The light instability of CH3NH3PbIxBr3–x is one of the biggest challenges for its application in tandem solar cells. Here we show that an improved crystallinity and grain size of CH3NH3PbIxBr3–x films could stabilize these materials under one sun illumination, improving both the efficiency and stability of the wide‐bandgap perovskite solar cells.
The kagome lattice1, which is the most prominent structural motif in quantum physics, benefits from inherent non-trivial geometry so that it can host diverse quantum phases, ranging from spin-liquid phases, to topological matter, to intertwined orders2, 3,4,5,6,7,8 and, most rarely, to unconventional su-perconductivity6,9. Recently, charge sensitive probes have indicated that the kagome superconductors AV3Sb5 (A = K, Rb, Cs)9,10,11 exhibit unconventional chiral charge order12, 13,14,15,16,17,18,19, which is analogous to the long-sought-after quantum order in the Haldane model20 or Varma model21. However, direct evidence for the time-reversal symmetry breaking of the charge order remains elusive. Here we use muon spin relaxation to probe the kagome charge order and superconductivity in KV3Sb5. We observe a noticeable enhancement of the internal field width sensed by the muon ensemble, which takes place just below the charge ordering temperature and persists into the superconducting state. Notably, the muon spin relaxation rate below the charge ordering temperature is substantially enhanced by applying an external magnetic field. We further show the multigap nature of superconductivity in KV3Sb5 and that the Tc/−2ab ratio (where Tc is the superconducting transition temperature and ab is the magnetic penetration depth in the kagome plane) is comparable to those of unconventional high-temperature superconductors. Our results point to time-reversal symmetry-breaking charge order intertwining with unconventional superconductivity in the correlated kagome lattice.
Hybrid organic-inorganic perovskites based on methylammonium lead (MAPbI) are an emerging material with great potential for high-performance and low-cost photovoltaics. However, for perovskites to become a competitive and reliable solar cell technology their instability and spatial variation must be understood and controlled. While the macroscopic characterization of the devices as a function of time is very informative, a nanoscale identification of their real-time local optoelectronic response is still missing. Here, we implement a four-dimensional imaging method through illuminated heterodyne Kelvin probe force microscopy to spatially (<50 nm) and temporally (16 s/scan) resolve the voltage of perovskite solar cells in a low relative humidity environment. Local open-circuit voltage (V) images show nanoscale sites with voltage variation >300 mV under 1-sun illumination. Surprisingly, regions of voltage that relax in seconds and after several minutes consistently coexist. Time-dependent changes of the local V are likely due to intragrain ion migration and are reversible at low injection level. These results show for the first time the real-time transient behavior of the V in perovskite solar cells at the nanoscale. Understanding and controlling the light-induced electrical changes that affect device performance are critical to the further development of stable perovskite-based solar technologies.
The combination of non-trivial band topology and symmetry breaking phases gives rise to novel quantum states and phenomena such as topological superconductivity, quantum anomalous Hall effect and axion electrodynamics. Evidence of intertwined charge density wave (CDW) and superconducting order parameters has recently been observed in a novel kagome material AV3Sb5 (A=K,Rb,Cs) that features a Z2 topological invariant in the electronic structure. However, the origin of the CDW and its intricate interplay with topological state has yet to be determined. Here, using hard x-ray scattering, we demonstrate a three-dimensional (3D) CDW with 2 × 2 × 2 superstructure in (Rb,Cs)V3Sb5. Unexpectedly, we find that the CDW fails to induce acoustic phonon anomalies at the CDW wavevector but yields a novel Raman mode that quickly damps into a broad continuum below the CDW transition temperature. Our observations exclude strong electron-phonon coupling driven CDW in AV3Sb5 and point to an unconventional particle-hole condensation mechanism that couples CDW, superconductivity and topological band structure.
Although all superconducting cuprates display charge-ordering tendencies, their low-temperature properties are distinct, impeding efforts to understand the phenomena within a single conceptual framework. While some systems exhibit stripes of charge and spin, with a locked periodicity, others host charge density waves (CDWs) without any obviously related spin order. Here we use resonant inelastic x-ray scattering (RIXS) to follow the evolution of charge correlations in the canonical stripe ordered cuprate La 1.875 Ba 0.125 CuO 4 (LBCO 1/8) across its ordering transition. We find that hightemperature charge correlations are unlocked from the wavevector of the spin correlations, signaling analogies to CDW phases in various other cuprates. This indicates that stripe order at low temperatures is stabilized by the coupling of otherwise independent charge and spin density waves, with important implications for the relation between charge and spin correlations in the cuprates.Charge density waves | Stripes | Superconductivity | Cuprates W hen holes are doped into the Mott insulating parent compounds of the cuprates, multiple competing interactions conspire to form a rich phase diagram. In the underdoped regime, holes can save energy by clustering together on neighboring sites in order to minimize the number of broken magnetic bonds, but by doing so they pay an extra energy cost of the increased inter-site Coulomb repulsion and reduced kinetic energy. Several early theoretical works suggested that frustration between these different ordering tendencies generates an instability towards spin density wave (SDW) order (1-5) and low-energy incommensurate SDW correlations were indeed observed around the same time (6-8). Such considerations were key to the discovery of "stripes" in the La2−x−y(Nd/Eu)y(Sr/Ba)xCuO4 or 214 family of cuprates. These correlations were found to be strongest at a doping level of 1/8 for which static spin and charge order forms at wavevectors related by a factor of two (9, 10). This phase was often conceptualized in terms of a dominant spin degree of freedom, as the underdoped cuprates have a large magnetic energy scale and a relatively small electronic density of states at the Fermi level (1-5). Furthermore, although high-temperature spin correlations were easily seen (7,8,10), directly detecting high-temperature charge correlations proved beyond the sensitivity of standard x-ray and neutron scattering measurements. Most compellingly, charge and spin ordering appeared, until recently, to be absent in cuprates in which there was a low-energy spin gap such as YBa2Cu3O6+x (YBCO), Bi1.5Pb0.5Sr1.54CaCu2O 8+δ (BSCCO2212), and HgBa2CuO 4+δ (HBCO1201), so the discovery of CDW correlations in these systems generated great interest (11)(12)(13)(14)(15)(16)(17)(18)(19). While the similarity of CDW phase diagrams in these materials may indicate a unified CDW mechanism (20, 21), many of the CDW properties reported in these materials were, however, notably different than that in LBCO 1/8. The CDW incommensurability...
While charge density wave (CDW) instabilities are ubiquitous to superconducting cuprates, the different ordering wavevectors in various cuprate families have hampered a unified description of the CDW formation mechanism. Here we investigate the temperature dependence of the low energy phonons in the canonical CDW ordered cuprate La1.875Ba0.125CuO4. We discover that the phonon softening wavevector associated with CDW correlations becomes temperature dependent in the hightemperature precursor phase and changes from a wavevector of 0.238 reciprocal space units (r.l.u.) below the ordering transition temperature up to 0.3 r.l.u. at 300 K. This high-temperature behavior shows that "214"-type cuprates can host CDW correlations at a similar wavevector to previously reported CDW correlations in non-"214"-type cuprates such as YBa2Cu3O 6+δ . This indicates that cuprate CDWs may arise from the same underlying instability despite their apparently different low temperature ordering wavevectors. arXiv:1712.04554v2 [cond-mat.supr-con]
Organolead trihalide perovskites (OTPs) are arising as a new generation of low-cost active materials for solar cells with efficiency rocketing from 3.5% to over 20% within only five years. From "dye" in dye sensitized solar cells to "hole conductors" and "electron conductors" in mesoscopic heterojunction solar cells, there has been a dramatic conceptual evolution on the function of OTPs in photovoltaic devices. OTPs were originally used as dyes in Grätzel cells, achieving a high efficiency above 15% which, however, did not manifest the excellent charge transport properties of OTPs. An analogy of OTPs to traditional semiconductors was drawn after the demonstration of highly efficient planar heterojunction structure OTP devices and the observation of their excellent bipolar transport properties with a large diffusion length exceeding 100 nm in CH 3 NH 3 PbI 3 (MAPbI 3) polycrystalline thin films. This review aims to provide the most recent advances in the understanding of the origin of the high OTP device efficiency. Specifically we will focus on reviewing the progress in understanding 1) the characterization of fantastic optoelectronic property of OTPs, 2) the unusual defect physics that originate the optoelectronic property; 3) morphology control of the perovskite film from fabrication process and film post-treatment, and 4) device interface and charge transport layers that dramatically
The nonexcitonic character for organometal trihalide perovskites is demonstrated by examining the field-dependent exciton dissociation behavior. It is found that photogenerated excitons can be effectively dissociated into free charges inside perovskite without the assistance of charge extraction layer or external field, which is a stark contrast to the charge-separation behavior in excitonic materials in the same photovoltaic operation system.
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