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Strong light-matter coupling can re-arrange the exciton energies in organic semiconductors. Here, we exploit strong coupling by embedding a fullerene-free organic solar cell (OSC) photo-active layer into an optical microcavity, leading to the formation of polariton peaks and a red-shift of the optical gap. At the same time, the open-circuit voltage of the device remains unaffected. This leads to reduced photon energy losses for the low-energy polaritons and a steepening of the absorption edge. While strong coupling reduces the optical gap, the energy of the charge-transfer state is not affected for large driving force donor-acceptor systems. Interestingly, this implies that strong coupling can be exploited in OSCs to reduce the driving force for electron transfer, without chemical or microstructural modifications of the photoactive layer. Our work demonstrates that the processes determining voltage losses in OSCs can now be tuned, and reduced to unprecedented values, simply by manipulating the device architecture.
Charge transport layers (CTLs) are key components of diffusion controlled perovskite solar cells, however, they can induce additional non-radiative recombination pathways which limit the open circuit voltage (V-OC) of the cell. In order to realize the full thermodynamic potential of the perovskite absorber, both the electron and hole transport layer (ETL/HTL) need to be as selective as possible. By measuring the photoluminescence yield of perovskite/CTL heterojunctions, we quantify the non-radiative interfacial recombination currents in pin- and nip-type cells including high efficiency devices (21.4%). Our study comprises a wide range of commonly used CTLs, including various hole-transporting polymers, spiro-OMeTAD, metal oxides and fullerenes. We find that all studied CTLs limit the V-OC by inducing an additional non-radiative recombination current that is in most cases substantially larger than the loss in the neat perovskite and that the least-selective interface sets the upper limit for the V-OC of the device. Importantly, the V-OC equals the internal quasi-Fermi level splitting (QFLS) in the absorber layer only in high efficiency cells, while in poor performing devices, the V-OC is substantially lower than the QFLS. Using ultraviolet photoelectron spectroscopy and differential charging capacitance experiments we show that this is due to an energy level mis-alignment at the p-interface. The findings are corroborated by rigorous device simulations which outline important considerations to maximize the V-OC. This work highlights that the challenge to suppress non-radiative recombination losses in perovskite cells on their way to the radiative limit lies in proper energy level alignment and in suppression of defect recombination at the interfaces.
Perovskite solar cells (PSCs) are one of the main research topics of the photovoltaic community; with efficiencies now reaching up to 24%, PSCs are on the way to catching up with classical inorganic solar cells. However, PSCs have not yet reached their full potential. In fact, their efficiency is still limited by nonradiative recombination, mainly via trap-states and by losses due to the poor transport properties of the commonly used transport layers (TLs). Indeed, state-of-the-art TLs (especially if organic) suffer from rather low mobilities, typically within 10(-5) and 10(-2) cm(-2) V-1 s(-1), when compared to the high mobilities, 1-10 cm(-2) V-1 s(-1), measured for perovskites. This work presents a comprehensive analysis of the effect of the mobility, thickness, and doping density of the transport layers based on combined experimental and modeling results of two sets of devices made of a solution-processed high-performing triple-cation (PCE approximate to 20%). The results are also cross-checked on vacuum-processed MAPbI(3) devices. From this analysis, general guidelines on how to optimize a TL are introduced and especially a new and simple formula to easily calculate the amount of doping necessary to counterbalance the low mobility of the TLs.
Context. On 27 April 2015, when comet 67P/Churyumov-Gerasimenko was at 1.76 au from the Sun and moving toward perihelion, the OSIRIS and VIRTIS-M instruments on board the Rosetta spacecraft simultaneously observed the evolving dust and gas coma during a complete rotation of the comet. Aims. We aim to characterize the spatial distribution of dust, H2O, and CO2 gas in the inner coma. To do this, we performed a quantitative analysis of the release of dust and gas and compared the observed H2O production rate with the rate we calculated using a thermophysical model. Methods. For this study we selected OSIRIS WAC images at 612 nm (dust) and VIRTIS-M image cubes at 612 nm, 2700 nm (H2O emission band), and 4200 nm (CO2 emission band). We measured the average signal in a circular annulus to study the spatial variation around the comet, and in a sector of the annulus to study temporal variation in the sunward direction with comet rotation, both at a fixed distance of 3.1 km from the comet center. Results. The spatial correlation between dust and water, both coming from the sunlit side of the comet, shows that water is the main driver of dust activity in this time period. The spatial distribution of CO2 is not correlated with water and dust. There is no strong temporal correlation between the dust brightness and water production rate as the comet rotates. The dust brightness shows a peak at 0 degrees subsolar longitude, which is not pronounced in the water production. At the same epoch, there is also a maximum in CO2 production. An excess of measured water production with respect to the value calculated using a simple thermophysical model is observed when the head lobe and regions of the southern hemisphere with strong seasonal variations are illuminated (subsolar longitude 270 degrees-50 degrees). A drastic decrease in dust production when the water production (both measured and from the model) displays a maximum occurs when typical northern consolidated regions are illuminated and the southern hemisphere regions with strong seasonal variations are instead in shadow (subsolar longitude 50 degrees-90 degrees). Possible explanations of these observations are presented and discussed.
On 2015 July 18, near perihelion at a heliocentric distance of 1.28 au, the Visible InfraRed Thermal Imaging Spectrometer (VIRTIS-M) on board the Rosetta spacecraft had the opportunity of observing dust activity in the inner coma with a view of the night side (shadowed side) of comet 67P/Churyumov-Gerasimenko. At the time of the measurements we present here, we observe a dust plume that originates on the far side of the nucleus. We are able to identify the approximate location of its source at the boundary between the Hapi and Anuket regions, and we find that it has been in darkness for some hours before the observation. Assuming that this time span is equal to the conductive time scale, we obtain a thermal inertia in the range 25-36 W K-1 m(-2) s(-1/2). These thermal inertia values can be used to verify with a 3D finite-element method (REM) numerical code whether the surface and subsurface temperatures agree with the values found in the literature. We explored three different configurations: (1) a layer of water ice mixed with dust beneath a dust mantle of 5 mm with thermal inertia of 36 J m(-2) K-1 S-0.5 ; (2) the same structure, but with thermal inertia of 100 J m(-2) K-1 S-0.5; (3) an ice-dust mixture that is directly exposed. Of these three configurations, the first seems to be the most reasonable, both for the low thermal inertia and for the agreement with the surface and subsurface temperatures that have been found for the comet 67P/Churyumov-Gerasimenko. The spectral properties of the plume show that the visible dust color ranged from 16 +/- 4.8%/100 nm to 13 +/- 2.6%/100 nm, indicating that this plume has no detectable color gradient. The morphology of the plume can be classified as a narrow jet that has an estimated total ejected mass of between 6 and 19 tons when we assume size distribution indices between -2.5 and -3.
Time-resolved crystallography reveals allosteric communication aligned with molecular breathing
(2019)
A comprehensive understanding of protein function demands correlating structure and dynamic changes. Using time-resolved serial synchrotron crystallography, we visualized half-of-the-sites reactivity and correlated molecular-breathing motions in the enzyme fluoroacetate dehalogenase. Eighteen time points from 30 milliseconds to 30 seconds cover four turnover cycles of the irreversible reaction. They reveal sequential substrate binding, covalent-intermediate formation, setup of a hydrolytic water molecule, and product release. Small structural changes of the protein mold and variations in the number and placement of water molecules accompany the various chemical steps of catalysis. Triggered by enzyme-ligand interactions, these repetitive changes in the protein framework’s dynamics and entropy constitute crucial components of the catalytic machinery.
We investigate spin-wave resonance modes and their damping in insulating thin films of bismuth-substituted yttrium iron garnet by performing femtosecond magneto-optical pump-probe experiments. For large magnetic fields in the range below the magnetization saturation, we find that the damping of high-order standing spin-wave (SSW) modes is about 40 times lower than that for the fundamental one. The observed phenomenon can be explained by considering different features of magnetic anisotropy and exchange fields that, respectively, define the precession frequency for fundamental and high-order SSWs. These results provide further insight into SSWs in iron garnets and may be exploited in many new photomagnonic devices.
We consider the first-passage problem for N identical independent particles that are initially released uniformly in a finite domain Ω and then diffuse toward a reactive area Γ, which can be part of the outer boundary of Ω or a reaction centre in the interior of Ω. For both cases of perfect and partial reactions, we obtain the explicit formulas for the first two moments of the fastest first-passage time (fFPT), i.e., the time when the first out of the N particles reacts with Γ. Moreover, we investigate the full probability density of the fFPT. We discuss a significant role of the initial condition in the scaling of the average fFPT with the particle number N, namely, a much stronger dependence (1/N and 1/N² for partially and perfectly reactive targets, respectively), in contrast to the well known inverse-logarithmic behaviour found when all particles are released from the same fixed point. We combine analytic solutions with scaling arguments and stochastic simulations to rationalise our results, which open new perspectives for studying the relevance of multiple searchers in various situations of molecular reactions, in particular, in living cells.
We present an analysis of two pulsating subdwarf B stars PHL 457 and EQ Psc observed during the K2 mission. The K2 light curves of both stars show variation consistent with irradiation of a cooler companion by the hot subdwarf. They also show higher frequency oscillations consistent with pulsation. Using new spectroscopic data, we measured the radial velocity, effective temperature, surface gravity, and helium abundance of both hot subdwarfs as a function of orbital phase. We confirm the previously published spectroscopic orbit of PHL 457, and present the first spectroscopic orbit of EQ Psc. The orbital periods are 0.313 and 0.801 d, respectively. For EQPsc, we find a strong correlation between T-eff and orbital phase, due to contribution of light from the irradiated companion. We calculated amplitude spectra, identified significant pulsation frequencies, and searched for multiplets and asymptotic period spacings. By means of multiplets and period spacing, we identified the degrees of several pulsation modes in each star. The g-mode multiplets indicate subsynchronous core rotation with periods of 4.6 d (PHL 457) and 9.4 d (EQ Psc). We made spectral energy disctribution (SED) fits of PHL 457 and EQ Psc using available broad-band photometry and Gaia data. While the SED of PHL 457 shows no evidence of a cool companion, the SED for EQPsc clearly shows an infrared (IR) access consistent with a secondary with a temperature of about 6800K and a radius of 0.23 R-circle dot. This is the first detection of an IR access in any sdB + dM binary.
“A chain is only as strong as its weakest link” says the proverb. But what about a collection of statistically identical chains: How long till all chains fail? The answer to this question is given by the max-min of a matrix whose (i,j)entry is the failure time of link j of chain i: take the minimum of each row, and then the maximum of the rows' minima. The corresponding min-max is obtained by taking the maximum of each column, and then the minimum of the columns' maxima. The min-max applies to the storage of critical data. Indeed, consider multiple backup copies of a set of critical data items, and consider the (i,j) matrix entry to be the time at which item j on copy i is lost; then, the min-max is the time at which the first critical data item is lost. In this paper we address random matrices whose entries are independent and identically distributed random variables. We establish Poisson-process limit laws for the row's minima and for the columns' maxima. Then, we further establish Gumbel limit laws for the max-min and for the min-max. The limit laws hold whenever the entries' distribution has a density, and yield highly applicable approximation tools and design tools for the max-min and min-max of large random matrices. A brief of the results presented herein is given in: Gumbel central limit theorem for max-min and min-max