 K. The numerical code was employed to evaluate the CSRS spectra acquired in the products of a laminar premixed methane/air flame provided on a Bunsen burner, for varying equivalence ratio in the range 0.6–1.05. The performance of the CO2 spectral model is assessed by extracting temperatures from 40-laser-shots averaged spectra, resulting in thermometry accuracy and precision of ∼5% and ∼1%, respectively, at temperatures as high as 2220 K. Validerad;2022;Nivå 2;2022-03-02 (hanlid);Funder: Netherlands Organization for Scientific Research (15690)

Significance: For optical methods to accurately assess hemoglobin oxygen saturation in vivo, an independently verifiable tissue-like standard is required for validation. For this purpose, we propose three hemoglobin preparations and evaluate methods to characterize them. Aim: To spectrally characterize three different hemoglobin preparations using multiple spectroscopic methods and to compare their absorption spectra to commonly used reference spectra. Approach: Absorption spectra of three hemoglobin preparations in solution were characterized using spectroscopic collimated transmission: whole blood, lysed blood, and ferrous-stabilized hemoglobin. Tissue-mimicking phantoms composed of Intralipid, and the hemoglobin solutions were characterized using spatial frequency-domain spectroscopy (SFDS) and enhanced perfusion and oxygen saturation (EPOS) techniques while using yeast to deplete oxygen. Results: All hemoglobin preparations exhibited similar absorption spectra when accounting for methemoglobin and scattering in their oxyhemoglobin and deoxyhemoglobin forms, respectively. However, systematic differences were observed in the fitting depending on the reference spectra used. For the tissue-mimicking phantoms, SFDS measurements at the surface of the phantom were affected by oxygen diffusion at the interface with air, associated with higher values than for the EPOS system. Conclusions: We show the validity of different blood phantoms and what considerations need to be addressed in each case to utilize them equivalently. Funding: This research was financially supported by VINNOVA grants via the Swelife and MedTech4Health programs (Grant Nos. 2016-02211, 2017-01435, and 2019-01522) and the Knut and Alice Wallenberg Foundation’s Center for Molecular Medicine at Linköping University (WCMM).

Engineering a low singlet-triplet energy gap (ΔEST) is necessary for efficient reverse intersystem crossing (rISC) in delayed fluorescence (DF) organic semiconductors but results in a small radiative rate that limits performance in LEDs. Here, we study a model DF material, BF2, that exhibits a strong optical absorption (absorption coefficient = 3.8 × 105 cm−1) and a relatively large ΔEST of 0.2 eV. In isolated BF2 molecules, intramolecular rISC is slow (delayed lifetime = 260 μs), but in aggregated films, BF2 generates intermolecular charge transfer (inter-CT) states on picosecond timescales. In contrast to the microsecond intramolecular rISC that is promoted by spin-orbit interactions in most isolated DF molecules, photoluminescence-detected magnetic resonance shows that these inter-CT states undergo rISC mediated by hyperfine interactions on a ~24 ns timescale and have an average electron-hole separation of ≥1.5 nm. Transfer back to the emissive singlet exciton then enables efficient DF and LED operation. Thus, access to these inter-CT states, which is possible even at low BF2 doping concentrations of 4 wt%, resolves the conflicting requirements of fast radiative emission and low ΔEST in organic DF emitters., A low singlet-triplet energy gap, necessary for delayed fluorescence organic semiconductors, results in a small radiative rate that limits performance in OLEDs. Here, the authors show that it is possible to reconcile these conflicting requirements in materials that can access both high oscillator strength intramolecular excitations and intermolecular charge transfer states.

Potassium (K) is one of the main and most hazardous trace species released to the gas-phase during thermochemical conversion of biomass. Accurate experimental data and models of K release are needed to better understand the chemistry involved. Tunable diode laser absorption spectroscopy (TDLAS) is used for simultaneous real-time in situ measurements of gas-phase atomic K, water (H2O) and gas temperature in the vicinity (boundary layer) of biomass particles during combustion in a laboratory single-particle reactor. Atomic K is detected in a wide dynamic range, including optically thick conditions, using direct absorption spectroscopy at the wavelength of 770 nm, while H2O and temperature are determined by calibration-free scanned wavelength modulation spectroscopy at 1398 nm. The high accuracy and repeatability of the setup allows to distinguish measurements with varying initial particle mass, laser beam height above the particle and fuel type. Four types of biomass with different ash composition are investigated: softwood, Salix, Miscanthus and wheat straw. For Salix and wheat straw, the K release behaviour is, for the first time, compared to a detailed numerical particle model taking into account the interaction between K/S/Cl composition in the particle ash. A good agreement is achieved between the measured and calculated time-resolved atomic K concentrations for the devolatilization phase of the biomass particles.

The chemical shift of core level binding energies makes electron spectroscopy for chemical analysis (ESCA) a workhorse analytical tool for science and industry. For some elements, close lying and overlapping spectral features within the natural life time broadening restrict applications. We establish how the core level binding energy chemical shift can be picked up experimentally by the additional selectivity through Auger electron photoelectron coincidence spectroscopy (APECS). Coincident measurement of Ni 3p photoemission with different MVV Auger regions from specific decay channels, narrows the 3p core-levels to a width of 1.2 eV, resolves the spin–orbit splitting of 1.6 eV and determines the chemical shift of Ni 3p levels of a Ni(111) single crystal and its oxidized surface layer to 0.6 eV.

Lidar is an effective tool for high-altitude atmospheric measurement in which a weak absorption line for the target gas is selected to ensure a large optical depth. The laser frequency stabilization to the line center is required, and a sub-Doppler (sD) spectroscopy of the target line is preferred as a frequency reference. In this paper, a novel universal sD noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS) instrumentation based on a fiber-coupled optical single-sideband electro-optic modulator (f-SSM) for the potential application in atmospheric lidar for different target gases with different types of lasers is reported. The f-SSM can replace all frequency actuators in the system, so as to eliminate the individual design of feedback servos that often are tailored for each laser. The universality of the instrumentation was demonstrated by the alternative use of either an Er-doped fiber laser or a whispering-gallery-mode laser. Then the instruments based on both lasers were used to produce the sD signals of acetylene, which worked as a frequency reference to stabilize the laser. By performing the lockings, relative frequency stabilizations of 8.3×10-13 and 7.5×10-13 at an integration time of 240 s were demonstrated.

Electrically conducting polymers (ECPs) are becoming increasingly important in areas such as optoelectronics, biomedical devices, and energy systems. Still, their detailed charge transport properties produce an anomalous optical conductivity dispersion that is not yet fully understood in terms of physical model equations for the broad range optical response. Several modifications to the classical Drude model have been proposed to account for a strong non-Drude behavior from terahertz (THz) to infrared (IR) ranges, typically by implementing negative amplitude oscillator functions to the model dielectric function that effectively reduce the conductivity in those ranges. Here we present an alternative description that modifies the Drude model via addition of positive-amplitude Lorentz oscillator functions. We evaluate this so-called Drude-Lorentz (DL) model based on the first ultra-wide spectral range ellipsometry study of ECPs, spanning over four orders of magnitude: from 0.41 meV in the THz range to 5.90 eV in the ultraviolet range, using thin films of poly(3,4-ethylenedioxythiophene): tosylate (PEDOT: Tos) as a model system. The model could accurately fit the experimental data in the whole ultrawide spectral range and provide the complex anisotropic optical conductivity of the material. Examining the resonance frequencies and widths of the Lorentz oscillators reveals that both spectrally narrow vibrational resonances and broader resonances due to localization processes contribute significantly to the deviation from the Drude optical conductivity dispersion. As verified by independent electrical measurements, the DL model accurately determines the electrical properties of the thin film, including DC conductivity, charge density, and (anisotropic) mobility. The ellipsometric method combined with the DL model may thereby become an effective and reliable tool in determining both optical and electrical properties of ECPs, indicating its future potential as a contact-free alternative to traditional electrical characterization. Funding Agencies|Swedish Research Council; Swedish Foundation for Strategic Research; Wenner-Gren Foundations; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009 00971]

We report on the progress, challenges and future directions of blue perovskite light-emitting diodes to facilitate their further development., Metal halide perovskites have excellent optical and electrical properties and can be easily processed via low-cost solution-based techniques like blade-coating and inkjet printing, promising a bright future for various optoelectronic applications. Recently, encouraging progress has been made in perovskite light-emitting diodes (PeLEDs). Green, red, and near-infrared PeLEDs have achieved high external quantum efficiencies of more than 20%. However, as historically blue electroluminescence remains challenging in all previous LED technologies, we are witnessing a similar case with the development of blue PeLEDs, an essential part of displays and solid-state lighting, which lag far behind those of their counterparts. Herein, we review the recent progress of blue PeLEDs and discuss the main challenges including colour instability, poor photoluminescence efficiency and emission quenching by interlayers. Future directions are provided to facilitate the development of efficient blue PeLEDs.

We report on fabrication of spatially-coherent columnar plasmonic nanostructure superlattice-type thin films with high porosity and strong optical anisotropy using glancing angle deposition. Subsequent and repeated depositions of silicon and gold lead to nanometer-dimension subcolumns with controlled lengths. We perform generalized spectroscopic ellipsometry measurements and finite element method computations to elucidate the strongly anisotropic optical properties of the highly-porous Si-Au slanted columnar heterostructures. The occurrence of a strongly localized plasmonic mode with displacement pattern reminiscent of a dark quadrupole mode is observed in the vicinity of the gold subcolumns. We demonstrate tuning of this quadrupole-like mode frequency within the near-infrared spectral range by varying the geometry of Si-Au slanted columnar heterostructures. In addition, coupled-plasmon-like and inter-band transition-like modes occur in the visible and ultra-violet spectral regions, respectively. We elucidate an example for the potential use of Si-Au slanted columnar heterostructures as a highly porous plasmonic sensor with optical read out sensitivity to few parts-per-million solvent levels in water. Funding Agencies|National Science Foundation (NSF) through the Nebraska Materials Research Science and Engineering Center (MRSEC) [DMR-1420645, CMMI 1337856, EAR 1521428, DMR 1808715]; German Research Foundation [FE 1532/1-1]; Air Force Research Office [FA9550-18-1-0360]; American Chemical Society [ACS PRF 59374-ND5]; University of Nebraska-Lincoln; J.A. Woollam Co., Inc.; J.A. Woollam Foundation

Utilizing Sb-based bulk epilayers on large-scale low-cost substrates such as GaAs for fabricating infrared (IR) photodetectors is presently attracting significant attention worldwide. For this study, three sample series of GaAsxSb1−x, In1−xGaxSb, and InAsxSb1−x with different compositions were grown on semi-insulating GaAs substrates by using molecular beam epitaxy (MBE) and appropriate InAs quantum dots (QDs) as a defect-reduction buffer layer. Photoluminescence (PL) signals from these samples were observed over a wide IR wavelength range from 2 μm to 12 μm in agreement with the expected bandgap, including bowing effects. In particular, interband PL signals from InAsxSb1−x and In1−xGaxSb samples even at room temperature show promising potential for IR photodetector applications.

We report the design and numerical results of a miniaturized and efficient plasmonic cut-off filter that is based on stepped impedance resonators and operates at telecom wavelengths.

Optics express 29(3), 4210 (2021). doi:10.1364/OE.415564, Optical parametric chirped-pulse amplification (OPCPA) is a light amplification technique that provides the combination of broad spectral gain bandwidth and large energy, directly supporting few-cycle pulses with multi-terawatt (TW) peak powers. Saturation in an OPCPA increases the stability and conversion efficiency of the system. However, distinct spectral components experience different gain and do not saturate under the same conditions, which reduces performance. Here, we describe a simple and robust approach to control the saturation for all spectral components. The demonstrated optimal saturation increases the overall gain, conversion efficiency and spectral bandwidth. We experimentally obtain an improvement of the pulse energy by more than 18%. This technique is easily implemented in any existing OPCPA system with a pulse shaper to maximize its output., Published by Soc., Washington, DC

Physical chemistry, chemical physics 23(14), 8246 - 8260 (2021). doi:10.1039/D1CP00430A, We report on the effects of electron collision and indirect ionization processes, occurring at photoexcitation and electron kinetic energies well below 30 eV, on the photoemission spectra of liquid water. We show that the nascent photoelectron spectrum and, hence, the inferred electron binding energy can only be accurately determined if electron energies are large enough that cross sections for quasi-elastic scattering processes, such as vibrational excitation, are negligible. Otherwise, quasi-elastic scattering leads to strong, down-to-few-meV kinetic energy scattering losses from the direct photoelectron features, which manifest in severely distorted intrinsic photoelectron peak shapes. The associated cross-over point from predominant (known) electronically inelastic to quasi-elastic scattering seems to arise at surprisingly large electron kinetic energies, of approximately 10–14 eV. Concomitantly, we present evidence for the onset of indirect, autoionization phenomena (occurring via superexcited states) within a few eV of the primary and secondary ionization thresholds. These processes are inferred to compete with the direct ionization channels and primarily produce low-energy photoelectrons at photon and electron impact excitation energies below ∼15 eV. Our results highlight that vibrational inelastic electron scattering processes and neutral photoexcitation and autoionization channels become increasingly important when photon and electron kinetic energies are decreased towards the ionization threshold. Correspondingly, we show that for neat water and aqueous solutions, great care must be taken when quantitatively analyzing photoelectron spectra measured too close to the ionization threshold. Such care is essential for the accurate determination of solvent and solute ionization energies as well as photoelectron branching ratios and peak magnitudes., Published by RSC Publ., Cambridge

Perovskite light emitting diodes suffer from poor operational stability, exhibiting a rapid decay of external quantum efficiency within minutes to hours after turn-on. To address this issue, we explore surface treatment of perovskite films with phenylalkylammonium iodide molecules of varying alkyl chain lengths. Combining experimental characterization and theoretical modelling, we show that these molecules stabilize the perovskite through suppression of iodide ion migration. The stabilization effect is enhanced with increasing chain length due to the stronger binding of the molecules with the perovskite surface, as well as the increased steric hindrance to reconfiguration for accommodating ion migration. The passivation also reduces the surface defects, resulting in a high radiance and delayed roll-off of external quantum efficiency. Using the optimized passivation molecule, phenylpropylammonium iodide, we achieve devices with an efficiency of 17.5%, a radiance of 1282.8 W sr−1 m−2 and a record T50 half-lifetime of 130 h under 100 mA cm−2., Perovskite light emitting diodes suffer from operational stability, showing rapid decay of performance within minutes to hours after turn-on. Here, the authors investigate how the steric and Coulomb interaction of ammonium passivation molecules with varying alkyl chain length can improve device stability by suppressing iodide ion migration.

Despite great challenges, the development of new molecular structures with multiple and even conflicting characteristics are eagerly pursued for exploring advanced applications. To develop high-performance chiral organic semiconducting molecules, a distorted π-system is required for strong coupling with circularly polarized light (CPL), whereas planar π-stacking systems are necessary for high charge-carrier mobility. To address this dilemma, in this work, we introduce a skeleton merging approach through distortion of a perylene diimide (PDI) core with four fused heteroaromatics to form an ortho-π-extended PDI double-[7]heterohelicene. PDI double helicene inherits a high dissymmetry factor from the helicene skeleton, and the extended π-planar system concurrently maintains a high level of charge transport properties. In addition, ortho-π-extension of the PDI skeleton brings about near-infrared (NIR) light absorption and ambipolar charge transport abilities, endowing the corresponding organic phototransistors with high photoresponsivity of 450 and 120 mA W−1 in p- and n-type modes respectively, along with a high external quantum efficiency (89%) under NIR light irradiations. Remarkably, these multiple characteristics enable high-performance broadband CPL detections up to NIR spectral region with chiral organic semiconductors., In organic semiconducting molecules materials, distorted π-systems enable strong coupling with circular polarized light while planar π-stacking systems are necessary for high charge-carrier mobility. Here, the authors address this dilemma by introducing a skeleton merging approach through distortion of a perylene diimide core with four fused heteroaromatics to form a π-extended double helicene.

A miniaturized and efficient tunable wide flat-top band-pass filter at NIR is proposed in a MIM plasmonic waveguide. Furthermore, numerical results illustrate that tunability is readily attained by varying length of right-angle trapezoid resonator.

Metal halide perovskites have shown rapid development in various fields such as photovoltaics, photodetectors, light-emitting diodes (LEDs), and optically pumped lasers owing to their superior optoelectronic properties. Here, we review the basic optoelectronic properties of halide perovskites from a photophysical perspective. We highlight that halide perovskites are promising in various optoelectronic devices functioning at a wide range of carrier densities. We discuss optically and electrically generated carrier density under two different excitation modes [continuous wave (CW) and pulsed] as well as the impact of carrier density on the optoelectronic behavior of perovskites. Moreover, we discuss lasing actions at high carrier densities and summarize key rules to evaluate the lasing actions. Last, we provide an outlook on perovskite-based electrically pumped lasers. Funding Agencies|ERC Starting GrantEuropean Research Council (ERC) [717026]; Swedish Energy Agency EnergimyndighetenSwedish Energy Agency [48758-1, 44651-1]; Swedish Foundation for International Cooperation in Research and Higher Education [CH2018-7736]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009-00971]

This paper reports design and numerical results of an ultra-compact, efficient and tunable plasmonic band-stop filter based on a metal-insulator-metal waveguide at optical channels. Furthermore, a wide-bandgap can be easily achieved by adjusting the width of the of the stub resonator.

Due to the high rate of optical losses and the extensive usage of noble metals, alternative plasmonic materials with maximum tunability and low loss are desired for future plasmonic and metamaterial devices and applications. Herein, the potential of aluminum‐doped zinc oxide (AZO), one of the most prominent members of the transparent conducting oxide family, is demonstrated, for its applicability in plasmonic metamaterials. Using first‐principles density functional theory, combined with optical calculations, AZO‐based, plasmonic split‐ring resonators (SRRs) as model examples are showcased. The results match with experimental reports for the optical dielectric functions of pure and 2.08% Al‐doped zinc oxide (ZnO), if the Hubbard model to the local density approximation is applied. The broadband optical dispersion data for varying dopant concentrations (0%, 2.08%, and 6.25%) are extracted and provided. The subsequent optical response analyses show the existence of pronounced plasmons and inductor–capacitor modes in Al‐doped ZnO SRRs and an enhancement in metallic characteristics and plasmonic performance of AZO upon increasing Al concentration. The findings predict AZO as a low‐loss plasmonic material with promising capability for enhancing future optoelectronics applications. The method introduces a new, versatile approach to design future optical materials of arbitrary geometry.

A rational host–guest concept design for the attainment of high efficiency at strong luminance from light‐emitting electrochemical cells (LECs) by suppression of exciton‐polaron quenching [Tang et al., Nature Communications 2017, 8, 1190] has been reported. However, a practical drawback with the presented host–guest LEC devices was that the operational stability is insufficient for many applications. Here, a systematic study is performed, revealing that a major culprit for the limited operational stability is that the employed n‐type host, 1,3‐bis[2‐(4‐tert‐butylphenyl)‐1,3,4‐oxadiazo‐5‐yl]benzene (OXD‐7), has a strong propensity for crystallization and that this crystallization results in a detrimental phase separation of the constituents in the active material during device operation. The authors, therefore, identify an alternative class of concept‐functional n‐type hosts in the form of spirobifluorene‐phosphine‐oxide compounds, and report that the replacement of OXD‐7 with amorphous 2,7‐bis(diphenylphosphoryl)‐9,9′‐spirobifluorene results in a much improved operational lifetime of 700 h at >100 cd m−2 during constant‐bias driving at an essentially retained high current efficacy of 37.9 cd A−1 and a strong luminance of 2940 cd m−2.

Gas modulation refractometry (GAMOR) is a methodology for assessment of gas refractivity, molar density, and pressure that, by a rapid gas modulation, exhibits a reduced susceptibility to various types of disturbances. Although previously demonstrated experimentally, no detailed analysis of its ability to reduce the pickup of drifts has yet been given. This work provides an explication of to what extent modulated refractometry in general, and GAMOR in particular, can reduce drifts, predominantly those of the cavity lengths, gas leakages, and outgassing. It is indicated that the methodology is insensitive to the linear parts of so-called campaign-persistent drifts and that it has a significantly reduced susceptibility to others. This makes the methodology suitable for high-accuracy assessments and out-of-laboratory applications.

Strong light-matter coupling can form hybrid states at new energy levels that share properties of both light and matter. This principle offers new routes to control material functions without modifying the chemical structure of molecules. In this work, we coupled ambipolar semiconducting thin films to a Fabry-Perot cavity and investigated effects on charge transport. By constructing thin-film transistors inside optical cavities, we could simultaneously study coupling features and charge transport in the same samples. The cavity resonance was detuned by controlling the thickness of the top spacer layer in the cavity. We found no significant influence on charge transport for our systems, which may be related to insufficiently strong coupling. Possible additional origins and future directions are also discussed. Funding Agencies|Wenner-Gren Foundations; Swedish Research CouncilSwedish Research CouncilEuropean Commission [621-2014-5599]; Swedish Foundation for Strategic ResearchSwedish Foundation for Strategic Research; AForsk foundation; National Research Foundation of Korea (NRF)National Research Foundation of Korea; Korea government (MSIT)Korean Government [2020R1A2C1102558]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009 00971]

The structural changes of water upon deep supercooling were studied through wide-angle x-ray scattering at SwissFEL. The experimental setup had a momentum transfer range of 4.5 Å-1, which covered the principal doublet of the x-ray structure factor of water. The oxygen-oxygen structure factor was obtained for temperatures down to 228.5 ± 0.6 K. Similar to previous studies, the second diffraction peak increased strongly in amplitude as the structural change accelerated toward a local tetrahedral structure upon deep supercooling. We also observed an anomalous trend for the second peak position of the oxygen-oxygen structure factor (q2). We found that q2 exhibits an unprecedented positive partial derivative with respect to temperature for temperatures below 236 K. Based on Fourier inversion of our experimental data combined with reference data, we propose that the anomalous q2 shift originates from that a repeat spacing in the tetrahedral network, associated with all peaks in the oxygen-oxygen pair-correlation function, gives rise to a less dense local ordering that resembles that of low-density amorphous ice. The findings are consistent with that liquid water consists of a pentamer-based hydrogen-bonded network with low density upon deep supercooling. QC 20220125

Nanoparticulate double-heterojunction photocatalysts comprising TiO2(Anatase)/WO3/TiO2(Rutile) were produced by a sol–gel method. The resulting photocatalysts exhibit clear synergistic effects when tested toward the degradation of methyl orange under both UV and visible light. Kinetic studies indicate that the degradation rate on the best double-heterojunction photocatalyst (10 wt % WO3-TiO2) depends mainly on the amount of dye concentration, contrary to pure oxides in which the degradation rate is limited by diffusion-controlled processes. The synergistic effects were confirmed through systematic and careful studies including holes and OH radical formation, X-ray diffraction, electron microscopy, elemental analysis, UV–vis diffuse reflectance spectroscopy, and surface area analysis. Our results indicate that the successful formation of a double heterojunction in the TiO2(Anatase)/WO3/TiO2(Rutile) system leads to enhanced photoactivity when compared to individual oxides and commercial TiO2 P25.

Funder: ERC Starting Grant (No. 717026), Bright and efficient blue emission is key to further development of metal halide perovskite light-emitting diodes. Although modifying bromide/chloride composition is straightforward to achieve blue emission, practical implementation of this strategy has been challenging due to poor colour stability and severe photoluminescence quenching. Both detrimental effects become increasingly prominent in perovskites with the high chloride content needed to produce blue emission. Here, we solve these critical challenges in mixed halide perovskites and demonstrate spectrally stable blue perovskite light-emitting diodes over a wide range of emission wavelengths from 490 to 451 nanometres. The emission colour is directly tuned by modifying the halide composition. Particularly, our blue and deep-blue light-emitting diodes based on three-dimensional perovskites show high EQE values of 11.0% and 5.5% with emission peaks at 477 and 467 nm, respectively. These achievements are enabled by a vapour-assisted crystallization technique, which largely mitigates local compositional heterogeneity and ion migration.

This paper presents design and simulation results of a super-compact and efficient plasmonic cut-off filter based on an asymmetric E-shaped resonator. Moreover, by modulating length of the resonator, cut-off wavelength can be easily adjusted.

GaAs-based semiconductors are highly attractive for diverse nonlinear photonic applications, owing to their non-centrosymmetric crystal structure and huge nonlinear optical coefficients. Nanostructured semiconductors, for example, nanowires (NWs), offer rich possibilities to tailor nonlinear optical properties and further enhance photonic device performance. In this study, it is demonstrated highly efficient second-harmonic generation in subwavelength wurtzite (WZ) GaAs NWs, reaching 2.5 × 10−5 W−1, which is about seven times higher than their zincblende counterpart. This enhancement is shown to be predominantly caused by an axial built-in electric field induced by spontaneous polarization in the WZ lattice via electric field-induced second-order nonlinear susceptibility and can be controlled optically and potentially electrically. The findings, therefore, provide an effective strategy for enhancing and manipulating the nonlinear optical response in subwavelength NWs by utilizing lattice engineering. Funding: Swedish Research Council European Commission [2019-04312]; Swedish Foundation for International Cooperation in Research and Higher Education (STINT) [JA2014-5698]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University [2009 00971]; KAKENHI from Japan Society of Promotion of Science [19H00855, 16H05970]; National Natural Science Foundation of China (NSFC) [12027805, 11991060]

Gold nanoparticles (AuNPs) are highly compelling nanomaterials for biomedical studies due to their unique optical properties. By leveraging the versatile optical properties of different gold nanostructures, the performance of biosensing and biomedical imaging can be dramatically improved in terms of their sensitivity, specificity, speed, contrast, resolution and penetration depth. Here we review recent advances of optical biosensing and bioimaging techniques based on three major optical properties of AuNPs: surface plasmon resonance, surface enhanced Raman scattering and luminescence. We summarize the fabrication methods and optical properties of different types of AuNPs, highlight the emerging applications of these AuNPs for novel optical biosensors and biomedical imaging innovations, and discuss the future trends of AuNP-based optical biosensors and bioimaging as well as the challenges of implementing these techniques in preclinical and clinical investigations. Funding Agencies|European UnionEuropean Commission [H2020-MSCA-ITN-2018-813680]; CSIR, IndiaCouncil of Scientific & Industrial Research (CSIR) - India; Department of Science and Technology, New Delhi, IndiaDepartment of Science & Technology (India) [DST/INSPIRE/04/2015/000932]; Science & Engineering Research Board (Government of India) [SB/DF/011/2019]; Damon Runyon Cancer Research Foundation (DFS) [06-13]; Susan G. Komen Breast Cancer FoundationSusan G. Komen Breast Cancer Foundation [SAB15-00003]; Mary Kay Foundation [017-14]; Center for Cancer Nanotechnology Excellence and Translation (CCNE-T) [NIH-NCI U54CA151459]; Pew Charitable Trusts; Alexander and Margaret Stewart Trust; Claire Giannini Fund; Donald E. and Delia B. Baxter Foundation; Skippy Frank Foundation

To understand the observed wear in WC/Co tools during machining of Ti-alloys, it is important to know which interfaces are present in the tool-workpiece contact zone. It has been shown that WC grains in contact with the workpiece form a C depleted layer consisting of BCC W, and as such, knowledge of which WC/W interfaces can be expected and which interfaces can be used as starting points for further computations are of great importance. Here, this is studied by the systematic construction of interfaces and evaluation of the work of adhesion and interfacial energies of 60,000 unique interfaces spread across six different interface systems made up of the basal and prismatic surfaces of WC and the low index surfaces of BCC W. Calculations are made using a classical approach in LAMMPS as well as subset analysis using first principles in VASP (Vienna Ab Initio Simulation Package). The results show trends as functions of strain and system size giving a large-scale overview of this system and finding the energetically preferred interface combination to be the type-I, W-terminated prismatic WC surface against the [110] surface of BCC W.

In optically pumped lasers, heat generated by the quantum defect causes detrimental fluctuations in the output mode, frequency, and power. Common heat-mitigation techniques use bulky mechanical coolers that introduce vibrations, leading to laser frequency and amplitude noise. Here, we present a radiation-balanced fiber laser, optically cooled by anti-Stokes fluorescence (ASF). The gain medium is a silica fiber with a 21-µm-diameter core doped with 2.06 wt. % Y b 3 + and co-doped with A l 2 O 3 and F- to reduce concentration quenching. The laser was core-pumped at 1040 nm to create both gain at 1065 nm and ASF cooling at atmospheric pressure. We demonstrate a maximum output power of 114 mW with a slope efficiency of 41% while maintaining near-zero average temperature change. This result could enable the development of fiber lasers with unprecedented coherence and stability.

A highly efficient and compact wide flat-top band-pass filter at NIR is realized in a MIM plasmonic waveguide. Besides, simulation results reveal that through tuning the length of resonators, a broadband band-pass transmission can be easily achieved.

Hard X-ray spectroscopy is an element specific probe of electronic state, but signals are weak and require intense light to study low concentration samples. Free electron laser facilities offer the highest intensity X-rays of any available light source. The light produced at such facilities is stochastic, with spikey, broadband spectra that change drastically from shot to shot. Here, using aqueous ferrocyanide, we show that the resonant X-ray emission (RXES) spectrum can be inferred by correlating for each shot the fluorescence intensity from the sample with spectra of the fluctuating, self-amplified spontaneous emission (SASE) source. We obtain resolved narrow and chemically rich information in core-to-valence transitions of the pre-edge region at the Fe K-edge. Our approach avoids monochromatization, provides higher photon flux to the sample, and allows non-resonant signals like elastic scattering to be simultaneously recorded. The spectra obtained match well with spectra measured using a monochromator. We also show that inaccurate measurements of the stochastic light spectra reduce the measurement efficiency of our approach. X-ray absorption and X-ray free electron lasers are important tools to study chemical and structural dynamics, but spectral details like pre-edge features are inherently hard to detect. Here, the authors show that stochastic spectroscopy can yield similar spectral information to monochromatic spectroscopies, while increasing signal yield and reducing acquisition time.

Journal of synchrotron radiation 28(5), 1296 - 1308 (2021). doi:10.1107/S1600577521007657 special issue: "Issue on 11th International Workshop on X-ray Radiation Damage to Biological Crystalline Samples", X-rays are routinely used for structural studies through scattering, and femtosecond X-ray lasers can probe ultrafast dynamics. We aim to capture the femtosecond dynamics of liquid samples using simulations and deconstruct the interplay of ionization and atomic motion within the X-ray laser pulse. This deconstruction is resolution dependent, as ionization influences the low momentum transfers through changes in scattering form factors, while atomic motion has a greater effect at high momentum transfers through loss of coherence. Our methodology uses a combination of classical molecular dynamics and plasma simulation on a protic ionic liquid to quantify the contributions to the scattering signal and how these evolve with time during the X-ray laser pulse. Our method is relevant for studies of organic liquids, biomolecules in solution or any low-Z materials at liquid densities that quickly turn into a plasma while probed with X-rays.Keywords: radiation damage; molecular dynamics; non-local thermodynamic equilibrium; protic ionic liquids; X-ray free-electron lasers., Published by Wiley-Blackwell, [S.l.]

Photoemission electron microscopy and imaging X-ray photoelectron spectroscopy are today frequently used to obtain chemical and electronic states, chemical shifts, work function profiles within the fields of surface- and material sciences. Lately, because of recent technological advances, these tools have also been valuable within life sciences. In this study, we have investigated the power of photoemission electron microscopy and imaging X-ray photoelectron spectroscopy for visualization of human neutrophil granulocytes. These cells, commonly called neutrophils, are essential for our innate immune system. We hereby investigate the structure and morphology of neutrophils when adhered to gold and silicon surfaces. Energy-filtered imaging of single cells are acquired. The characteristic polymorphonuclear cellular nuclei divided into 2-S lobes is visualized. Element-specific imaging is achieved based on O 1s, P 2p, C 1s, Si 2p, and N is core level spectra, delivering elemental distribution with submicrometer resolution, illustrating the strength of this type of cellular morphological studies. Funding Agencies|Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [SFO-Mat-LiU 2009-00971]; Swedish Research Council VRSwedish Research Council [2019-02409]; Knut and Alice Wallenberg Foundation KAWKnut & Alice Wallenberg Foundation [2014.0276]; CTS [CTS 18:399 19:379]; Centre in Nanoscience and Nanotechnology at LiTH (CeNano) at Linkoping University

Ion pairing is commonly considered as a culprit for the reduced ionic conductivity in polymer electrolyte systems. However, this simple thermodynamic picture should not be taken literally, as ion pairing is a dynamical phenomenon. Here we construct model poly(ethylene oxide)-bis(trifluoromethane)sulfonimide lithium salt systems with different degrees of ion pairing by tuning the solvent polarity and examine the relation between the cation-anion distinct conductivity sigma(d)(+-) and the lifetime of ion pairs tau(+-) using molecular dynamics simulations. It is found that there exist two distinct regimes where sigma(d)(+-) scales with 1/tau(+-) and tau(+-), respectively, and the latter is a signature of longer-lived ion pairs that contribute negatively to the total ionic conductivity. This suggests that ion pairs are kinetically different depending on the solvent polarity, which renders the ion-pair lifetime highly important when discussing its effect on ion transport in polymer electrolyte systems.

Assessments of refractivity in a Fabry-Perot (FP) cavity by refractometry often encompass a step in which the penetration depth of the light into the mirrors is estimated to correct for the fraction of the cavity length into which no gas can penetrate. However, as it is currently carried out, this procedure is not always coherently performed. Here, we discuss a common pitfall that can be a reason for this and provide a recipe on how to perform FP-cavity-based refractometry without any influence of mirror penetration depth. Errata: C. Forssén, I. Silander, J. Zakrisson, M. Zelan, and O. Axner , "Retraction: “Fabry–Perot-cavity-based refractometry without influence of mirror penetration depth” [J. Vac. Sci. Technol. B 39, 065001 (2021)]", Journal of Vacuum Science & Technology B 40, 037001 (2022) https://doi.org/10.1116/6.0001829

Contemporary ultrafast science requires reliable sources of high-energy few-cycle light pulses. Currently two methods are capable of generating such pulses: post compression of short laser pulses and optical parametric chirped-pulse amplification (OPCPA). Here we give a comprehensive overview on the post-compression technology based on optical Kerr-effect or ionization, with particular emphasis on energy and power scaling. Relevant types of post compression techniques are discussed including free propagation in bulk materials, multiple-plate continuum generation, multi-pass cells, filaments, photonic-crystal fibers, hollow-core fibers and self-compression techniques. We provide a short theoretical overview of the physics as well as an in-depth description of existing experimental realizations of post compression, especially those that can provide few-cycle pulse duration with mJ-scale pulse energy. The achieved experimental performances of these methods are compared in terms of important figures of merit such as pulse energy, pulse duration, peak power and average power. We give some perspectives at the end to emphasize the expected future trends of this technology.

Solutions of the differential equations for the diffuse components of the four-flux model are obtained, including explicit expressions for the collimated-diffuse and diffuse-diffuse reflectance and transmittance for an optical three-layer system. We establish a method to invert collimated-diffuse reflectance and transmittance in order to obtain the spectral variation of all average pathlength parameters and forward scattering ratios, by applying a spectral simulated annealing method. The inversion procedure was tested with synthetic collimated-diffuse reflectance and transmittance spectra and showed very good convergence. Subsequently, the method was applied to measured spectra of a light scattering and absorbing medium containing TiO2 particles in a low-absorbing matrix, which was enclosed between two glass slides. Hence the present paper, together with our previous one, wherein we inverted collimated-collimated reflectance and transmittance spectra to obtain scattering and absorption coefficients, establishes a reliable inversion method for obtaining all parameters in the most general version of the four-flux theory from experimental data.

Bragg coherent diffraction imaging is a powerful strain imaging tool, often limited by beam-induced sample instability for small particles and high power densities. Here, we devise and validate an adapted diffraction volume assembly algorithm, capable of recovering three-dimensional datasets from particles undergoing uncontrolled and unknown rotations. We apply the method to gold nanoparticles which rotate under the influence of a focused coherent x-ray beam, retrieving their three-dimensional shapes and strain fields. The results show that the sample instability problem can be overcome, enabling the use of fourth generation synchrotron sources for Bragg coherent diffraction imaging to their full potential. Research conducted at MAX IV, a Swedish national user facility, is supported by the Swedish Research council under Contract No. 2018-07152, the Swedish Governmental Agency for Innovation Systems under Contract No. 2018-04969, and Formas under Contract No. 2019-02496. This work has also received funding from the ÅForsk Foundation (Contract No. 17-408), the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (Contract No. 801847), from the Olle Engkvist Foundation, from the Swedish Research council (Contract No. 2018-00234), and from NanoLund.

Communications Physics 3(1), 107 (2020). doi:10.1038/s42005-020-0348-9, Published by Springer Nature, London

Quenching of vibrational excitations in resonant inelastic X-ray scattering (RIXS) spectra of liquid acetic acid is observed. At the oxygen core resonance associated with localized excitations at the O–H bond, the spectra lack the typical progression of vibrational excitations observed in RIXS spectra of comparable systems. We interpret this phenomenon as due to strong rehybridization of the unoccupied molecular orbitals as a result of hydrogen bonding, which however cannot be observed in x-ray absorption but only by means of RIXS. This allows us to address the molecular structure of the liquid, and to determine a lower limit for the average molecular chain length.

Photofragmentation spectroscopy is combined with tunable diode laser absorption spectroscopy to measure the line shape of the fragment species. This provides flexibility in choosing the UV pulse location within the line shape and accurate quantification of both target species and background fragment concentrations, even under optically thick conditions. The technique is demonstrated by detection of potassium hydroxide (KOH) and atomic potassium K(g) above solid KOH converted in a premixed methane-air flat flame. Time series of KOH(g) and K(g) concentrations are recorded as a function of solid KOH mass and flame stoichiometry. The total substance released during the conversion is in good agreement with the initial solid KOH mass. Under fuel-rich conditions, increased K(g) concentrations at the expense of KOH(g) are observed compared to thermodynamic equilibrium.

We present the first experimental determination of the intra-atomic exchange energy between the inner 4f and the outer 6s5d shells in rare-earth elements. Inelastic electron tunneling spectroscopy on individual rare-earth atoms adsorbed on metal-supported graphene reveals an element-dependent excitation, with energy between 30 and 170 meV, linearly increasing with the spin angular momentum of the 4f shell. This observation is possible owing to the strong spin polarization of the outer shells, characteristic of rare-earth adatoms on graphene. This polarization gives rise to a giant magnetoresistance of up to 75% observed for Dy on graphene/Ir(111) single-atom magnets. Density functional theory calculations of the 6s5d shell spin polarizations and of their intra-atomic exchange constants with the 4f shell yield exchange energies in agreement with the experimental values. These results prove that the description of the spin dynamics in RE considering only the 4f - 5d interaction is oversimplified. A more realistic treatment requires us to consider a multishell intra-atomic exchange in which both 6s and 5d shells are taken into account, with the 4f - 6s contribution possibly prevailing over the 4f - 5d one. Our findings are important for the general understanding of magnetism in rare earths, whether they are in bulk compounds or as surface adsorbed atoms and clusters. The results presented here also push for a revision of the description of the spin dynamics in rare-earth-based systems.

We report the design and characteristics of a simple and compact mode-locked Er-doped fiber laser and its application to broadband cavity-enhanced spectroscopy. The graphene mode-locked polarization maintaining oscillator consumes less than 5 W of power. It is thermally stabilized, enclosed in a 3D printed box, and equipped with three actuators that control the repetition rate: fast and slow fiber stretchers, and metal-coated fiber section. This allows wide tuning of the repetition rate and its stabilization to an external reference source. The applicability of the laser to molecular spectroscopy is demonstrated by detecting CO2 in air using continuous-filtering Vernier spectroscopy with absorption sensitivity of 5.5 × 10−8 cm−1 in 50 ms.