Suchergebnisse

The external quantum efficiency of perovskite light-emitting diodes (PeLEDs) has advanced quickly during the past few years. However, under pulsed operation, an operation mode which is important for display and visible light communication, the performance of PeLEDs changes a lot and requires in-depth understanding to facilitate these applications. Here, we report the response of PeLEDs under pulsed operation in the range of 10 Hz to 20 kHz. Beyond transient effects in the low frequencies, we find that for higher frequencies (>500 Hz) the transient electroluminescence intensity depends strongly on the duty cycle. This feature is much more pronounced and of different origin than that in conventional LEDs. We rationalise our experimental observations using a mathematical model and assign these features to the effect of mobile ionic charges in the perovskite. Our work also provides important implications for the operation of PeLEDs under the steady state, where accumulation of mobile ions at the interfaces could be beneficial for high electroluminescence yields but harmful for the long-term stability. ; Funding: ERC Starting Grants [717026, 851676]; Swedish Energy Agency EnergimyndighetenSwedish Energy Agency [48758-1]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009-00971]

Chemical state analysis in X-ray photoelectron spectroscopy (XPS) relies on assigning well-defined binding energy values to core level electrons originating from atoms in particular bonding configurations. Here, we present direct evidence for the violation of this paradigm. It is shown that the C 1s peak due to C-C/C-H bonded atoms from adventitious carbon (AdC) layers accumulating on Al and Au foils splits into two distinctly different contributions, as a result of vacuum level alignment at the AdC/foil interface. The phenomenon is observed while simultaneously recording the spectrum from two metal foils in electric contact with each other. This finding exposes fundamental problems with the reliability of reported XPS data as C 1s peak of AdC is routinely used for binding energy scale referencing. The use of adventitious carbon in XPS should thus be discontinued as it leads to nonsense results. Consequently, ISO and ASTM charge referencing guides need to be rewritten. ; Funding Agencies|Knut and Alice Wallenberg FoundationKnut & Alice Wallenberg Foundation [KAW2016.0358]; Swedish Research Council VR Grant [2018-03957]; Swedish Energy AgencySwedish Energy Agency [51201-1]; VINNOVAVinnova [2019-04882]; Carl Tryggers Stiftelse [CTS 17:166, CTS 15:219, CTS 14:431]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009-00971]

The evolution of the electronic structure and optical transition upon n-doping of poly(9,9-dioctylfluorene) (PFO) films is elucidated with photoelectron spectroscopy, optical absorption, density functional theory (DFT), and time-dependent DFT (TD-DFT) calculations. Optical absorption measurements extending into near infrared show two low-energy absorption features at low doping ratios and an additional peak at a higher energy of similar to 2.2 eV that disappears with increasing doping ratios. A gap state (i.e., polaronic state) close to the Fermi level and a significantly destabilized highest valence band appear in the experimentally measured ultraviolet photoelectron spectra. These experimental results are interpreted by the TD-DFT calculations, which show that the lower energy peaks originate from the excitation from polaronic states to the conduction band, while the higher energy peak mainly originates from the destabilized valence band to conduction band transitions and only appears at low doping ratios (c(red) <= 50%, 0.5 potassium atom per fluorene monomer). The DFT calculations further indicate that polaron pairs rather than bipolarons are preferentially formed at high doping ratios. Comparing the results of doped glassy and beta-phase films, we find that the ordered segments in the beta-phase film disappear due to the dopant (potassium) insertion, resulting in a similar polaronic structure. ; Funding Agencies|Knut and Alice Wallenberg Foundation project "Tail of the Sun"; Swedish Foundation for Strategic ResearchSwedish Foundation for Strategic Research [SE13-0060]; Swedish Research CouncilSwedish Research CouncilEuropean Commission [2016-05498, 2016-05990]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009 00971]

One of the most critical challenges in perovskite light-emitting diodes (PeLEDs) lies in poor operational stability. Although field dependent ion migration is believed to play an important role in the operation of perovskite optoelectronic devices, a complete understanding of how it affects the stability of PeLEDs is still missing. Here, we report a unique self-repairing behavior that the electroluminescence of moderately degraded PeLEDs can almost completely restore to their initial performance after resting. We find that the accumulated halides within the hole transport layer undergo back diffusion toward the surface of the perovskite layer during resting, repairing the vacancies and thus resulting in electroluminescence recovery. These findings indicate that one of the dominant degradation pathways in PeLEDs is the generation of halide vacancies at perovskite/hole transport layer interface during operation. We thus further passivate this key interface, which results in a high external quantum efficiency of 22.8% and obviously improved operational stability. ; Funding Agencies|ERCEuropean Research Council (ERC)European Commission [717026]; Swedish Energy Agency EnergimyndighetenSwedish Energy Agency [48758-1]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009-00971]; DFGGerman Research Foundation (DFG)European Commission [SPP 2196, 424216076]; China Scholarship CouncilChina Scholarship Council [201906830040]; Nanjing University of Aeronautics and Astronautics PhD short-term visiting scholar project [180608DF06]; Priority Academic Program Development of Jiangsu Higher Education Institutions; Swiss Federal Office of Energy (SFOE)-BFE [SI/501805-01]

The high-pressure synthesis of rhenium nitride pernitride with a crystal structure that is unusual for transition metal dinitrides and high values of hardness and bulk modulus attracted significant attention to this system. We investigate the thermodynamic and electronic properties of the P2(1)/c phase of ReN2 and compare them with two other polytypes, the C2/m and P4/mbm phases, suggested in the literature. Our calculations of the formation enthalpy at zero temperature show that the former phase is the most stable of the three up to a pressure p = 170 GPa, followed by the stabilization of the P4/mbm phase at higher pressure. The theoretical prediction is confirmed by diamond anvil cell synthesis of the P4/mbm ReN2 at approximate to 175 GPa. Considering the effects of finite temperature in the quasiharmonic approximation at p = 100 GPa we demonstrate that the P2(1)/c phase has the lowest free energy of formation at least up to 1000 K. Our analysis of the pressure dependence of the electronic structure of rhenium nitride pernitride shows the presence of two electronic topological transitions around 18 GPa, when the Fermi surface changes its topology due to the appearance of an electron pocket at the high-symmetry Y-2 point of the Brillouin zone while the disruption of the neck takes place slightly off from the Gamma-A line. ; Funding Agencies|Knut and Alice Wallenberg Foundation (Wallenberg Scholar Grant) [KAW-2018.0194]; Swedish Government Strategic Research Areas in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009 00971]; SeRC, the Swedish Research Council (VR) [2019-05600]; VINN Excellence Center Functional Nanoscale Materials (FunMat-2) [201605156]; Russian Science FoundationRussian Science Foundation (RSF) [18-12-00492]; Swedish Research CouncilSwedish Research CouncilEuropean Commission [2016-07213]

We theoretically study helicity-dependent photocurrent in a three-dimensional topological insulator Bi2Te3 under elastic scattering of different symmetries. By exploring spin-selective optical transitions and symmetry-breaking scattering, we are able to address the out-of-plane spin texture of the topological helical surface states and to generate directional, spin-polarization tunable photocurrent that is otherwise forbidden for the original C-3v symmetry of the surface. This can be achieved regardless of the Fermi level, even under the condition when the topological states are inaccessible in dark. This work paves the way to robustly explore the out-of-plane spin texture for harvesting opto-spintronic functionalities of topological insulators. ; Funding Agencies|Linkoping University; Swedish Research CouncilSwedish Research Council [2016-05091]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009-00971]

We show by electron spin resonance (ESR) and Raman spectroscopies that the crystal phase transition of the lead-free double-perovskite Cs2AgBiBr6 has a profound symmetry-breaking effect on the high spin states of, for example, a transition-metal ion Fe3+ and the vibrational modes. It lifts their degeneracy when the crystal undergoes the cubic-tetragonal phase transition, splitting the six-fold degenerate S = 5/2 state of Fe3+ to three Kramer doublets and the enharmonic breathing mode T-g of the MBr6 octahedra (M = Ag, Bi, Fe) into E-g + A(g). The magnitudes of both spin and Raman line splitting are shown to directly correlate with the strength of the tetragonal strain field. This work, in turn, demonstrates the power of the ESR and Raman spectroscopies in probing structural phase transitions and in providing in-depth information on the interplay between the structural, spin, and vibrational properties of lead-free double perovskites, a newly emerging and promising class of materials for low-cost and high-efficiency photovoltaics and optoelectronics. ; Funding Agencies|Swedish Research CouncilSwedish Research Council [VR-2017-05285]; Linkoping University; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009 00971]; Knut and Alice Wallenberg FoundationKnut & Alice Wallenberg Foundation [KAW 2019.0082]

Black phase CsPbI3 is attractive for optoelectronic devices, while usually it has a high formation energy and requires an annealing temperature of above 300 degrees C. The formation energy can be significantly reduced by adding HI in the precursor. However, the resulting films are not suitable for light-emitting applications due to the high trap densities and low photoluminescence quantum efficiencies, and the low temperature formation mechanism is not well understood yet. Here, we demonstrate a general approach for deposition of gamma -CsPbI3 films at 100 degrees C with high photoluminescence quantum efficiencies by adding organic ammonium cations, and the resulting light-emitting diode exhibits an external quantum efficiency of 10.4% with suppressed efficiency roll-off. We reveal that the low-temperature crystallization process is due to the formation of low-dimensional intermediate states, and followed by interionic exchange. This work provides perspectives to tune phase transition pathway at low temperature for CsPbI3 device applications. Exploiting low-temperature formed black phase CsPbI3 for light-emitting applications remains a challenge. Here, the authors propose a method to enable the deposition of gamma -CsPbI3 films at 100C and demonstrate a light-emitting diode with an external quantum efficiency of 10.4% with suppressed efficiency roll-off. ; Funding Agencies|Major Research Plan of the National Natural Science Foundation of ChinaNational Natural Science Foundation of China (NSFC) [91733302]; National Natural Science Foundation of ChinaNational Natural Science Foundation of China (NSFC) [51703094, 61935017, 61974066]; Natural Science Foundation of Jiangsu Province, ChinaNatural Science Foundation of Jiangsu Province [BK20170991]; National Science Fund for Distinguished Young ScholarsNational Natural Science Foundation of China (NSFC)National Science Fund for Distinguished Young Scholars [61725502]; Major Program of Natural Science Research of Jiangsu Higher Education Institutions of China [18KJA510002]; National Key Research and Development Program of China [2018YFB0406704]; Natural Science Fund for Colleges and Universities in Jiangsu Province of China [17KJB150023]; ERC Starting GrantEuropean Research Council (ERC) [717026]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009-00971]; Marie Skodowska-Curie [798861]; Linkoping University

Thermal conductivity of AlxGa1-xN layers with 0 <= x <= 0.96 and variable thicknesses is systematically studied by combined thermoreflectance measurements and a modified Callaway model. We find a reduction in the thermal conductivity of AlxGa1-xN by more than one order of magnitude compared to that of GaN, which indicates a strong effect of phonon-alloy scattering. It is shown that the short-mean free path phonons are strongly scattered, which leads to a major contribution of the long-mean free path phonons to the thermal conductivity. In thin layers, the long-mean free path phonons become efficiently scattered by the boundaries, resulting in a further decrease in the thermal conductivity. Also, an asymmetry of thermal conductivity as a function of Al content is experimentally observed and attributed to the mass difference between Ga and Al host atoms. ; Funding Agencies|Swedish Governmental Agency for innovation systems (VINOVA) under Competence Center Program [2016-05190]; Swedish Research Council VRSwedish Research Council [2016-00889, 2017-03714]; Swedish Foundation for Strategic ResearchSwedish Foundation for Strategic Research [RIF14-055, EM16-0024]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University, Faculty Grant SFO Mat LiU [2009-00971]; NSFNational Science Foundation (NSF) [CBET-1336464, DMR-1506159]

Investigating magnetic materials at realistic conditions with first-principles methods is a challenging task due to the interplay of vibrational and magnetic degrees of freedom. The most difficult contribution to include in simulations is represented by the longitudinal magnetic degrees of freedom [longitudinal spin fluctuation (LSF)] due to their inherent many-body nature; nonetheless, schemes that enable to take into account this effect on a semiclassical level have been proposed and employed in the investigation of magnetic systems. However, assessment of the effect of vibrations on LSF is lacking in the literature. For this reason, in this work we develop a supercell approach within the framework of constrained density functional theory to calculate self-consistently the size of local-environment-dependent magnetic moments in the paramagnetic, high-temperature state in the presence of lattice vibrations and for liquid Fe in different conditions. First, we consider the case of bcc Fe at the Curie temperature and ambient pressure. Then, we perform a similar analysis on bcc Fe at Earths inner-core conditions, and we find that LSFs stabilize nonzero moments which affect atomic forces and the electronic density of states of the system. Finally, we employ the present scheme on liquid Fe at the melting point at ambient pressure and at Earths outer-core conditions (p approximate to 200 GPa, T approximate to 6000 K). In both cases, we obtain local magnetic moments of sizes comparable to the solid-state counterparts. ; Funding Agencies|Swedish Research Council (VR) through International Career GrantSwedish Research Council [2014-6336, 2019-05403]; Marie Sklodowska Curie Actions [INCA 600398]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009 00971]; Knut and Alice Wallenberg Foundation (Wallenberg Scholar Grant) [KAW-2018.0194]; Swedish Foundation for Strategic Research through the Future Research Leaders 6 program [FFL 15-0290]

We study the origin of layer decoupling in ordered multilayer graphene grown by high temperature sublimation on C-face 4H-SiC. The mid-infrared optical Hall effect technique is used to determine the magnetic field dependence of the inter-Landau level transition energies and their optical polarization selection rules, which unambiguously show that the multilayer graphene consists of electronically decoupled layers. Transmission electron microscopy reveals no out-of-plane rotational disorder between layers in the stack, which is in contrast to what is typically observed for C-face graphene grown by low temperature sublimation. It is found that the multilayer graphene maintains AB-stacking order with increased interlayer spacing by 2.4%-8.4% as compared to highly oriented pyrolytic graphite. Electron energy loss spectroscopy mapping reveals Si atoms trapped in between layers, which are proposed to be the cause for the observed increased interlayer spacing leading to layer decoupling. Based on our results, we propose a defect-driven growth evolution mechanism for multilayer graphene on C-face SiC via high temperature sublimation. ; Funding Agencies|Swedish Research Council VRSwedish Research Council [2016-00889]; Swedish Foundation for Strategic ResearchSwedish Foundation for Strategic Research [FL12-0181, RIF 14-0074, RIF14-055]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [SFO Mat LiU 2009-00971]

We employ a first-principles cluster-expansion method in combination with canonical Monte Carlo simulations to study the effect of spin-orbit coupling on the alloying behavior of multilayer Bi1-xSbx. Our simulations reveal that spin-orbit coupling plays an essential role in determining the configurational thermodynamics of Bi and Sb atoms. Without the presence of spin-orbit coupling, Bi1-xSbx is predicted to exhibit at low-temperature chemical ordering of Bi and Sb atoms, leading to formation of an ordered structure at x approximate to 0.5. Interestingly, the spin-orbit-coupling effect intrinsically induced by the existence of Bi and Sb results in the disappearance of chemical ordering of the constituent elements within an immiscible region existing at T < 370 K, and consequently Bi1-xSbx displays merely a tendency toward local segregation of Bi and Sb atoms, resulting in coexistence of Bi-rich and Sb-rich Bi1-xSbx solid solutions without the formation of any ordered structure of Bi1-xSbx as predicted in the absence of spin-orbit coupling. These findings distinctly highlight an influence of spin-orbit coupling on the alloying behavior of Bi1-xSbx and probably other alloys composed of heavy elements, where the spin-orbit-coupling effect is supposed to be robust. ; Funding Agencies|Chulalongkorn UniversityChulalongkorn University [CUGR_62_66_23_26]; Thailand Toray Science Foundation (TTSF); Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009 00971]; Swedish Foundation for Strategic Research through the Future Research Leaders 6 program [FFL 15-0290]; Swedish Research Council (VR)Swedish Research Council [2019-05403]; Knut and Alice Wallenberg Foundation (Wallenberg Scholar Grant) [KAW-2018.0194]

The record high photoinduced current and power conversion efficiencies of organic solar cells (OSCs) should be attributed to the significant contribution of non-fullerene electron acceptors via hole transfer to electron donors and/or a pronounced decrease in energy losses for exciton dissociation by aligned highest occupied molecular orbitals (HOMOs) or lowest unoccupied molecular orbitals (LUMOs). However, the hole transfer mechanism in those highly efficient non-fullerene OSCs with small HOMO offsets has not been extensively studied and fully understood, yet. Herein, we comparatively study the hole transfer kinetics in two OSCs with a positive (0.05 eV) and a negative (-0.07 eV) HOMO offset (Delta HOMO) based on polymer donor PTQ10 paired with non-fullerene acceptors ZITI-C or ZITI-N. Short-circuit current densities (J(sc)) of 20.42 and 12.81 mA cm(-2) are achieved in the OSCs based on PTQ10:ZITI-C (Delta HOMO = 0.05 eV) and PTQ10:ZITI-N (Delta HOMO = -0.07 eV) with an optimized donor (D):acceptor (A) ratio of 1:1, respectively, despite the small and even negative Delta HOMO. Results from time-resolved transient absorption spectroscopy show slower hole transfer (14.3 ps) in PTQ10:ZITI-N than that (3.7 ps) in PTQ10:ZITI-C. To understand the decent J(sc) value in the OSCs of PTQ10:ZITI-N, the temperature and electric field dependences of hole transfer are investigated in low-donor-content OSCs (D:A ratio of 1:9) in which photocurrent is dominated by the contribution via hole transfer from ZITI-N to PTQ10. Devices based on PTQ10:ZITI-C and PTQ10:ZITI-N show similar free charge generation behavior as a function of temperature, whereas the external quantum efficiencies of the PTQ10:ZITI-N device exhibit a much stronger bias dependence than that of PTQ10:ZITI-C, which suggests that the electric field facilitates exciton dissociation in PTQ10:ZITI-N where the energetic driving force alone cannot efficiently dissociate excitons. ; Funding Agencies|Swedish Government Strategic Research Area in Material Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU ) [200900971]; Swedish Research CouncilSwedish Research Council [2017-04123]; Knut and Alice Wallenberg FoundationKnut & Alice Wallenberg Foundation [2016.0059]; China Scholarship Council (CSC)China Scholarship Council; National Key R&D Program of China [2019YFA0705900, 2017YFA0204701]; National Natural Science Foundation of ChinaNational Natural Science Foundation of China [21572234, 21661132006, 91833304]

Ytterligare forskningsfinansiärer: Knut and Alice WallenbergFoundation for a Fellowship Grant and Project funding (KAW 2015.0043), Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University (Faculty Grant SFO MatLiUNo. 2009 00971), Swedish Research Council VR-RFI (#2017-00646_9), Swedish Foundation for Strategic Research(contract RIF14-0053)

We report on optimization of growth conditions of GaAs/GaNAs/GaAs core/shell/shell nanowire (NW) structures emitting at ~1 μm, aiming to increase their light emitting efficiency. A slight change in growth temperature is found to critically affect optical quality of the active GaNAs shell and is shown to result from suppressed formation of non-radiative recombination (NRR) centers under the optimum growth temperature. By employing the optically detected magnetic resonance spectroscopy, we identify gallium vacancies and gallium interstitials as being among the dominant NRR defects. The radiative efficiency of the NWs can be further improved by post-growth annealing at 680 °C, which removes the gallium interstitials. ; Funding agencies: Swedish Energy AgencySwedish Energy Agency [P40119-1]; Swedish Research CouncilSwedish Research Council [2015-05532]; Swedish Foundation for International Cooperation in Research and Higher Education (STINT) [JA2014-5698]; Swedish Government Strategic Res