Wavelength-dependent Absorption Research Articles

Wavelength-Dependent Nonlinear Optical Absorption and Broadband Optical Limiting in Au-Fe2O3-rGO Nanocomposites

Broadband optical limiting and wavelength-dependent nonlinear absorption studies of Au-Fe2O3-(15, 25, 40 wt %)rGO (reduced graphene oxide) nanocomposites were investigated using the Z-scan technique and excited with femtosecond (700–900 nm, 80 MHz, 150 fs) laser pulses. A reduction in the graphene perfect (La) domain and ID/IG ratio observed in the Raman data and the appearance of a Au 4f and Fe 2p singlet along with a shift in the C 1s state toward higher energy in the XPS data, peak broadening in the XRD data, and different mass residues left out with respect to content of rGO in the TG-DTA data strongly indicated the incorporation of Au-Fe2O3 nanostructures on solar exfoliated reduced graphene oxide. Selected aread electron diffraction data ascertained the presence of Au and Fe2O3 as a composite, and transmission electron microscopy (TEM) data revealed that the nano-octahedra Au-Fe2O3 turned themselves into nanospindles during incorporation of rGO. Ground state absorption spectra illustrated a pure and...

Black and brown carbon over central Amazonia: long-term aerosol measurements at the ATTO site

Abstract. The Amazon rainforest is a sensitive ecosystem experiencing the combined pressures of progressing deforestation and climate change. Its atmospheric conditions oscillate between biogenic and biomass burning (BB) dominated states. The Amazon further represents one of the few remaining continental places where the atmosphere approaches pristine conditions during occasional wet season episodes. The Amazon Tall Tower Observatory (ATTO) has been established in central Amazonia to investigate the complex interactions between the rainforest ecosystem and the atmosphere. Physical and chemical aerosol properties have been analyzed continuously since 2012. This paper provides an in-depth analysis of the aerosol's optical properties at ATTO based on data from 2012 to 2017. The following key results have been obtained. The aerosol scattering and absorption coefficients at 637 nm, σsp,637 and σap,637, show a pronounced seasonality with lowest values in the clean wet season (mean ± SD: σsp,637=7.5±9.3 M m−1; σap,637=0.68±0.91 M m−1) and highest values in the BB-polluted dry season (σsp,637=33±25 M m−1; σap,637=4.0±2.2 M m−1). The single scattering albedo at 637 nm, ω0, is lowest during the dry season (ω0=0.87±0.03) and highest during the wet season (ω0=0.93±0.04). The retrieved BC mass absorption cross sections, αabs, are substantially higher than values widely used in the literature (i.e., 6.6 m2 g−1 at 637 nm wavelength), likely related to thick organic or inorganic coatings on the BC cores. Wet season values of αabs=11.4±1.2 m2 g−1 (637 nm) and dry season values of αabs=12.3±1.3 m2 g−1 (637 nm) were obtained. The BB aerosol during the dry season is a mixture of rather fresh smoke from local fires, somewhat aged smoke from regional fires, and strongly aged smoke from African fires. The African influence appears to be substantial, with its maximum from August to October. The interplay of African vs. South American BB emissions determines the aerosol optical properties (e.g., the fractions of black vs. brown carbon, BC vs. BrC). By analyzing the diel cycles, it was found that particles from elevated aerosol-rich layers are mixed down to the canopy level in the early morning and particle number concentrations decrease towards the end of the day. Brown carbon absorption at 370 nm, σap,BrC,370, was found to decrease earlier in the day, likely due to photo-oxidative processes. BC-to-CO enhancement ratios, ERBC, reflect the variability of burnt fuels, combustion phases, and atmospheric removal processes. A wide range of ERBC between 4 and 15 ng m−3 ppb−1 was observed with higher values during the dry season, corresponding to the lowest ω0 levels (0.86–0.93). The influence of the 2009/2010 and 2015/2016 El Niño periods and the associated increased fire activity on aerosol optical properties was analyzed by means of 9-year σsp and σap time series (combination of ATTO and ZF2 data). Significant El Niño-related enhancements were observed: in the dry season, σsp,637 increased from 24±18 to 48±33 M m−1 and σap, 637 from 3.8±2.8 to 5.3±2.5 M m−1. The absorption Ångström exponent, åabs, representing the aerosol absorption wavelength dependence, was mostly <1.0 with episodic increases upon smoke advection. A parameterization of åabs as a function of the BC-to-OA mass ratio for Amazonian aerosol ambient measurements is presented. The brown carbon (BrC) contribution to σap at 370 nm was obtained by calculating the theoretical BC åabs, resulting in BrC contributions of 17 %–29 % (25th and 75th percentiles) to σap 370 for the entire measurement period. The BrC contribution increased to 27 %–47 % during fire events under El Niño-related drought conditions from September to November 2015. The results presented here may serve as a basis to understand Amazonian atmospheric aerosols in terms of their interactions with solar radiation and the physical and chemical-aging processes that they undergo during transport. Additionally, the analyzed aerosol properties during the last two El Niño periods in 2009/2010 and 2015/2016 offer insights that could help to assess the climate change-related potential for forest-dieback feedbacks under warmer and drier conditions.

Absorption by water increases fluorescence image contrast of biological tissue in the shortwave infrared

Recent technology developments have expanded the wavelength window for biological fluorescence imaging into the shortwave infrared. We show here a mechanistic understanding of how drastic changes in fluorescence imaging contrast can arise from slight changes of imaging wavelength in the shortwave infrared. We demonstrate, in 3D tissue phantoms and in vivo in mice, that light absorption by water within biological tissue increases image contrast due to attenuation of background and highly scattered light. Wavelengths of strong tissue absorption have conventionally been avoided in fluorescence imaging to maximize photon penetration depth and photon collection, yet we demonstrate that imaging at the peak absorbance of water (near 1,450 nm) results in the highest image contrast in the shortwave infrared. Furthermore, we show, through microscopy of highly labeled ex vivo biological tissue, that the contrast improvement from water absorption enables resolution of deeper structures, resulting in a higher imaging penetration depth. We then illustrate these findings in a theoretical model. Our results suggest that the wavelength-dependent absorptivity of water is the dominant optical property contributing to image contrast, and is therefore crucial for determining the optimal imaging window in the infrared.

Performance analysis of receiver of parabolic trough solar collector: Effect of selective coating, vacuum and semitransparent glass cover

Present work encompasses developing a new methodology to incorporate the heat transfer characteristics of the evacuated space (vacuum) in the annulus region between the absorber tube and glass cover and the effect of selective coatings on the steel absorber tube for a 3-dimensional computational fluid dynamics model of a parabolic trough solar collector (PTSC) receiver. In the present work, glass cover has been modeled semitransparent to the incoming solar flux, which has been applied on the glass cover. Wavelength-dependent absorption properties of glass cover material also has been modeled. In the current work, the direct normal irradiation and the mass flow rate of heat transfer fluid (HTF) has been varied to check their individual effect on the performance of PTSC absorber tube. Circumferential temperature distribution of absorber tube and glass cover has been found out; heat transfer to HTF and pressure drop of HTF in the absorber tube have also been calculated. A comparative study has been undertaken to highlight the relative contribution of the vacuum and selective coating on the receiver performance. The value of circumferential temperature difference at mid-length of absorber tube was found to be 14.78 K for 750 W/m2, which increases to 19.70 K for direct normal irradiation of 1000 W/m2. When vacuum is replaced by air in the annulus region, PTSC absorber performance decreases by 4.82%. Similarly, because of use of selective coating, the thermal efficiency of the receiver increased by 34.59%.

Study of the absorption coefficient of graphene-polymer composites

In this work, we have prepared a series of polydimethylsiloxane (PDMS) composites containing various graphene flakes loadings (0.02–2 wt%), and their broadband optical properties are being investigated. We demonstrate the tunability and evolution of transmittance and reflection spectra of the composites in a wide spectral range (0.4–200 μm) as a function of graphene content. Using these data we derive the broadband wavelength-dependent absorption coefficient (α) values. Our results show that α is roughly constant in the visible and IR ranges, and, surprisingly, is approximately one order of magnitude lower in the terahertz regime, suggesting different terahertz radiation scattering mechanism in our composite. Our material could be useful for applications in optical communication, sensing or ultrafast photonics.

Assessment of skin lesions produced by focused, tunable, mid-infrared chalcogenide laser radiation.

Traditionally, fractional laser treatments are performed with focused laser sources operating at a fixed wavelength. Using a tunable laser in the mid-infrared wavelength range, wavelength-dependent absorption properties on the ablation process and thermal damage formation were assessed with the goal to obtain customizable tissue ablations to provide guidance in finding optimized laser exposure parameters for clinical applications. Laser tissue experiments were carried out on full thickness ex vivo human abdominal skin using a mid-infrared tunable chromium-doped zinc selenide/sulfide chalcogenide laser. The laser has two independent channels: a continuous wave (CW) output channel which covers a spectrum ranging from 2.4 μm to 3.0 μm with up to 9.2 W output power, and a pulsed output channel which ranges from 2.35 μm to 2.95 μm. The maximum pulse energy of the pulsed channel goes up to 2.8 mJ at 100 Hz to 1,000 Hz repetition rate with wavelength-dependent pulse durations of 4-7 ns. Total ablation depth, ablation efficiency, and coagulation zone thickness were highly correlated to wavelength, pulse width, and pulse energy. Using the same total radiant exposure at 2.85 μm wavelength resulted in 10-times smaller coagulation zones and 5-times deeper ablation craters for one hundred 6 ns pulses compared to one 100 ms pulse. For a fixed pulse duration of 6 ns and a total radiant exposure of 2.25 kJ/cm2 the ablation depth increased with longer wavelengths. The tunable laser system provides a useful research tool to investigate specific laser parameters such as wavelength on lesion shape, ablation depth and thermal tissue damage. It also allows for customization of the characteristics of laser lesions and therefore facilitates the selection of suitable laser parameters for optimized fractional laser treatments. Lasers Surg. Med. 50:961-972, 2018.© 2018 Wiley Periodicals, Inc.

Source Apportionment of Brown Carbon Absorption by Coupling Ultraviolet–Visible Spectroscopy with Aerosol Mass Spectrometry

The impact of brown carbon (BrC) on climate has been widely acknowledged but remains uncertain, because either its contribution to absorption is being ignored in most climate models or the associated mixed emission sources and atmospheric lifetime are not accounted for. In this work, we propose positive matrix factorization as a framework to apportion the contributions of individual primary and secondary organic aerosol (OA) source components of BrC absorption, by combining long-term aerosol mass spectrometry (AMS) data with concurrent ultraviolet–visible (UV-vis) spectroscopy measurements. The former feature time-dependent factor contributions to OA mass, and the latter consist of wavelength-dependent absorption coefficients. Using this approach for a full-year case study, we estimate for the first time the mass absorption efficiency (MAE) of major light-absorbing water-soluble OA components in the atmosphere. We show that secondary biogenic OA contributes negligibly to absorption despite dominating the ...

Investigation of the absorption Ångström exponent and its relation to physicochemical properties for mini-CAST soot

In this work, a mini-CAST soot generator was used to produce soot with different optical and physicochemical characteristics. Absorption Ångström exponents (AAE) expressing the absorption wavelength dependence were assessed by multiwavelength in-situ and filter-based (aethalometer) laser extinction. The two optical techniques showed good agreement. For the chosen mini-CAST operating conditions, AAEs between 1 and 3.5 were found. Soot with high mass-fractions of organic carbon (OC) and pyrolytic carbon (PC) determined with thermal optical analysis were associated with AAEs significantly higher than 1. Heating to 250 and 500°C removed the majority of polycyclic aromatic hydrocarbons. However, the thermal-optical analysis revealed that OC and PC were abundant in the soot with AAE > 2 also after heating the aerosol. Analysis of mass absorption cross section ratios for elemental carbon and OC indicated that elevated AAEs also after heating to 500°C could be related to persistent OC and PC components and/or the refractory soot. By comparing the mini-CAST soot optical properties with soot properties derived from in-situ extinction measurements in a premixed flame, mini-CAST soot with a higher AAE could be identified as less mature soot.Copyright © 2018 The Authors

Computational Study of Plasmon Interaction in Organic Media: a Comparison Between Analytical and Numerical Model for Dimer

In the present work, an investigation of wavelength-dependent absorption spectrum of spherical nanoparticles with different arrangements in organic medium using discrete dipole approximation (DDA) has been performed. Specifically, we study the impact of different arrangements such as monomer, dimer (compositionally symmetric and asymmetric), 1D array of spherical nanoparticle on surface plasmon resonance (SPR) peak position, and its spectral broadening in distinct regimes of the electromagnetic spectrum. Three different organic materials such as P3HT:PCBM blend (Poly(3-hexyl thiophene))-(phenyl-C61-buryricacid methyl ester), P3HT(poly (3-hexyl thiophene)), and PEOPT ((4’-(1”, 4”, 7”-trioaoctyl) phenyl) theophany) have been chosen in the present work to study the absorption and scattering spectrum of MNP. Further, near-field pattern of homo-dimer nanogeometry is also shown in the present study. We also observed that on increasing the interacting number of particles in 1D array, the corresponding FWHM (full width at half maxima) value increases as well, which covers the large spectral region of the electromagnetic spectrum. The comparison between dipole model and numerical model has been performed to analyze the extinction behavior of smaller size (d << λ) metal nano dimer which shows a good agreement in 400–600nm wavelength range.

High-resolution retinal swept source optical coherence tomography with an ultra-wideband Fourier-domain mode-locked laser at MHz A-scan rates.

We present a new 1060 nm Fourier domain mode locked laser (FDML laser) with a record 143 nm sweep bandwidth at 2∙ 417 kHz = 834 kHz and 120 nm at 1.67 MHz, respectively. We show that not only the bandwidth alone, but also the shape of the spectrum is critical for the resulting axial resolution, because of the specific wavelength-dependent absorption of the vitreous. The theoretical limit of our setup lies at 5.9 µm axial resolution. In vivo MHz-OCT imaging of human retina is performed and the image quality is compared to the previous results acquired with 70 nm sweep range, as well as to existing spectral domain OCT data with 2.1 µm axial resolution from literature. We identify benefits of the higher resolution, for example the improved visualization of small blood vessels in the retina besides several others.

Multiphoton Absorption Order of CsPbBr3 As Determined by Wavelength-Dependent Nonlinear Optical Spectroscopy

CsPbBr3 is a direct-gap semiconductor where optical absorption takes place across the fundamental bandgap, but this all-inorganic halide perovskite typically exhibits above-bandgap emission when excited over an energy level, lying above the conduction-band minimum. We probe this bandgap anomaly using wavelength-dependent multiphoton absorption spectroscopy and find that the fundamental gap is strictly two-photon forbidden, rendering it three-photon absorption (3PA) active. Instead, two-photon absorption (2PA) commences when the two-photon energy is resonant with the optical gap, associated with the level causing the anomaly. We determine absolute nonlinear optical dispersion over this 3PA-2PA region, which can be explained by two-band models in terms of the optical gap. The polarization dependence of 3PA and 2PA is also measured and explained by the relevant selection rules. CsPbBr3 is highly luminescent under multiphoton absorption at room temperature with marked polarization and wavelength dependence at the 3PA-2PA crossover and therefore has potential for nonlinear optical applications.

Optical measurement of volume fraction and organic mass fraction of ultra-fine soot particles emitted from inverse diffusion flames

Soot particles of various organic carbon (OC) contents were generated with a triple co-flow burner. TEM images showed that the primary particle boundaries were more ambiguous when OC contents were high. A set of diode lasers of various wavelengths and a white light source were used to measure light extinction over a wide range of wavelengths (450–850nm), and the logarithm of the light intensity ratio was plotted asa function of the inverse of the various wavelengths. The slopes of the plot were taken from the both ends of the wavelength range, and their ratio was calculated. The results show that when the OC contents are high, the ratio increases to approximately 10, whereas the ratio remains nearly constant at a value of 1 when the OC contents are minimal. The analysis of the slope ratios shows that the wavelength-dependent absorption behavior of soot does not depend on the soot volume fraction or the soot particle size; rather, the slope ratio depends only on the soot’s refractive index, which in turn is related to its OC contents. In addition, the soot volume fraction and OC contents can be simultaneously identified without any chemical analysis based on the pre-determined relationship between the slope ratio and the organic fraction of soot.

Correlating Light Absorption with Various Nanostructure Geometries in Vertically Aligned Si Nanowire Arrays

Exploring the interactions between light and nanostructures contributes greatly to understanding and engineering nanoscale optical phenomena related to device performance. However, this often involves a compromise between uniformity and scalability. Given that optical properties, and especially light absorption, are governed by the geometries of nanostructures, this study investigated the correlation between light absorption and vertically aligned silicon nanowire (v-SiNW) arrays synthesized using KrF stepper lithography. Controlled growth experiments of the v-SiNW arrays indicated that their geometrical parameters strongly influence their corresponding light absorption properties, as confirmed by reflection measurements and finite difference time domain (FDTD) simulations, which showed specific wavelength-dependent absorption. Moreover, the extent of tapering the v-SiNW arrays was modulating to achieve broad absorption of visible light resulting from the gradual change in diameter and to optimize their o...

Nonlinear optical properties of Au–Ag core–shell nanorods for all-optical switching

Au–Ag core–shell nanorods with surface plasmon resonance wavelengths of 760–840 nm were prepared. Wavelength-dependent nonlinear absorption coefficients (β) and nonlinear refractive indices (γ) of the nanorods were measured by using Z-scan techniques. The corresponding one-photon and two-photon figures of merit (W and T) were calculated from β and γ. The results show that the requirements of W > 1 and T < 1 for the application of all-optical switching could be achieved for all the samples over a broad wavelength range. These observations make the Au–Ag core–shell nanorods a good candidate for all-optical switching devices.

Ultrafast carrier dynamics in type-II ZnO-SnO heterostructure thin films

We investigate the carrier relaxation and charge transfer dynamics in type-II ZnO-SnO heterojunction thin films using wavelength-dependent femtosecond transient absorption measurements. Under SnO-selective excitation conditions, absorption signals related to ZnO are observed on a subpicosecond time scale, which indicates ultrafast electron transfer from SnO to ZnO. The spatial separation of electrons and holes across the ZnO-SnO interface leads to a long-lived carrier decay process with a lifetime of ∼4 ns, 2 times longer than resonant excitation of both ZnO and SnO in the heterostructures. Our results provide a framework for understanding the photophysics of tin oxide semiconductor heterostructures.

Low Threshold Multiexciton Optical Gain in Colloidal CdSe/CdTe Core/Crown Type-II Nanoplatelet Heterostructures.

Colloidal cadmium chalcogenide core/crown type-II nanoplatelet heterostructures, such as CdSe/CdTe, are promising materials for lasing and light-emitting applications. Their rational design and improvement requires the understanding of the nature of single- and multiexciton states. Using pump fluence and wavelength-dependent ultrafast transient absorption spectroscopy, we have identified three spatially and energetically distinct excitons (in the order of increasing energy): interface-localized charge transfer exciton (XCT, with electron in the CdSe core bound to the hole in the CdTe crown), and CdTe crown-localized XCdTe and CdSe core-localized XCdSe excitons. These exciton levels can be filled sequentially, with each accommodating two excitons (due to electron spin degeneracy) to generate one to six exciton states (with lifetimes of ≫1000, 209, 43.5, 11.8, 5.8, and 4.5 ps, respectively). The spatial separation of these excitons prolongs the lifetime of multiexciton states. Optical gain was observed in tri- (XXCTXCdTe) and four (XXCTXXCdTe) exciton states. Because of the large absorption cross section of nanoplatelets, an optical gain threshold as low as ∼43 μJ/cm2 can be achieved at 550 nm excitation for a colloidal solution sample. This low gain threshold and the long triexciton (gain) lifetime suggest potential applications of these 2D type-II heterostructures as low threshold lasing materials.

The influence of wavelength-dependent absorption and temperature gradients on temperature determination in laser-heated diamond-anvil cells

In situ temperature measurements in laser-heated diamond-anvil cells (LHDACs) are among the most fundamental experiments undertaken in high-pressure science. Despite its importance, few efforts have been made to examine the alteration of thermal radiation spectra of hot samples by wavelength-dependent absorption of the sample itself and temperature gradients within the sample and their influence on temperature measurements while laser heating. In this study, we take (Mg, Fe)O ferropericlase as an example to evaluate the effects of these two factors. Iron-rich ferropericlase shows strong wavelength-dependent absorption in the wavelength range used to determine temperature, which, together with temperature gradients can account for largely aliased apparent temperatures in some experiments obtained by Wien fitting of detected thermal radiation intensities (e.g., an offset of ∼700 K for a 3300 K melting temperature). In general, wavelength-dependent absorption and temperature gradients of samples are two key factors to consider in order to rigorously constrain temperatures, which have been largely ignored in previous LHDAC studies.

Generation and UV-VIS-NIR spectral responses of organo-mineral aerosol for modelling soil derived dust

Various optical properties of laboratory constructed clay minerals coated by humic acid were determined in this study. For the preparation of organo-clay complexes, an adsorption method was conducted in Ca2+ dominated aquaeous solutions, which provides the opportunity to generate solely internally mixed aerosol particles with complete surface covering. The wavelength dependent optical absorption and scattering coefficients of the syntetised organo-clay complexes and the single clay components were measured in-situ in aerosol phase, using multi-wavelength photoacoustic and scattering instruments. Other climate relevant optical properties such as mass absorption and scattering coefficients, absorption enhancement factor, the imaginary part of complex refractive index, single scattering albedo and coating thickness were also deduced from the measured data. The estimated thickness of humic acid coating was about 10–20 nm. Even such relatively thin shell substantially enhanced the measured absorption of the clay particles with an enhancement factor of about 3–7 in the visible-near ultraviolet range, while caused smaller changes in the mass scattering values. As a cumulative effect, the coating decreased the single scattering albedo of the clay particles; from 0.99 ± 0.04 to 0.93 ± 0.04 in case of illite and from 0.99 ± 0.04 to 0.90 ± 0.03 in case of kaolin at 525 nm. The HA coating slightly modified the shape, the particles became less excentric. We presented a new method capable of generating solely internally mixed particles. Applying this method we experimentally demonstrated the strong effect of a light absorbing coating on the optical properties of dust particle.

RADIATIVE TRANSFER MODEL OF DUST ATTENUATION CURVES IN CLUMPY, GALACTIC ENVIRONMENTS

ABSTRACT The attenuation of starlight by dust in galactic environments is investigated through models of radiative transfer in a spherical, clumpy interstellar medium (ISM). We show that the attenuation curves are primarily determined by the wavelength dependence of absorption rather than by the underlying extinction (absorption+scattering) curve; the observationally derived attenuation curves cannot constrain a unique extinction curve unless the absorption or scattering efficiency is specified. Attenuation curves consistent with the “Calzetti curve” are found by assuming the silicate-carbonaceous dust model for the Milky Way (MW), but with the 2175 Å bump suppressed or absent. The discrepancy between our results and previous work that claimed the Small Magellanic Cloud dust to be the origin of the Calzetti curve is ascribed to the difference in adopted albedos; we use the theoretically calculated albedos, whereas the previous works adopted albedos derived empirically from observations of reflection nebulae. It is found that the attenuation curves calculated with the MW dust model are well represented by a modified Calzetti curve with a varying slope and UV bump strength. The strong correlation between the slope and UV bump strength, as found in star-forming galaxies at , is well reproduced when the abundance of the UV bump carriers is assumed to be 30%–40% of that of the MW dust; radiative transfer effects lead to shallower attenuation curves with weaker UV bumps as the ISM is more clumpy and dustier. We also argue that some local starburst galaxies have a UV bump in their attenuation curves, albeit very weak.

Stochastic interference of fluorescence radiation in random media with large inhomogeneities

Stochastic interference of fluorescence light outgoing from a dye-doped coarse-grained random medium, which was pumped by the continuous-wave laser radiation, was experimentally studied. It was found that the contrast of random interference patterns highly correlates with the wavelength-dependent fluorescence intensity and reaches its minimum in the vicinity of the cusp of emission spectrum. The decay in the contrast of spectrally selected speckle patterns was interpreted in terms of the pathlength distribution broadening for fluorescence radiation propagating in the medium. This broadening is presumably caused by the wavelength-dependent negative absorption of the medium.