The organic-inorganic hybrid lead trihalide perovskites have been emerging as the most attractive photovoltaic materials. As regulated by Shockley-Queisser theory, a formidable materials science challenge for improvement to the next level requires further band-gap narrowing for broader absorption in solar spectrum, while retaining or even synergistically prolonging the carrier lifetime, a critical factor responsible for attaining the near-band-gap photovoltage. Herein, by applying controllable hydrostatic pressure, we have achieved unprecedented simultaneous enhancement in both band-gap narrowing and carrier-lifetime prolongation (up to 70% to ∼100% increase) under mild pressures at ∼0.3 GPa. The pressure-induced modulation on pure hybrid perovskites without introducing any adverse chemical or thermal effect clearly demonstrates the importance of band edges on the photon-electron interaction and maps a pioneering route toward a further increase in their photovoltaic performance. . The remarkable photovoltaic performance is attributed to its strong and broad (up to ∼800 nm) light absorption (10), as well as the long diffusion lengths facilitated by its extraordinarily long carrier lifetimes (∼100 ns in thin film) despite its modest mobility (11,12,15,16). To further approach the Shockley-Queisser limit (17, 18), it is highly desirable to tune the crystal structure of perovskite in the way that can synergistically narrow down the band gap for broader solar spectrum absorption (10) and prolong carrier lifetime for greater photovoltage (7,11,12,15,16). However, compositional modification suffers from challenges, such as the largely shortened carrier lifetime (∼50 ps), and thus considerable loss of photovoltage upon the replacement of Pb by Sn (5, 19), or the largely widened band gap, and thus low photocurrent when I is substituted with Br or Cl (16). It also has been demonstrated that using formamidinium (FA) cations instead of MA cations in organic-inorganic perovskite materials narrows down the band gap; however, a shorter carrier lifetime is generated inevitably (20). In fact, to date, there is no reported method for simultaneously achieving band-gap narrowing and carrier-lifetime prolongation for MAPbI 3 .Nonetheless, the chance is to rescrutinize the band structure of MAPbI 3 . The relatively long carrier lifetimes of 10 2 to ∼10 3 ns observed in MAPbI 3 single crystals originate from their unique defect physics (21). First-principles calculations demonstrated that the readily formed point defects such as interstitial MA ions and/or Pb vacancies create shallow states with trap energy less than 0.05 eV below the conduction band minimum (CBM), or above the valence band maximum (VBM), rather than detrimental deep traps at the middle of the forbidden zone, which typically lead to nonradiative recombination (21). The uneven distribution of the trap states has been identified further by in-depth electronic characterization of MAPbI 3 perovskite single crystals, concluding that the traps are close to the conduction an...
The high water storage capacity of minerals in Earth's mantle transition zone (410- to 660-kilometer depth) implies the possibility of a deep H2O reservoir, which could cause dehydration melting of vertically flowing mantle. We examined the effects of downwelling from the transition zone into the lower mantle with high-pressure laboratory experiments, numerical modeling, and seismic P-to-S conversions recorded by a dense seismic array in North America. In experiments, the transition of hydrous ringwoodite to perovskite and (Mg,Fe)O produces intergranular melt. Detections of abrupt decreases in seismic velocity where downwelling mantle is inferred are consistent with partial melt below 660 kilometers. These results suggest hydration of a large region of the transition zone and that dehydration melting may act to trap H2O in the transition zone.
Nature 457, 863-867 (2009) This Letter presents the results of high-pressure experiments and ab initio evolutionary crystal structure predictions, and found a new boron phase that we named c-B 28 . This phase is comprised of icosahedral B 12 clusters and B 2 pairs in a NaCl-type arrangement, stable between 19 and 89 GPa, and exhibits evidence for charge transfer (for which our best estimate is d < 0.48) between the constituent clusters to give (B 2 ) d1 (B 12 ) d2 . We have recently found that the same highpressure boron phase may have given rise to the Bragg reflections reported by Wentorf in 1965 (ref. 1), although the chemical composition was not analysed and the data (subsequently deleted from the Powder Diffraction File database) seems to not have been used to propose a structure model. We also note that although we used the terms 'partially ionic' and 'ionic' to emphasize the polar nature of the high-pressure boron phase and the influence this polarity has on several physical properties of the elemental phase, the chemical bonding in c-B 28 is predominantly covalent.We acknowledge N. Dubrovinskaia, L. Dubrovinsky, E. Yu Zarechnaya, Y. Filinchuk, D. Chernyshov, V. Dmitriev, A. S. Mikhaylushkin, I. A. Abrikosov & S. I. Simak for drawing these issues to our attention.
Bond length and bond angle exhibited by valence electrons is essential to the core of chemistry. Using lead‐based organic–inorganic perovskite compounds as an exploratory platform, it is demonstrated that the modulation of valence electrons by compression can lead to discovery of new properties of known compounds. Yet, despite its unprecedented progress, further efficiency boost of lead‐based organic–inorganic perovskite solar cells is hampered by their wider bandgap than the optimum value according to the Shockley–Queisser limit. By modulating the valence electron wavefunction with modest hydraulic pressure up to 2.1 GPa, the optimized bandgap for single‐junction solar cells in lead‐based perovskites, for the first time, is achieved by narrowing the bandgap of formamidinium lead triiodide (HC(NH2)2PbI3) from 1.489 to 1.337 eV. Strikingly, such bandgap narrowing is partially retained after the release of pressure to ambient, and the bandgap narrowing is also accompanied with double‐prolonged carrier lifetime. With First‐principles simulation, this work opens a new dimension in basic chemical understanding of structural photonics and electronics and paves an alternative pathway toward better photovoltaic materials‐by‐design.
N6-methyladenosine (m6A) epitranscriptional modification has recently gained much attention. Through the development of m6A sequencing, the molecular mechanism and importance of m6A have been revealed. m6A is the most abundant internal modification in higher eukaryotic mRNAs, which plays crucial roles in mRNA metabolism and multiple biological processes. In this review, we introduce the characteristics of m6A regulators, including “writers” that create m6A mark, “erasers” that show demethylation activity and “readers” that decode m6A modification to govern the fate of modified transcripts. Moreover, we highlight the roles of m6A modification in several common cancers, including solid and non-solid tumors. The regulators of m6A exert enormous functions in cancer development, such as proliferation, migration and invasion. Especially, with the underlying mechanisms being uncovered, m6A and its regulators are expected to be the targets for the diagnosis and treatment of cancers.
Optical spectroscopy techniques, including visible and near infrared (IR) Raman and synchrotron IR methods have been applied to study solid nitrogen at megabar pressures. We find that nitrogen becomes totally opaque above 150 GPa, accompanied by the disappearance of Raman and IR vibrational excitations, while new broad IR and Raman bands become visible. Optical absorption measurements reveal that the semiconducting absorption edge responsible for the change of color is characterized by the presence of a wide Urbach-like tail and a high-energy (Tauc) region. These data are consistent with the dissociation of molecular nitrogen into a nonmolecular (possibly amorphous) phase.
Diamond-anvil-cell techniques have been developed to confine and measure hydrogen samples under static conditions to pressures above 300 GPa from 12 to 300 K using synchrotron infrared and optical absorption techniques. A decreasing absorption threshold in the visible spectrum is observed, but the material remains transparent at photon energies down to 0.1 eV at pressures to 360 GPa over a broad temperature range. The persistence of the strong infrared absorption of the vibron characteristic of phase III indicates the stability of the paired state of hydrogen. There is no evidence for the predicted metallic state over these conditions, in contrast to recent reports, but electronic properties consistent with semimetallic behavior are observed.
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