Temperature dependence of ice optical constants: Implications for simulating the single-scattering properties of cold ice clouds

For a spectrum from ultraviolet to microwave and a temperature range from 160 to 270 K, the optical constants of water ice are compiled on the basis of the Kramers-Kronig relation in conjunction with existing datasets reported in literature. Significant temperature dependence is observed in both the mid-infrared and longer wavelengths. A sensitivity study at wavelengths in the infrared split window region indicates that the temperature dependence of the single-scattering properties of ice crystals is not negligible. Thus, it is necessary to take into account the temperature dependence of ice optical constants when simulating the radiative properties of cirrus clouds for various applications to remote sensing under cirrus cloud conditions.     

The infra-red and Raman spectra of ice

This paper has reviewed all of the available work on the infra-red and Raman spectroscopy of hexagonal and cubic ice. It has been shown by the studies of Maisch (1956) and Ockman (1957) that it is not possible to obtain a unique solution to the structure problem of ice by measuring its polarized vibration spectrum. However, Maisch's observation of the constancy of the depolarization ratio across each of the bands in the hydrogen stretching region is a strong argument for a disordered structure.

Satisfactory assignments have only been made for the three bands originating in the fundamental modes of the water molecule and for the six strong bands which can be correlated with the overtone and combination modes of the liquid and vapour spectra. An explicit characterization of the low frequency bands in terms of lattice motions must await a solution to the lattice-dynamical problem as well as a careful study of the low frequency, polarized spectra of single crystals.

The solution to the dynamical problem of the ice lattice should make possible a determination of the crystal anharmonicities. This would then enable one to assign the overtone and combination bands.     

有冰海区油膜光谱特征研究

近些年有冰海区石油的勘探、开发以及运输频度逐年上升,这增加了冰区溢油发生的风险。试验通过测量海水、碎冰、整冰等不同背景条件下轻柴油和原油油膜的可见光-近红外光谱反射率曲线,并与洁净的海水、碎冰和平整冰光谱曲线进行比较,得到能够有效识别冰区溢油的波段。测量结果表明：同一油种在不同背景下油膜的光谱反射率曲线有所差异,同一油种同一背景下由于分布形态不同光谱反射率曲线也有所差异。但同一油种的油膜仍呈现出许多区别于背景的共同特征：以海水、碎冰或整冰为背景的轻柴油油膜的光谱反射率曲线呈现“先低后高”、部分“相伴而行”的特点;海水、碎冰和整冰中原油油膜的光谱反射率曲线在750～770 nm区间出现楔状反射峰的典型特点。根据以上特点可以将溢油污染海水/海冰与洁净海水/海冰很好的区分开来,从而为遥感监测冰区溢油时的波段选择和溢油识别提供参考和依据。     

DFT‐assisted interpretation of the Raman spectra of hydrogen‐ordered ice XV

The vibrational spectra of the condensed phases of water often show broad and strongly overlapping spectral features which can make spectroscopic interpretations and peak assignments difficult. The Raman spectra of hydrogen‐ordered H₂O and D₂O ice XV are reported here, and it is shown that the spectra can be fully interpreted in terms of assigning normal modes to the various spectral features by using density functional theory (DFT) calculations. The calculated lattice‐vibration spectrum of the experimental antiferroelectric structure is in good agreement with the experimental data whereas the spectrum of a ferroelectric Cc structure, which computational studies have suggested as the crystal structure of ice XV, differs substantially. Moreover, the calculated coupled O–H stretch spectrum also seems in better agreement with the experiment than the calculated spectrum for the Cc structure. Both the hydrogen bonds as well as the covalent bonds appear to be stronger in hydrogen‐ordered ice XV than in the hydrogen‐disordered counterpart ice VI. A new type of stretching mode is identified, and it is speculated that this kind of mode might be relevant for other condensed water phases as well. Furthermore, the ice XV spectra are compared to the spectra of ice VIII which is the only other high‐pressure phase of ice for which detailed spectroscopic assignments have been made so far. In summary, we have established a link between crystallographic data and spectroscopic information in the case of ice XV by using DFT‐calculated spectra. Such correlations may eventually help interpreting the vibrational spectra of more structurally‐disordered aqueous systems. Copyright © 2012 John Wiley & Sons, Ltd.     

Millimeter/submillimeter nonlinear spectroscopy

The techniques of coherent transient spectroscopy have been successfully applied to the microwave and optical regions of the spectrum, but lack of suitable sources has prevented convenient extension to the millimeter/submillimeter region where several strong molecular transitions occur. Analysis of the experimental requirements and theory for such experiments considering several molecules including H₂O and CH₃Cl indicates how such experiments can be performed employing recently developed oscillators with increased power.     

Analysis on suitability of pure and α-Histidine doped KDP crystals in high speed applications

Ferroelectric Potassium Dihydrogen Phosphate (KDP) crystals are widely used in modern short wavelength laser techniques, non-linear and integrated optics. The pure and α-Histidine doped KDP crystals were procured from SRM Institute of Science and Technology, Chennai. The presence of additive in the doped KDP crystal is confirmed through X-Ray diffraction patterns and the lattice parameters were evaluated. Also, Fourier Transform Infrared spectrum confirms the presence of α-Histidine in the doped crystals. The dielectric behaviour of the pure and doped crystals have been studied in the microwave region using K-band microwave bench equipped with the Gunn oscillator and guided with rectangular wave guide.     

Origin of low-frequency local vibrational modes in high density amorphous ice

Incoherent-inelastic neutron scattering data are obtained from 5-80 K for high-density amorphous (hda) ice in the region 0-135 cm(-1). An excess contribution to the vibrational density of states is identified near 20 cm(-1). The origin of these vibrations has been identified by lattice dynamics calculations on an "experimental" structure derived from reverse Monte Carlo analysis of hda ice neutron diffraction data. An interpretation that localized oscillations of short chains and isolated water molecules are responsible for the excess low-frequency modes is consistent with our data.     

The effect of antifreeze proteins and poly(vinyl alcohol) on the nucleation of ice: a preliminary study

Three substances have been tested for ice nucleation inhibition. These were an antifreeze protein AFP III from the fish Macrozoarces americanus, an antifreeze glycoprotein AFGP from the fish Dissostichus mawsoni, and an 80% hydrolysed poly(vinyl alcohol) with a molecular weight of 9 to 10 kD. A nucleation spectrometer was used to test nucleation inhibition at a range of concentrations against two types of ice nuclei: those present in tap water and a bacterial nucleator from Pseudomonas syringae. The PVA reduced the nucleation temperature of tap water and the bacterial dispersions at all the concentrations which were tested. The AFGP reduced the nucleation temperature of tap water but enhanced the nucleation activity of the bacterial nucleators. At low concentrations the AFP III reduced the nucleation temperature of both tap water and the bacterial nucleator. At high concentrations the AFP III enhanced the nucleation temperature of the bacterial nucleator and broadened the nucleation spectrum of the tap water to encompass the nucleation spread of the control. The possible mechanisms of nucleation suppression and enhancement are discussed.     

Possibilities of the observation of the discrete spectrum of the water dimer at equilibrium in millimeter-wave band

Attempts of experimental observations of the water dimer spectrum at equilibrium conditions have lasted for more than 40 years since the dimeric hypothesis for extra absorption, but have not yielded any positive confirmed result. In the present paper a new approach is considered: using a high-resolution millimeter-wave spectrum of the water dimer at equilibrium, calculated by a rigorous fully quantum method, we show the potential existence of discernible spectral series of discrete features of the water dimer, which correspond to J+1←J, K lines of E₁ symmetry, already observed in cold molecular beam experiments and having, therefore, well-defined positions. The intensity of spectral series and contrast to the remaining continuum-like spectrum of the dimer are calculated and compared with the monomer absorption. The suitability of two types of microwave spectrometers for observing these series is considered. The collisional line-width of millimeter lines of the dimer at equilibrium is estimated and the width of IR dimer bands is discussed. It is pointed out that the large width of IR dimer bands may pose difficulties for their reliable observation and conclusive separation from the rest of absorption in water vapor. This situation contrasts with the suggested approach of dimer detection in millimeter-waves.     

Thermodynamic discontinuity between low-density amorphous ice and supercooled water

A combination of reverse Monte Carlo, molecular dynamics, and lattice dynamics simulations were used to obtain structural and thermodynamic data for low-density amorphous ice. A thermodynamically discontinuous transformation to a phase with properties and a structure consistent with supercooled liquid water is found to occur at approximately 130 K. Quantum corrections have a profound effect on thermodynamic properties and the location of important thermodynamic points in the water phase diagram.     

Relation between the two-dimensional self-avoiding walk and the Eden model

When the interface of a two-dimensional lattice gas is grown by an algorithm producing self-avoiding walks, some features of the Eden model appear. The scaling behavior of the widths and lengths of these interfaces and of their accessible perimeters are examined in several regions of the phase diagram. It is found that both the accessible perimeter and the interface behave like the Eden model below a critical point. Above this point, only the accessible perimeter behaves like the Eden model. The behavior in the critical region is suprisingly the same for the interface and its external perimeter but is different from the Eden model.     

基于星载辐射计AMSR-E不同波段的北极海冰折射系数提取

海冰折射系数是一个重要的地球物理参数。利用Hong Approximation(HA)算法和星载辐射计AMSR-E数据,基于不同微波频段(6.9,10.7,23,37,89 GHz)实现北极地区不同季节海冰折射系数反演。首先对反演所用关键数据海冰密集度反演算法的系点进行优化,反演结果与验证数据平均偏差分别为3.00%和-0.50%,低于其它常用算法。结果表明：冬季一年冰和夏季海冰的折射系数反演结果在所有微波频段的平均值范围为(1.78~1.75)和(1.72~1.70),与前人研究结果基本一致,但冬季多年冰在较高频率的折射系数与前人结果偏差较大,高于10.7 GHz的微波频段不能用于冬季多年冰折射系数的提取;综合利用不同波段海冰折射系数反演结果能够有效识别沿岸冰间湖(比如冬季6.9 GHz),区分多年冰与一年冰(冬季89 GHz),并能确定多夏季海冰边缘融化范围(夏季6.9 GHz)。     

IR spectroscopic study of surface properties of amorphous water ice

The state of the surface of amorphous ice with a specific surface area of about 160 m²/g obtained by the condensation of water vapor at 77 K is studied by IR spectroscopy. As the temperature increases to 130–160 K, absorption bands of surface hydroxyl groups vanish, whereas changes in bands characteristic of hydroxyl groups in the bulk of ice are indicative of a phase transition of ice from amorphous to the polycrystalline structure. The surface sites of amorphous ice are characterized with low-temperature adsorption of carbon monoxide. It is shown that there are two types of CO adsorption sites, free hydroxyl groups and oxygen atoms of surface coordinately unsaturated water molecules. Upon adsorption of nitrogen, methane, and carbon monoxide, in addition to the perturbation of surface OH groups, reversible changes in the spectrum are observed in the region of vibrations of bulk hydroxyls, which indicate that the strength of hydrogen bonds between water molecules in the surface layer of icy particles increases approaching the strength of these bonds in the crystal and that the ice surface becomes less amorphous. These results indicate that the properties of the ice surface layer substantially depend on the presence of adsorbed molecules.     

用传输矩阵法(TMM)研究二维光子晶体传输特性

将传输矩阵法(TMM)用于光子晶体传输特性的理论研究，采用Mur近似吸收边界和周期边界来截断计算区域，研究了以TM模正入射时，二维方格子光子晶体在完整周期结构下和有缺陷结构下的透过率谱；在微波波段制作了光子晶体模型，并设计了实验装置；实验与数值模拟计算取得了基本一致的结果。     

Fermi bubbles: giant, multibillion-year-old reservoirs of Galactic center cosmic rays

Recently evidence has emerged for enormous features in the γ-ray sky observed by the Fermi-LAT instrument: bilateral "bubbles" of emission centered on the core of the Galaxy and extending to around ± 10 kpc from the Galactic plane. These structures are coincident with a nonthermal microwave "haze" and an extended region of x-ray emission. The bubbles' γ-ray emission is characterized by a hard and relatively uniform spectrum, relatively uniform intensity, and an overall luminosity 4×10(37) erg/s, around 1 order of magnitude larger than their microwave luminosity while more than order of magnitude less than their x-ray luminosity. Here we show that the bubbles are naturally explained as due to a population of relic cosmic ray protons and heavier ions injected by processes associated with extremely long time scale (? 8 Gyr) and high areal density star formation in the Galactic center.     

CF4/Ar微波放电与CS2反应的可见化学发光研究

利用交叉分子束-化学发光研究方法,研究了气相条件下不同反应压力时CF4／Ar微波放电的产物与二硫化碳CS的交叉反应在可见区(300～900nm)的化学发光,利用密度泛函B3LYP和二阶微扰MP2理论分别在6-311 G(3df,2pd)和6-311 G(d,p)基组下计算了可能的反应产物电子基态的构型和振动频率,将得到的光谱标识为F2S2电子激发态的发射谱,通过对光谱和产物的分析,认为微波放电得到的亚稳态的Ar原子与CS发生碰撞反应使CS解离为S原子和CS,解离得到的S原子与微波放电产生的F原子发生多步反应得到了F2S2的激发态。     

Lawless Universe: Science and the Hunt for Reality

The four chief features to be expected in the infra-red absorption spectrum of a semiconductor are :—the intrinsic edge, lattice bands, impurity bands, and free carrier absorption. The first two of these, which have been explored with high resolution, are discussed in detail. Measurements of the absorption spectrum near the intrinsic edge in germanium and silicon show that indirect transitions take place, and that ‘excitons’ are formed; and the intrinsic energy gap can be deduced accurately. The lattice bands yield the main features of the lattice vibration spectrum.     

Nonlinear spectrum reshaping and gap-soliton-train trapping in optically induced photonic structures

We report the first theoretical prediction and experimental demonstration of gap soliton trains in a self-defocusing photonic lattice. Without a priori spectral or phase engineering, a stripe beam whose spatial power spectrum lies only in one transverse direction evolves into a gap soliton train with power spectrum growing also in the orthogonal direction due to nonlinear transport and spectrum reshaping. Our results suggest that, in nonlinear k-space evolution, energy can transfer not only between regions of normal and anomalous diffraction, but also from initially excited regions to initially unexcited regions.     

The conductivity properties of protons in ice and mechanism of magnetization of liquid water

From a study of electrical conductivity of protons in the hydrogen-bonded chains in ice we confirm that the magnetization of liquid water is caused by proton transfer in closed hydrogen-bonded chains occurring as a first order phase transition, through which the ice becomes liquid water. We first study the conductive properties of proton transfer along molecular chains in ice crystals in our model. Ice is a typical hydrogen-bonded molecular system, in which the interaction of localized fluctuation of hydrogen ions (H⁺) with deformation of a structure of hydroxyl group (OH) results in soliton motion of the protons along the molecular chains via ionic and bonded defects. We explain further the quantum conductive properties of proton transfer and determine its mobility and conductivity under constant electric-field using a new theory of proton transfer, which agree with experimental values. From features of first order phase-transition for ice, and some experimental data of pure and magnetized water we confirm further that there are not only free water molecules, but also many linear and closed hydrogen-bonded chains consisting of many polarized water-molecules in the liquid water. Thus a ring proton-current, which resembles to a “molecular current” or a “small magnet” in solids, can occur in the closed hydrogen-bond chains under action of an externally applied magnetic field. Then the water molecules in the closed chains can be orderly arrayed due to the magnetic interaction among these ring proton currents and the externally applied magnetic field. This is just the magnetized effect of the water. In such a case the optical and electronic properties of the water, including the dielectric constant, magnetoconductivity, refraction index, Raman and Infrared absorption spectra, are changed. We determine experimentally the properties of the magnetized water which agree with the theoretical results of our model. However, the magnetized effect of water is, in general, very small, and vanishes at temperatures above 100 ^○C.     

Hydrogen bonds and van der waals forces in ice at ambient and high pressures

The first principles methods, density-functional theory and quantum Monte Carlo, have been used to examine the balance between van der Waals (vdW) forces and hydrogen bonding in ambient and high-pressure phases of ice. At higher pressure, the contribution to the lattice energy from vdW increases and that from hydrogen bonding decreases, leading vdW to have a substantial effect on the transition pressures between the crystalline ice phases. An important consequence, likely to be of relevance to molecular crystals in general, is that transition pressures obtained from density-functional theory exchange-correlation functionals which neglect vdW forces are greatly overestimated.