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This dissertation reports an internal signal amplification mechanism for light detection, cycling excitation process (CEP). This mechanism relies on the localized bandtail states which involve Auger excitation process and k-selection rule relaxation. There were many previous works showing attractive characteristics of CEP devices, including high detection efficiency, low noise, high speed, low operation voltage, etc. This work mainly demonstrates the experimental characterization and physical models for the amorphous silicon (a-Si) CEP detectors. CEP mechanism has the fundamental difference from impact ionization in all APDs. One of the significant differences is its intrinsically athermalized performance. The temperature sensitivity of the standard a-Si CEP detectors from 200 K to 350 K is found to be nearly temperature independent. This athermalized multiplication characteristic in a-Si CEP detectors offers significant advantages over the impact ionization process in conventional APDs. Temperature sensitivity is a key consideration for detector arrays with readout circuits in LiDAR and imaging applications. The athermalized property can tolerate large temperature variations to achieve stable gain and photon detection efficiency, as well as low pixilation noise with the relaxation of precise temperature control. The detection range of CEP devices can be designed for certain wavelengths by assembling a proper absorption medium. An innovative design of an uncooled high-performance, longwave-infrared quantum detector made of an a-Ge layer and an a-Si layer is demonstrated. The photoexcitation mainly occurs in a-Ge and then the carriers can transport to the a-Si layer for multiplication. This detector has the highest detectivity among the reported room-temperature LWIR quantum detectors and the NEP value sets the world record. This LWIR quantum detector has great potential to meet the performance and cost requirements for many applications: night vision, robotic and machine vision, medical imaging, remote sensing, etc. Finally, the first stage of the CMOS compatible process development for several CEP detector structures is accomplished. The characterization of a-Si deposition by CMOS foundry works in parallel with the design of the hybrid process: incorporating CMOS process and laboratory process. The hybrid process flow for both parts has been demonstrated with the sample layout set for singular device designs and pixel arrays.

We report on methane (CH4) stable isotope (d13C and d2H) measurements from landfast sea ice collected near Barrow (Utqiagvik, Alaska) and Cape Evans (Antarctica) over the winter-to-spring transition. These measurements provide novel insights into pathways of CH4 production and consumption in sea ice. We found substantial differences between the two sites. Sea ice overlying the shallow shelf of Barrow was supersaturated in CH4 with a clear microbial origin, most likely from methanogenesis in the sediments. We estimated that in situ CH4 oxidation consumed a substantial fraction of the CH4 being supplied to the sea ice, partly explaining the large range of isotopic values observed (d13C between -68.5 and -48.5 ‰ and d2H between -246 and -104 ‰). Sea ice at Cape Evans was also supersaturated in CH4 but with surprisingly high d13C values (between -46.9 and -13.0 ‰), whereas d2H values (between -313 and -113 ‰) were in the range of those observed at Barrow.These are the first measurements of CH4 isotopic composition in Antarctic sea ice. Our data set suggests a potential combination of a hydrothermal source, in the vicinity of the Mount Erebus, with aerobic CH4 formation in sea ice, although the metabolic pathway for the latter still needs to be elucidated. Our observations show that sea ice needs to be considered as an active biogeochemical interface, contributing to CH4 production and consumption, which disputes the standing paradigm that sea ice is an inert barrier passively accumulating CH4 at the ocean-atmosphere boundary.

The objective of this study was to assess the O2 budget in the water under sea ice combining observations and modelling. Modelling was used to discriminate between physical processes, gas-specific transport (i.e. ice-atmosphere gas fluxes and gas bubble buoyancy) and bacterial respiration (BR) and to constrain bacterial growth efficiency (BGE). A module describing the changes of the under-ice water properties, due to brine rejection and temperature-dependent BR, was implemented in the one-dimensional halo-thermodynamic sea ice model LIM1D. Our results show that BR was the dominant biogeochemical driver of O2 concentration in the water under ice (in a system without primary producers), followed by gas specific transport. The model suggests that the actual contribution of BR and gas specific transport to the change in seawater O2 concentration was 37% during ice growth and 48% during melt. BGE in the water under sea ice, as retrieved from the simulated O2 budget, was found to be between 0.4 and 0.5, which is in line with published BGE values for cold marine waters. Given the importance of BR to seawater O2 in the present study, it can be assumed that bacteria contribute substantially to organic matter consumption and gas fluxes in ice-covered polar oceans. In addition, we propose a parameterization of polar marine bacterial respiration, based on the strong temperature dependence of bacterial respiration and the high growth efficiency observed here, for further biogeochemical ocean modelling applications, such as regional or large-scale Earth System models., SCOPUS: ar.j, info:eu-repo/semantics/published

The ongoing changes in the extent and the properties of sea ice, associated with the warming climate, are affecting the polar ecosystem and the interactions between the atmosphere, sea ice and the underlying waters. How sea ice biogeochemistry will change in the foreseeable future is currently uncertain, but is a crucial problem to tackle.To better understand how sea ice biogeochemistry could change, we investigated the factors regulating the distribution of some dissolved compounds (e.g. nutrients, dissolved organic matter (DOM)) and gaseous compounds (e.g. Ar, O2, N2, CH4) in sea ice, from ice growth to ice decay. The results were obtained from a 19-day indoor experiment in Hamburg (Germany) and a five-month-long field survey in Barrow (Alaska). They were then compared to the physical properties of the ice (temperature, salinity, and other derived parameters such as brine volume fraction) and different biological parameters (bacterial activity, bacterial abundance, chlorophyll-a and phaeopigments).Our work indicates that the physical properties of sea ice exert a strong influence on the distribution of the biogeochemical compounds in the ice, through their impact on brine dynamics, gas bubble formation and ice permeability. We have described 4 stages of brine dynamics, which affect the distribution of the dissolved compounds (e.g. silicate and DOM) in sea ice. However, inert gas (Ar) shows a different dynamic in comparison to the dissolved compounds, indicating a different transport pathway. We suggest that the formation of gas bubbles in sea ice is responsible for that different transport pathway, because gas bubbles should move upward owing to their buoyancy in comparison to brine, while dissolved compounds are drained downward due to gravity. Our observations further indicate that the critical permeability threshold for the upward gas bubble transport should range between 7.5 and 10 % of brine volume fraction, which is higher than the 5 % suggested for the downward brine transport. Increasing ice permeability and prolonged gas exchange tend to draw gas concentrations toward their solubility values, except when the under-ice water is supersaturated relative to the atmosphere (e.g. CH4) or when in-situ production occurs in sea ice (e.g. O2).Because ammonium and O2 obviously accumulate in the ice layers where convection is limited, we suggest that the changes of these biogeochemical compounds in sea ice depend on the competing effect between the physical transport and the biological activity; the biological impact on these biogeochemical compounds in sea ice is obvious when the biological production rate exceeds largely the physical transport rate. We further discussed on the potential of using Ar and N2 as inert tracers to correct the physical controls on O2 and to determine the net community production in sea ice.In addition to the physical and biological controls, the chemical properties of some biogeochemical compounds (e.g. nitrate, ammonium, DOM) may further influence their distribution in sea ice; further investigations are however needed to confirm this.Finally, based on our findings, we present an update of the processes regulating the distribution of gases in sea ice, with references to recent observations supporting each of the process. We also provide some insights on how sea ice biogeochemistry could change in the future and the research priorities for an accurate quantification of these changes.Les changements dans l’extension et les propriétés de la glace de la mer, liés au réchauffement climatique, affectent l’écosystème polaire, ainsi que les interactions entre l’atmosphère, la glace de mer et l’eau sous-jacente. Cependant, des incertitudes subsistent quant aux changements potentiels qui affecteront la biogéochimie de la glace de mer dans un futur proche.Afin de mieux comprendre les changements potentiels qui affecteront la biogéochimie de la glace de mer, nous avons étudié les facteurs qui influencent la distribution de certains composés dissouts (e.g. nutriments, matière organique dissoute (DOM)) et gazeux (e.g. Ar, O2, N2, CH4) au sein de la glace de mer, depuis la croissance de la glace, jusqu’à sa fonte. Les résultats ont été obtenus à partir d’une expérience de 19 jours dans un bassin expérimental à Hambourg (Allemagne) et une étude de terrain de 5 mois à Barrow (Alaska). Ils ont été ensuite comparés aux propriétés physiques de la glace (température, salinité et autres paramètres dérivés) et à des paramètres biologiques (activité bactérienne, abondance bactérienne, chlorophylle-a et phaeopigments).Nos travaux ont montré que les propriétés physiques de la glace exercent une forte influence sur la répartition des composes biogéochimiques dans la glace de mer, à travers leur impact sur la dynamique des saumures, la formation de bulles de gaz et la perméabilité de la glace. Nous avons décrit 4 stades dans la dynamique des saumures qui influencent la distribution des composés dissouts (e.g. silice et DOM) dans la glace. Cependant, le gaz inerte étudié (Ar) montre une dynamique différente de celle des composés dissouts, indiquant un mécanisme de transport différent. Nous suggérons que la formation de bulles de gaz dans la glace de mer est le mécanisme responsable de cette différence, parce que les bulles de gaz devraient migrer vers le haut, à cause de leur différence de densité par rapport aux saumures, alors que les saumures sont drainées vers le bas à cause de la gravité. Nos observations montrent également que le seuil critique de perméabilité pour l’ascension des bulles de gaz devrait se trouver entre 7.5 et 10 % de volume relatif en saumure ;seuil qui est plus élevé que les 5 % suggérés pour le transport de saumure vers le bas. L’augmentation de la perméabilité de la glace et les échanges de gaz prolongés tendent à amener les concentrations de gaz vers leur valeur de solubilité, sauf lorsque l’eau sous-jacente présente une sursaturation parrapport à l’atmosphère (e.g. CH4), ou lorsque une production in-situ se produit au sein de la glace (e.g. O2).Etant donné que l’ammonium et O2 s’accumulent clairement dans les couches de glace où la convection est limitée, nous suggérons que les variations de ces composés biogéochimiques dans la glace dépendent de la balance entre le transport physique et l’activité biologique ;l’impact de cette dernière sur les composés biogéochimiques est particulièrement visible lorsque le taux de production biologique du composé excède largement la vitesse d’élimination du composé par le transport physique. Nous avons ensuite discuté du potentiel d’utiliser Ar et N2 comme traceurs inertes pour corriger l’impact des processus physiques sur les variations de O2, afin de déterminer la production communautaire nette dans la glace de mer.Les propriétés chimiques de certains composés biogéochimiques (e.g. nitrate, ammonium, DOM) pourraient également influencer leur répartition au sein de la glace de mer, en plus des processus physiques et biologiques. Cependant, il est nécessaire d’avoir plus d’études à ce sujet pour confirmer cela.Enfin, sur base de nos résultats, nous présentons une mise à jour des processus qui régulent la répartition des gaz dans la glace de mer, avec des références à des observations récentes qui illustrent chacun des processus. Nous donnons également un aperçu des changements qui pourraient affecter la biogéochimie de la glace de mer à l’avenir, et des pistes de recherches pour une quantification précise de ces changements., Doctorat en Sciences, info:eu-repo/semantics/nonPublished

A cross-linked polyurethane with a novel nonlinear optical (NLO) chromophore [2-(4′-N,N-dihydroxyethylphenylazo)-3,5-dinitrothiophene] covalently incorporated for second-order optical nonlinearity was developed. High optical-quality films can be obtained from the prepared polymer. Resonance-enhanced second-harmonic coefficient (d33) of 66 pm V−1 at 1.064 μm fundamental wavelength of the poled films was obtained. Test on temporal stability shows that when the films were kept in an oven at 100°C for 1000 h in air, 75% of the NLO signal still remained.

2-Aminothiophene derivatives are the key intermediates for the present synthesis. It is known that the synthesis of 2-aminothiophene is troublesome although it is a rather simple heterocycle. In this work, an early report was newly developed as a basis for the efficient synthesis of thiophene-ring-containing chromophore components for photonic polymers. 2-Amino-5-nitrothiophene and 2-amino-3,5-dinitrothiophene were synthesized in excellent yield. After diazotization, the 2-aminothiophene derivatives were directly treated with N-phenyldiethanolamine to afford two-electron push–pull compounds. A similar styryl compound was also prepared. All of these chromophore molecules have further polymerizable hydroxy groups on one end of the molecule. These compounds are currently showing interesting potential in making highly sensitive, nonlinear optical polymeric materials.