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Increasing Earth’s surface air temperature yields an intensification of its hydrological cycle. As a consequence, the risk of river floods will increase regionally within the next two decades due to the atmospheric warming caused by past anthropogenic greenhouse gas emissions. The direct economic losses caused by these floods can yield regionally heterogeneous losses and gains by propagation within the global trade and supply network. Here we show that, in the absence of large-scale structural adaptation, the total economic losses due to fluvial floods will increase in the next 20 years globally by 17% despite partial compensation through market adjustment within the global trade network. China will suffer the strongest direct losses, with an increase of 82%. The United States is mostly affected indirectly through its trade relations. By contrast to the United States, recent intensification of the trade relations with China leaves the European Union better prepared for the import of production losses in the future.
This thesis covers the topic ”Thinning and Turbulence in Aqueous Films”. Experimental studies in two-dimensional systems gained an increasing amount of attention during the last decade. Thin liquid films serve as paradigms of atmospheric convection, thermal convection in the Earth’s mantle or turbulence in magnetohydrodynamics. Recent research on colloids, interfaces and nanofluids lead to advances in the developtment of micro-mixers (lab-on-a-chip devices). In this project a detailed description of a thin film experiment with focus on the particular surface forces is presented. The impact of turbulence on the thinning of liquid films which are oriented parallel to the gravitational force is studied. An experimental setup was developed which permits the capturing of thin film interference patterns under controlled surface and atmospheric conditions. The measurement setup also serves as a prototype of a mixer on the basis of thermally induced turbulence in liquid thin films with thicknesses in the nanometer range. The convection is realized by placing a cooled copper rod in the center of the film. The temperature gradient between the rod and the atmosphere results in a density gradient in the liquid film, so that different buoyancies generate turbulence. In the work at hand the thermally driven convection is characterized by a newly developed algorithm, named Cluster Imaging Velocimetry (CIV). This routine determines the flow relevant vector fields (velocity and deformation). On the basis of these insights the flow in the experiment was investigated with respect to its mixing properties. The mixing characteristics were compared to theoretical models and mixing efficiency of the flow scheme calculated. The gravitationally driven thinning of the liquid film was analyzed under the influence of turbulence. Strong shear forces lead to the generation of ultra-thin domains which consist of Newton black film. Due to the exponential expansion of the thin areas and the efficient mixing, this two-phase flow rapidly turns into the convection of only ultra-thin film. This turbulence driven transition was observed and quantified for the first time. The existence of stable convection in liquid nanofilms was proven for the first time in the context of this work.
Wisotzki, Lutz ; Bacon, R. ; Brinchmann, J. ; Cantalupo, S. ; Richter, Philipp ; Schaye, J. ; Schmidt, Kasper Borello ; Urrutia, Tanya ; Weilbacher, Peter Michael ; Akhlaghi, M. ; Bouche, N. ; Contini, T. ; Guiderdoni, B. ; Herenz, E. C. ; Inami, H. ; Kerutt, Josephine Victoria ; Leclercq, F. ; Marino, R. A. ; Maseda, M. ; Monreal-Ibero, A. ; Nanayakkara, T. ; Richard, J. ; Saust, R. ; Steinmetz, Matthias ; Wendt, Martin
Galaxies are surrounded by large reservoirs of gas, mostly hydrogen, that are fed by inflows from the intergalactic medium and by outflows from galactic winds. Absorption-line measurements along the lines of sight to bright and rare background quasars indicate that this circumgalactic medium extends far beyond the starlight seen in galaxies, but very little is known about its spatial distribution. The Lyman-alpha transition of atomic hydrogen at a wavelength of 121.6 nanometres is an important tracer of warm (about 104 kelvin) gas in and around galaxies, especially at cosmological redshifts greater than about 1.6 at which the spectral line becomes observable from the ground. Tracing cosmic hydrogen through its Lyman-a emission has been a long-standing goal of observational astrophysics(1-3), but the extremely low surface brightness of the spatially extended emission is a formidable obstacle. A new window into circumgalactic environments was recently opened by the discovery of ubiquitous extended Lyman-alpha emission from hydrogen around high-redshift galaxies(4,5). Such measurements were previously limited to especially favourable systems(6-8) or to the use of massive statistical averaging(9,10) because of the faintness of this emission. Here we report observations of low-surface-brightness Lyman-alpha emission surrounding faint galaxies at redshifts between 3 and 6. We find that the projected sky coverage approaches 100 per cent. The corresponding rate of incidence (the mean number of Lyman-alpha emitters penetrated by any arbitrary line of sight) is well above unity and similar to the incidence rate of high-column-density absorbers frequently detected in the spectra of distant quasars(11-14). This similarity suggests that most circumgalactic atomic hydrogen at these redshifts has now been detected in emission.
We have used techniques of nonlinear dynamics to compare a special model for the reversals of the Earth's magnetic field with the observational data. Although this model is rather simple, there is no essential difference to the data by means of well-known characteristics, such as correlation function and probability distribution. Applying methods of symbolic dynamics we have found that the considered model is not able to describe the dynamical properties of the observed process. These significant differences are expressed by algorithmic complexity and Renyi information.
The dynamics of noisy bistable systems is analyzed by means of Lyapunov exponents and measures of complexity. We consider both the classical Kramers problem with additive white noise and the case when the barrier fluctuates due to additional external colored noise. In case of additive noise we calculate the Lyapunov exponents and all measures of complexity analytically as functions of the noise intensity resp. the mean escape time. For the problem of fluctuating barrier the usual description of the dynamics with the mean escape time is not sufficient. The application of the concept of measures of complexity allows to describe the structures of motion in more detail. Most complexity measures sign the value of correlation time at which the phenomenon of resonant activation occurs with an extremum.
Wojcik, Michal ; Brinkmann, Pia ; Zdunek, Rafał ; Riebe, Daniel ; Beitz, Toralf ; Merk, Sven ; Cieslik, Katarzyna ; Mory, David ; Antonczak, Arkadiusz
Laser-induced breakdown spectroscopy (LIBS) analysers are becoming increasingly common for material classification purposes. However, to achieve good classification accuracy, mostly noncompact units are used based on their stability and reproducibility. In addition, computational algorithms that require significant hardware resources are commonly applied. For performing measurement campaigns in hard-to-access environments, such as mining sites, there is a need for compact, portable, or even handheld devices capable of reaching high measurement accuracy. The optics and hardware of small (i.e., handheld) devices are limited by space and power consumption and require a compromise of the achievable spectral quality. As long as the size of such a device is a major constraint, the software is the primary field for improvement. In this study, we propose a novel combination of handheld LIBS with non-negative tensor factorisation to investigate its classification capabilities of copper minerals. The proposed approach is based on the extraction of source spectra for each mineral (with the use of tensor methods) and their labelling based on the percentage contribution within the dataset. These latent spectra are then used in a regression model for validation purposes. The application of such an approach leads to an increase in the classification score by approximately 5% compared to that obtained using commonly used classifiers such as support vector machines, linear discriminant analysis, and the k-nearest neighbours algorithm.
The conversion of light energy into other molecular energetic degrees of freedom is often dominated by ultrafast, non-adiabatic processes. Femtosecond spectroscopy with optical pulses has helped in shaping our understanding of crucial processes in molecular energy-conversion. The advent of new, ultrashort and bright X-ray free electron laser sources opens the possibility to use X-ray-typical element and site sensitivity for ultrafast molecular research. We present two types of spectroscopy, ultrafast Auger and ultrafast X-ray absorption spectroscopy, and discuss their sensitivity to molecular processes. While Auger spectroscopy is able to monitor bond distance changes in the vicinity of an X-ray created core hole, near-edge absorption spectroscopy can deliver high-fidelity information on non-adiabatic transitions involving lone-pair orbitals. We demonstrate these features on the example of the UV-excited nucleobase thymine, investigated at the oxygen K-edge. We find a C-O bond elongation in the Auger data in addition to pi pi*/n pi* non-adiabatic transition in X-ray near-edge absorption. We compare the results from both methods and draw a conclusive scenario of non-adiabatic molecular relaxation after UV excitation.
Wolf, Thomas J. A. ; Holzmeier, Fabian ; Wagner, Isabella ; Berrah, Nora ; Bostedt, Christoph ; Bozek, John ; Bucksbaum, Philip H. ; Coffee, Ryan ; Cryan, James ; Farrell, Joe ; Feifel, Raimund ; Martinez, Todd J. ; McFarland, Brian ; Mucke, Melanie ; Nandi, Saikat ; Tarantelli, Francesco ; Fischer, Ingo ; Gühr, Markus
Molecules often fragment after photoionization in the gas phase. Usually, this process can only be investigated spectroscopically as long as there exists electron correlation between the photofragments. Important parameters, like their kinetic energy after separation, cannot be investigated. We are reporting on a femtosecond time-resolved Auger electron spectroscopy study concerning the photofragmentation dynamics of thymine. We observe the appearance of clearly distinguishable signatures from thymine′s neutral photofragment isocyanic acid. Furthermore, we observe a time-dependent shift of its spectrum, which we can attribute to the influence of the charged fragment on the Auger electron. This allows us to map our time-dependent dataset onto the fragmentation coordinate. The time dependence of the shift supports efficient transformation of the excess energy gained from photoionization into kinetic energy of the fragments. Our method is broadly applicable to the investigation of photofragmentation processes.
Wolf, Thomas J. A. ; Holzmeier, Fabian ; Wagner, Isabella ; Berrah, Nora ; Bostedt, Christoph ; Bozek, John ; Bucksbaum, Philip H. ; Coffee, Ryan ; Cryan, James ; Farrell, Joe ; Feifel, Raimund ; Martinez, Todd J. ; McFarland, Brian ; Mucke, Melanie ; Nandi, Saikat ; Tarantelli, Francesco ; Fischer, Ingo ; Gühr, Markus
Molecules often fragment after photoionization in the gas phase. Usually, this process can only be investigated spectroscopically as long as there exists electron correlation between the photofragments. Important parameters, like their kinetic energy after separation, cannot be investigated. We are reporting on a femtosecond time-resolved Auger electron spectroscopy study concerning the photofragmentation dynamics of thymine. We observe the appearance of clearly distinguishable signatures from thymine′s neutral photofragment isocyanic acid. Furthermore, we observe a time-dependent shift of its spectrum, which we can attribute to the influence of the charged fragment on the Auger electron. This allows us to map our time-dependent dataset onto the fragmentation coordinate. The time dependence of the shift supports efficient transformation of the excess energy gained from photoionization into kinetic energy of the fragments. Our method is broadly applicable to the investigation of photofragmentation processes.
Wolf, Thomas J. A. ; Parrish, Robert M. ; Myhre, Rolf H. ; Martinez, Todd J. ; Koch, Henrik ; Gühr, Markus
We studied the photoinduced ultrafast relaxation dynamics of the nucleobase thymine using gas-phase time-resolved photoelectron spectroscopy. By employing extreme ultraviolet pulses from high harmonic generation for photoionization, we substantially extend our spectral observation window with respect to previous studies. This enables us to follow relaxation of the excited state population all the way to low-lying electronic states including the ground state. In thymine, we observe relaxation from the optically bright (1)pi pi* state of thymine to a dark (1)n pi* state within 80 +/- 30 fs. The (1)n pi* state relaxes further within 3.5 +/- 0.3 ps to a low-lying electronic state. By comparison with quantum chemical simulations, we can unambiguously assign its spectroscopic signature to the (3)pi pi* state. Hence, our study draws a comprehensive picture of the relaxation mechanism of thymine including ultrafast intersystem crossing to the triplet manifold.
Perovskite solar cells have become one of the most studied systems in the quest for new, cheap and efficient solar cell materials. Within a decade device efficiencies have risen to >25% in single-junction and >29% in tandem devices on top of silicon. This rapid improvement was in many ways fortunate, as e. g. the energy levels of commonly used halide perovskites are compatible with already existing materials from other photovoltaic technologies such as dye-sensitized or organic solar cells. Despite this rapid success, fundamental working principles must be understood to allow concerted further improvements. This thesis focuses on a comprehensive understanding of recombination processes in functioning devices.
First the impact the energy level alignment between the perovskite and the electron transport layer based on fullerenes is investigated. This controversial topic is comprehensively addressed and recombination is mitigated through reducing the energy difference between the perovskite conduction band minimum and the LUMO of the fullerene. Additionally, an insulating blocking layer is introduced, which is even more effective in reducing this recombination, without compromising carrier collection and thus efficiency. With the rapid efficiency development (certified efficiencies have broken through the 20% ceiling) and thousands of researchers working on perovskite-based optoelectronic devices, reliable protocols on how to reach these efficiencies are lacking. Having established robust methods for >20% devices, while keeping track of possible pitfalls, a detailed description of the fabrication of perovskite solar cells at the highest efficiency level (>20%) is provided. The fabrication of low-temperature p-i-n structured devices is described, commenting on important factors such as practical experience, processing atmosphere & temperature, material purity and solution age. Analogous to reliable fabrication methods, a method to identify recombination losses is needed to further improve efficiencies. Thus, absolute photoluminescence is identified as a direct way to quantify the Quasi-Fermi level splitting of the perovskite absorber (1.21eV) and interfacial recombination losses the transport layers impose, reducing the latter to ~1.1eV. Implementing very thin interlayers at both the p- and n-interface (PFN-P2 and LiF, respectively), these losses are suppressed, enabling a VOC of up to 1.17eV. Optimizing the device dimensions and the bandgap, 20% devices with 1cm2 active area are demonstrated. Another important consideration is the solar cells’ stability if subjected to field-relevant stressors during operation. In particular these are heat, light, bias or a combination thereof. Perovskite layers – especially those incorporating organic cations – have been shown to degrade if subjected to these stressors. Keeping in mind that several interlayers have been successfully used to mitigate recombination losses, a family of perfluorinated self-assembled monolayers (X-PFCn, where X denotes I/Br and n = 7-12) are introduced as interlayers at the n-interface. Indeed, they reduce interfacial recombination losses enabling device efficiencies up to 21.3%. Even more importantly they improve the stability of the devices. The solar cells with IPFC10 are stable over 3000h stored in the ambient and withstand a harsh 250h of MPP at 85◦C without appreciable efficiency losses. To advance further and improve device efficiencies, a sound understanding of the photophysics of a device is imperative. Many experimental observations in recent years have however drawn an inconclusive picture, often suffering from technical of physical impediments, disguising e. g. capacitive discharge as recombination dynamics. To circumvent these obstacles, fully operational, highly efficient perovskites solar cells are investigated by a combination of multiple optical and optoelectronic probes, allowing to draw a conclusive picture of the recombination dynamics in operation. Supported by drift-diffusion simulations, the device recombination dynamics can be fully described by a combination of first-, second- and third-order recombination and JV curves as well as luminescence efficiencies over multiple illumination intensities are well described within the model. On this basis steady state carrier densities, effective recombination constants, densities-of-states and effective masses are calculated, putting the devices at the brink of the radiative regime. Moreover, a comprehensive review of recombination in state-of-the-art devices is given, highlighting the importance of interfaces in nonradiative recombination. Different strategies to assess these are discussed, before emphasizing successful strategies to reduce interfacial recombination and pointing towards the necessary steps to further improve device efficiency and stability. Overall, the main findings represent an advancement in understanding loss mechanisms in highly efficient solar cells. Different reliable optoelectronic techniques are used and interfacial losses are found to be of grave importance for both efficiency and stability. Addressing the interfaces, several interlayers are introduced, which mitigate recombination losses and degradation.
Wolff, Christian Michael ; Canil, Laura ; Rehermann, Carolin ; Nguyen, Ngoc Linh ; Zu, Fengshuo ; Ralaiarisoa, Maryline ; Caprioglio, Pietro ; Fiedler, Lukas ; Stolterfoht, Martin ; Kogikoski, Junior, Sergio ; Bald, Ilko ; Koch, Norbert ; Unger, Eva L. ; Dittrich, Thomas ; Abate, Antonio ; Neher, Dieter
Woodfield, Emma E. ; Glauert, Saraha A. ; Menietti, J. Douglas ; Averkamp, Terrance F. ; Horne, Richard B. ; Shprits, Yuri
Electron acceleration at Saturn due to whistler mode chorus waves has previously been assumed to be ineffective; new data closer to the planet show it can be very rapid (factor of 104 flux increase at 1 MeV in 10 days compared to factor of 2). A full survey of chorus waves at Saturn is combined with an improved plasma density model to show that where the plasma frequency falls below the gyrofrequency additional strong resonances are observed favoring electron acceleration. This results in strong chorus acceleration between approximately 2.5 R-S and 5.5 R-S outside which adiabatic transport may dominate. Strong pitch angle dependence results in butterfly pitch angle distributions that flatten over a few days at 100s keV, tens of days at MeV energies which may explain observations of butterfly distributions of MeV electrons near L = 3. Including cross terms in the simulations increases the tendency toward butterfly distributions. Plain Language Summary Radiation belts are hazardous regions found around several of the planets in our Solar System. They consist of very hot, electrically charged particles trapped in the magnetic field of the planet. At Saturn the most important way to heat these particles has for many years been thought to involve the particles drifting closer toward the planet. This paper adds to the emerging idea at Saturn that a different way to heat the particles is also possible where the heating is done by waves, in a similar way to what we find at the Earth. We use recent information from the Cassini spacecraft on the number and location of particles and also of the waves strength and location combined with computer simulations to show that a particular wave called chorus is excellent at heating the particles where the surrounding number of cold particles is low.
Woodfield, Emma E. ; Horne, Richard B. ; Glauert, S. A. ; Menietti, J. D. ; Shprits, Yuri ; Kurth, William S.
At Saturn electrons are trapped in the planet’s magnetic field and accelerated to relativistic energies to form the radiation belts, but how this dramatic increase in electron energy occurs is still unknown. Until now the mechanism of radial diffusion has been assumed but we show here that in-situ acceleration through wave particle interactions, which initial studies dismissed as ineffectual at Saturn, is in fact a vital part of the energetic particle dynamics there. We present evidence from numerical simulations based on Cassini spacecraft data that a particular plasma wave, known as Z-mode, accelerates electrons to MeV energies inside 4 RS (1 RS = 60,330 km) through a Doppler shifted cyclotron resonant interaction. Our results show that the Z-mode waves observed are not oblique as previously assumed and are much better accelerators than O-mode waves, resulting in an electron energy spectrum that closely approaches observed values without any transport effects included.
The availability of large data sets has allowed researchers to uncover complex properties in complex systems, such as complex networks and human dynamics. A vast number of systems, from the Internet to the brain, power grids, ecosystems, can be represented as large complex networks. Dynamics on and of complex networks has attracted more and more researchers’ interest. In this thesis, first, I introduced a simple but effective dynamical optimization coupling scheme which can realize complete synchronization in networks with undelayed and delayed couplings and enhance the small-world and scale-free networks’ synchronizability. Second, I showed that the robustness of scale-free networks with community structure was enhanced due to the existence of communities in the networks and some of the response patterns were found to coincide with topological communities. My results provide insights into the relationship between network topology and the functional organization in complex networks from another viewpoint. Third, as an important kind of nodes of complex networks, human detailed correspondence dynamics was studied by both data and the model. A new and general type of human correspondence pattern was found and an interacting priority-queues model was introduced to explain it. The model can also embrace a range of realistic social interacting systems such as email and letter communication. My findings provide insight into various human activities both at the individual and network level. Fourth, I present clearly new evidence that human comment behavior in on-line social systems, a different type of interacting human dynamics, is non-Poissonian and a model based on the personal attraction was introduced to explain it. These results are helpful for discovering regular patterns of human behavior in on-line society and the evolution of the public opinion on the virtual as well as real society. Finally, there are conclusion and outlook of human dynamics and complex networks.
Computer-based analysis of preservice teachers' written reflections could enable educational scholars to design personalized and scalable intervention measures to support reflective writing. Algorithms and technologies in the domain of research related to artificial intelligence have been found to be useful in many tasks related to reflective writing analytics such as classification of text segments. However, mostly shallow learning algorithms have been employed so far. This study explores to what extent deep learning approaches can improve classification performance for segments of written reflections. To do so, a pretrained language model (BERT) was utilized to classify segments of preservice physics teachers' written reflections according to elements in a reflection-supporting model. Since BERT has been found to advance performance in many tasks, it was hypothesized to enhance classification performance for written reflections as well. We also compared the performance of BERT with other deep learning architectures and examined conditions for best performance. We found that BERT outperformed the other deep learning architectures and previously reported performances with shallow learning algorithms for classification of segments of reflective writing. BERT starts to outperform the other models when trained on about 20 to 30% of the training data. Furthermore, attribution analyses for inputs yielded insights into important features for BERT's classification decisions. Our study indicates that pretrained language models such as BERT can boost performance for language-related tasks in educational contexts such as classification.
Several large-scale cryosphere elements such as the Arctic summer sea ice, the mountain glaciers, the Greenland and West Antarctic Ice Sheet have changed substantially during the last century due to anthropogenic global warming. However, the impacts of their possible future disintegration on global mean temperature (GMT) and climate feedbacks have not yet been comprehensively evaluated. Here, we quantify this response using an Earth system model of intermediate complexity. Overall, we find a median additional global warming of 0.43 degrees C (interquartile range: 0.39-0.46 degrees C) at a CO2 concentration of 400 ppm. Most of this response (55%) is caused by albedo changes, but lapse rate together with water vapour (30%) and cloud feedbacks (15%) also contribute significantly. While a decay of the ice sheets would occur on centennial to millennial time scales, the Arctic might become ice-free during summer within the 21st century. Our findings imply an additional increase of the GMT on intermediate to long time scales. The disintegration of cryosphere elements such as the Arctic summer sea ice, mountain glaciers, Greenland and West Antarctica is associated with temperature and radiative feedbacks. In this work, the authors quantify these feedbacks and find an additional global warming of 0.43 degrees C.
Würfel, Uli ; Perdigón-Toro, Lorena ; Kurpiers, Jona ; Wolff, Christian Michael ; Caprioglio, Pietro ; Rech, Jeromy James ; Zhu, Jingshuai ; Zhan, Xiaowei ; You, Wei ; Shoaee, Safa ; Neher, Dieter ; Stolterfoht, Martin
Charge extraction in organic solar cells (OSCs) is commonly believed to be limited by bimolecular recombination of photogenerated charges. However, the fill factor of OSCs is usually almost entirely governed by recombination processes that scale with the first order of the light intensity. This linear loss was often interpreted to be a consequence of geminate or trap-assisted recombination. Numerical simulations show that this linear dependence is a direct consequence of the large amount of excess dark charge near the contact. The first-order losses increase with decreasing mobility of minority carriers, and we discuss the impact of several material and device parameters on this loss mechanism. This work highlights that OSCs are especially vulnerable to injected charges as a result of their poor charge transport properties. This implies that dark charges need to be better accounted for when interpreting electro-optical measurements and charge collection based on simple figures of merit.
Fragmentation of endohedral fullerene Ho3N@C-80 in an intense femtosecond near-infrared laser field
(2018)
Xiong, Hui ; Fang, Li ; Osipov, Timur ; Kling, Nora G. ; Wolf, Thomas J. A. ; Sistrunk, Emily ; Obaid, Razib ; Gühr, Markus ; Berrah, Nora
The fragmentation of gas phase endohedral fullerene, Ho3N@C-80, was investigated using femtosecond near-infrared laser pulses with an ion velocity map imaging spectrometer. We observed that Ho+ abundance associated with carbon cage opening dominates at an intensity of 1.1 x 10(14) W/cm(2). As the intensity increases, the Ho+ yield associated with multifragmentation of the carbon cage exceeds the prominence of Ho+ associated with the gentler carbon cage opening. Moreover, the power law dependence of Ho+ on laser intensity indicates that the transition of the most likely fragmentation mechanisms occurs around 2.0 x 10(14) W/cm(2).
The Role of Super-Atom Molecular Orbitals in Doped Fullerenes in a Femtosecond Intense Laser Field
(2017)
Xiong, Hui ; Mignolet, Benoit ; Fang, Li ; Osipov, Timur ; Wolf, Thomas J. A. ; Sistrunk, Emily ; Gühr, Markus ; Remacle, Francoise ; Berrah, Nora
The interaction of gas phase endohedral fullerene Ho3N@C-80 with intense (0.1-5 x 10(14) W/cm(2)), short (30 fs), 800 nm laser pulses was investigated. The power law dependence of Ho3N@C-80(q+), q = 1-2, was found to be different from that of C-60. Time-dependent density functional theory computations revealed different light-induced ionization mechanisms. Unlike in C-60, in doped fullerenes, the breaking of the cage spherical symmetry makes super atomic molecular orbital (SAMO) states optically active. Theoretical calculations suggest that the fast ionization of the SAMO states in Ho3N@C-80 is responsible for the n = 3 power law for singly charged parent molecules at intensities lower than 1.2 x 10(14) W/cm(2).