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Funding: J.L.P. thanks the University of St Andrews for funding and the Carnegie Trust for a Research Incentive Grant (RIG008653). The authors also thank EPSRC for funding (EP/T019298/1, EP/R023751/1 and EP/V034138/1). L.K.J. thanks UKRI for a Future Leaders Fellowship (MR/T022094/1). One of the great advantages of organic–inorganic metal halides is that their structures and properties are highly tuneable and this is important when optimizing materials for photovoltaics or other optoelectronic devices. One of the most common and effective ways of tuning the electronic structure is through anion substitution. Here, we report the inclusion of bromine into the layered perovskite [H3N(CH2)6NH3]PbBr4 to form [H3N(CH2)6NH3]PbBr4·Br2, which contains molecular bromine (Br2) intercalated between the layers of corner-sharing PbBr6 octahedra. Bromine intercalation in [H3N(CH2)6NH3]PbBr4·Br2 results in a decrease in the band gap of 0.85 eV and induces a structural transition from a Ruddlesden–Popper-like to Dion–Jacobson-like phase, while also changing the conformation of the amine. Electronic structure calculations show that Br2 intercalation is accompanied by the formation of a new band in the electronic structure and a significant decrease in the effective masses of around two orders of magnitude. This is backed up by our resistivity measurements that show that [H3N(CH2)6NH3]PbBr4·Br2 has a resistivity value of one order of magnitude lower than [H3N(CH2)6NH3]PbBr4, suggesting that bromine inclusion significantly increases the mobility and/or carrier concentration in the material. This work highlights the possibility of using molecular inclusion as an alternative tool to tune the electronic properties of layered organic–inorganic perovskites, while also being the first example of molecular bromine inclusion in a layered lead halide perovskite. By using a combination of crystallography and computation, we show that the key to this manipulation of the electronic structure is the formation of halogen bonds between the Br2 and Br in the [PbBr4]∞ layers, which is likely to have important effects in a range of organic–inorganic metal halides. Publisher PDF

E.J.C., O.M., and C.P. acknowledge financial support from the Leverhulme Trust Research Project Grant No. RPG-2017-109. O.M. is grateful for funding via the Leverhulme Trust Early Career Fellowship ECF-2021-170. A.S.G. acknowledges funding through an EPSRC Early Career Fellowship EP/ T011130/1. A.S.G. and H.T. acknowledge funding through the Humboldt Foundation and the Max Planck Institute for Solid State Research. The authors thank the Science and Technology Facilities Council for beamtime allocated at ISIS through proposal RB1990046 (DOI: 10. 5286/ISIS.E.RB1990046) and the Swiss Muon Source at the Paul Scherrer Institute through proposal numbers 20150959 and 20211440. The authors are grateful for access to the MPMS3 instrument at The Royce Discovery Centre at the University of Sheffield (EPSRC grant no. EP/R00661X/1) and the PPMS instrument at the University of St. Andrews (EPSRC grant no. EP/T031441/1). Ba2CuTeO6 has attracted significant attention as it contains a two-leg spin ladder of Cu2+ cations that lies in close proximity to a quantum critical point. Recently, Ba2CuTeO6 has been shown to accommodate chemical substitutions, which can significantly tune its magnetic behavior. Here, we investigate the effects of substitution for non-magnetic Zn2+ impurities at the Cu2+ site, partitioning the spin ladders. Results from bulk thermodynamic and local muon magnetic characterization on the Ba2Cu1 – xZnxTeO6 solid solution (0 ≤ x ≤ 0.6) indicate that Zn2+ partitions the Cu2+ spin ladders into clusters and can be considered using the percolation theory. As the average cluster size decreases with increasing Zn2+ substitution, there is an evolving transition from long-range order to spin-freezing as the critical cluster size is reached between x = 0.1 to x = 0.2, beyond which the behavior became paramagnetic. This demonstrates well-controlled tuning of the magnetic disorder, which is highly topical across a range of low-dimensional Cu2+-based materials. However, in many of these cases, the chemical disorder is also relatively strong in contrast to Ba2CuTeO6 and its derivatives. Therefore, Ba2Cu1 – xZnxTeO6 provides an ideal model system for isolating the effect of defects and segmentation in low-dimensional quantum magnets. Publisher PDF

Funding: We gratefully acknowledge support from the Leverhulme Trust (Grant No. RL-2016-006 [P.D.C.K., B.E., T.A., A.R., C.B.]), the European Research Council (through the QUESTDO project, 714193 [P.D.C.K., G.R.S.]), the Engineering and Physical Sciences Research Council (Grant Nos. EP/T02108X/1 [P.D.C.K., P.A.E.M.] and EP/N032128/1 [D.A.M., G.B.]), and the Center for Computational Materials Science at the Institute for Materials Research for allocations on the MASAMUNE-IMR supercomputer system (Project No. 202112-SCKXX-0510 [R.B.V., M.S.B.]). S.B., E.A.M. and A.Z. gratefully acknowledge studentship support from the International Max-Planck Research School for Chemistry and Physics of Quantum Materials. Research conducted at MAX IV, a Swedish national user facility, is supported by the Swedish Research council under contract 2018-07152, the Swedish Governmental Agency for Innovation Systems under contract 2018-04969, and Formas under contract 2019-02496. The research leading to this result has been supported by the project CALIPSOplus under the Grant Agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020. Spin–valley locking is ubiquitous among transition metal dichalcogenides with local or global inversion asymmetry, in turn stabilizing properties such as Ising superconductivity, and opening routes towards ‘valleytronics’. The underlying valley–spin splitting is set by spin–orbit coupling but can be tuned via the application of external magnetic fields or through proximity coupling. However, only modest changes have been realized to date. Here, we investigate the electronic structure of the V-intercalated transition metal dichalcogenide V1/3NbS2 using microscopic-area spatially resolved and angle-resolved photoemission spectroscopy. Our measurements and corresponding density functional theory calculations reveal that the bulk magnetic order induces a giant valley-selective Ising coupling exceeding 50 meV in the surface NbS2 layer, equivalent to application of a ~250 T magnetic field. This energy scale is of comparable magnitude to the intrinsic spin–orbit splittings, and indicates how coupling of local magnetic moments to itinerant states of a transition metal dichalcogenide monolayer provides a powerful route to controlling their valley–spin splittings. Postprint

Funding: LKJ acknowledges funding from UKRI-FLF through MR/T022094/1. LKJ also acknowledges, Professor Iain Baikie for assistance with the work function and APS measurements, and Professor Phil King and Gordon Kentish, School of Physics and Astronomy, University of St Andrews for the XRD measurements and would like to acknowledge (EPSRC): EP/T023449/1. This research used resources of the Advanced Light Source, a U.S. DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. Work was performed at beamline 12.3.2, beamline scientist Nobumichi Tamura. M. A. acknowledges support by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under Contract No. DE-AC02-05-CH11231 (D2S2 program KCD2S2). Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. IDWS acknowledges funding from EPSRC through EP/l017008/1. Indoor photovoltaics are receiving tremendous attention due to the continuous development of the Internet of Things. The present study reports how the fast processing of the triple halide perovskite enables the retention of chlorine and the beneficial role of chlorine in enhancing the indoor light harvesting of a wide bandgap triple anion (TA) perovskite CH3NH3PbI2.6Br0.2Cl0.2. The kinetics of chlorine incorporation/escape investigated by in situ grazing incidence wide-angle X-ray scattering revealed the escape of chlorine after the first ten minutes of thermal annealing and the findings were corroborated with elemental analysis by wavelength dispersive X-ray spectroscopy. The best-performing TA perovskite indoor-photovoltaic device achieved a steady-state power conversion efficiency (PCE) of 25.1% with an output power density of ∼75 μW cm−2 under 1000 lux indoor illumination (0.3 mW cm−2 irradiance). Improved crystalline quality, reduced density of trap states and longer carrier lifetime were achieved by the triple anion alloying method. The detrimental role of the commonly used hole transporting layer (HTL) of Spiro-MeOTAD under indoor lighting conditions leading to J–V hysteresis was also investigated, which could then be effectively suppressed by replacing Spiro-MeOTAD with undoped P3HT. The optimized TA perovskite indoor PV cells were then successfully used to wirelessly power a textile fiber-based temperature sensor. The results from the present study demonstrate a novel route to incorporate chlorine effectively and maximize the steady state power output from halide perovskite indoor photovoltaic devices and their promising potential for the IoT industry. Publisher PDF

Funding: China Scholarship Council - 2019 06250199, 2020 06250026; Engineering and Physical Sciences Research Council - EP/L017008, EP/P010482/1. Multiresonant thermally activated delayed fluorescence (MR-TADF) compounds are attractive as emitters for organic light-emitting diodes (OLEDs) as they can simultaneously harvest both singlet and triplet excitons to produce light in the device and show very narrow emission spectra, which translates to excellent color purity. Here, we report the first example of an MR-TADF emitter (DOBDiKTa) that fuses together fragments from the two major classes of MR-TADF compounds, those containing boron (DOBNA) and those containing carbonyl groups (DiKTa) as acceptor fragments in the MR-TADF skeleton. The resulting molecular design, this compound shows desirable narrowband pure blue emission and efficient TADF character. The co-host OLED with DOBDiKTa as the emitter showed a maximum external quantum efficiency (EQEmax) of 17.4 %, an efficiency roll-off of 32 % at 100 cd m−2, and Commission Internationale de l’Éclairage (CIE) coordinates of (0.14, 0.12). Compared to DOBNA and DiKTa, DOBDiKTa shows higher device efficiency with reduced efficiency roll-off while maintaining a high color purity, which demonstrates the promise of the proposed molecular design. Publisher PDF

Funding: The authors acknowledge funding support from the Army Research Office, NTT Research, and the QNEXT DOE National Quantum Information Science Research Center. B.M. acknowledges funding from the Q-NEXT DOE National Quantum Information Science Research Center and the NSF Graduate Research Fellowship. Cavity quantum electrodynamics (QED) with cooperativity far greater than unity enables high-fidelity quantum sensing and information processing. The high-cooperativity regime is often reached through the use of short single-mode resonators. More complicated multimode resonators, such as the near-confocal optical Fabry-Prot cavity, can provide intracavity atomic imaging in addition to high cooperativity. This capability has recently proved important for exploring quantum many-body physics in the driven-dissipative setting. In this work, we show that a confocal-cavity–QED microscope can realize cooperativity in excess of 110. This cooperativity is on par with the very best single-mode cavities (which are far shorter) and 21 times greater than single-mode resonators of similar length and mirror radii. The 1.7-μm imaging resolution is naturally identical to the photon-mediated interaction range. We measure these quantities by determining the threshold of cavity superradiance when small optically tweezed Bose-Einstein condensates are pumped at various intracavity locations. Transmission measurements of an ex situ cavity corroborate these results. We provide a theoretical description that shows how cooperativity enhancement arises from the dispersive coupling to the atoms of many near-degenerate modes. Publisher PDF

Funding: Horizon 2020 Framework Programme - 838885; Leverhulme Trust - RPG-2016-047; Engineering and Physical Sciences Research Council - EP/L017008, EP/P010482/1; Fonds de la Recherche Scientifiques de Belgique - 2.5020.11; Walloon Region - n1117545; Fonds De La Recherche Scientifique - FNRS - F.4534.21. Two multiresonant thermally activated delayed fluorescence (MR-TADF) emitters are presented and it is shown how further borylation of a deep-blue MR-TADF emitter, DIDOBNA-N, both blueshifts and narrows the emission producing a new near-UV MR-TADF emitter, MesB-DIDOBNA-N, are shown. DIDOBNA-N emits bright blue light (ΦPL = 444 nm, FWHM = 64 nm, ΦPL = 81%, τd = 23 ms, 1.5 wt% in TSPO1). The deep-blue organic light-emitting diode (OLED) based on this twisted MR-TADF compound shows a very high maximum external quantum efficiency (EQEmax) of 15.3% for a device with CIEy of 0.073. The fused planar MR-TADF emitter, MesB-DIDOBNA-N shows efficient and narrowband near-UV emission (λPL = 402 nm, FWHM = 19 nm, ΦPL = 74.7%, τd = 133 ms, 1.5 wt% in TSPO1). The best OLED with MesB-DIDOBNA-N, doped in a co-host, shows the highest efficiency reported for a near-UV OLED at 16.2%. With a CIEy coordinate of 0.049, this device also shows the bluest EL reported for a MR-TADF OLED to date. Publisher PDF

Quantum information processing is a key technology in the ongoing second quantum revolution, with a wide variety of hardware platforms competing toward its realization. An indispensable component of such hardware is a measurement device, i.e., a quantum detector that is used to determine the outcome of a computation. The act of measurement in quantum mechanics, however, is naturally invasive as the measurement apparatus becomes entangled with the system that it observes. This always leads to a disturbance in the observed system, a phenomenon called quantum measurement backaction, which should solely lead to the collapse of the quantum wave function and the physical realization of the measurement postulate of quantum mechanics. Here we demonstrate that backaction can fundamentally change the quantum system through the detection process. For quantum information processing, this means that the readout alters the system in such a way that a faulty measurement outcome is obtained. Specifically, we report a backaction-induced population switching, where the bare presence of weak, nonprojective measurements by an adjacent charge sensor inverts the electronic charge configuration of a semiconductor double quantum dot system. The transition region grows with measurement strength and is suppressed by temperature, in excellent agreement with our coherent quantum backaction model. Our result exposes backaction channels that appear at the interplay between the detector and the system environments, and opens new avenues for controlling and mitigating backaction effects in future quantum technologies., Physical Review Research, 5 (2), ISSN:2643-1564

We are grateful to EPSRC for equipment and research grants (EP/L017008/1 and EP/R035164/1) and for a Ph.D. studentship to P.E.B. (EP/R513337/1). Dr. L. K. Jagadamma acknowledges support from a Marie Skłodowska-Curie Individual Fellowship (745776) and funding from UKRI-FLF through grant MR/T022094/1. Charge diffusion and extraction are crucial steps in the operation of solar cells. Here we show that time-resolved photoluminescence can be used to study electron diffusion in hybrid perovskite films and subsequent transfer to the adjacent electron extraction layer. As diffusion and transfer to the extraction layer are consecutive processes, they can be hard to distinguish, but by exciting from each side of the sample we can separate them and identify which process limits charge extraction. We find that the introduction of a fullerene monolayer between the methylammonium lead iodide (MAPbI3) and the electron-transporting SnO2 layers greatly increases the electron transfer velocity between them to the extent that electron diffusion limits the rate of electron extraction. Our results suggest that increasing the electron diffusion coefficient in MAPbI3 would further enhance the electron extraction rate, which could result in more efficient n–i–p type solar cells. Publisher PDF

P.H.M. and M.D.B. received PhD studentship support from the UK Engineering and Physical Science Research Council via Grant No. EP/L015110/1. C.P. and P.J.W.M. are supported by the European Research Council under the European Union's Horizon 2020 research and innovation programme (Microstructured Topological Materials Grant No. 715730). E. Z. acknowledges support from the International Max Planck Research School for Chemistry and Physics of Quantum Materials (IMPRS-CPQM). Irradiation experiments performed on the SIRIUS platform were supported by the French National Network of Accelerators for Irradiation and Analysis of Molecules and Materials (EMIR&A) under Project No. EMIR 2019 18-7099. The delafossite metal PtCoO2 is among the highest-purity materials known, with low-temperature mean free path up to 5 μm in the best as-grown single crystals. It exhibits a strongly faceted, nearly hexagonal Fermi surface. This property has profound consequences for nonlocal transport within this material, such as in the classic ballistic-regime measurement of bend resistance in mesoscopic squares. Here, we report the results of experiments in which high-energy electron irradiation was used to introduce pointlike disorder into such squares, reducing the mean free path and therefore the strength of the ballistic-regime transport phenomena. We demonstrate that high-energy electron irradiation is a well-controlled technique to cross from nonlocal to local transport behavior and therefore determine the nature and extent of unconventional transport regimes. Using this technique, we confirm the origins of the directional ballistic effects observed in delafossite metals and demonstrate how the strongly faceted Fermi surface both leads to unconventional transport behavior and enhances the length scale over which such effects are important. © 2023 authors. Published by the American Physical Society. Published by the American Physical Society under the terms of the "https://creativecommons.org/licenses/by/4.0/"Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Open access publication funded by the Max Planck Society. Publisher PDF

We describe an optical method to directly measure position-dependent thermal diffusivity of reflective single crystal samples across a broad range of temperatures for condensed matter physics research. Two laser beams are used, one as a source to locally modulate the sample temperature, and the other as a probe of sample reflectivity, which is a function of the modulated temperature. Thermal diffusivity is obtained from the phase delay between source and probe signals. We combine this technique with a microscope setup in an optical cryostat, in which the sample is placed on a 3-axis piezo-stage, allowing for spatially resolved measurements. Furthermore, we demonstrate experimentally and mathematically that isotropic in-plane diffusivity can be obtained when overlapping the two laser beams instead of separating them in the traditional way, which further enhances the spatial resolution to a micron scale, especially valuable when studying inhomogeneous or multidomain samples. We discuss in detail the experimental conditions under which this technique is valuable, and demonstrate its performance on two stoichiometric bilayer ruthenates: Sr3Ru2O7 and Ca3Ru2O7. The spatial resolution allowed us to study the diffusivity in single domains of the latter, and we uncovered a temperature-dependent in-plane diffusivity anisotropy. Finally, we used the enhanced spatial resolution enabled by overlapping the two beams to measure temperature-dependent diffusivity of Ti-doped Ca3Ru2O7, which exhibits a metal-insulator transition. We observed large variations of transition temperature over the same sample, originating from doping inhomogeneity, and pointing to the power of spatially resolved techniques in accessing inherent properties., 30 pages, 5 figures in the main text, and 5 figures in Appendix

Funding: M. Co. and V. M. A. are grateful for funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under project No. 419036043. A. V. acknowledges the support from the Russian Science Foundation under the Project 18-12-00429. M. Cy. and E. M. G. acknowledge funding from EPSRC grant no. EP/T01377X/1. B.W. L. and J. K. were supported by EPSRC grant no. EP/T014032/1. Studies of the dynamics of open quantum systems are limited by the large Hilbert space of typical environments, which is too large to be treated exactly. In some cases, approximate descriptions of the system are possible, for example when the environment has a short memory time or only interacts weakly with the system. Accurate numerical methods exist but these are typically restricted to baths with Gaussian correlations, such as non-interacting bosons. Here we present a method for simulating open quantum systems with arbitrary environments that consist of a set of independent degrees of freedom. Our approach automatically reduces the large number of environmental degrees of freedom to those which are most relevant. Specifically, we show how the process tensor describing the effect of the environment can be iteratively constructed and compressed using matrix product state techniques. We demonstrate the power of this method by applying it to a range of open quantum systems, including with bosonic, fermionic, and spin environments. The versatility and efficiency of our automated compression of environments method provides a practical general-purpose tool for open quantum systems. Postprint

AKG is grateful to the Royal Society for Newton International Fellowship NF171163. We acknowledge support from the Engineering and Physical Sciences Research Council of the UK (grants EP/P010482/1 and EP/L017008/1). We are also grateful for financial support from the University of St Andrews Restarting Research and Restarting Interdisciplinary Research Funding Schemes (SARRF and SARIRF) which are funded through the Scottish Funding Council grant reference SFC/AN/08/020. We have designed a highly twisted small TADF emitter PXZ-α-DK based on an a-diketone (α-DK) as a strong acceptor and phenoxazine (PXZ) as a strong donor to obtain red-shifted emission in comparison to the equivalent a-diketone linked to 9,9-dimethyl-9,10-dihydroacridine (DMAC). The PXZ-α-DK shows emission at 586 nm and DMAC-α-DK shows emission at 548 nm in 1,3-bis(N-carbazolyl)benzene (mCP) host at 1.5 wt% doping of the emitter, with short-delayed lifetimes of 6.9 μs for PXZ-α-DK and 7.6 μs for DMAC-α-DK. OLEDs fabricated using these emitters show green electroluminescence at 555 nm for DMAC-α-DK, with a maximum external quantum efficiency, EQEmax, of 6.3%, and orange electroluminescence at 585 nm for PXZ-α-DK, with an EQEmax of 0.8%. We corroborate the optoelectronic properties of these emitters with DFT calculations. Postprint

We would like to thank the China Scholarships Council for a studentship to CH. PSH and WZ thank the Welch Foundation (Grant E-1457) and the National Science Foundation (DMR-2002319) for support. Two-dimensional (2D) organic−inorganichybrid copper perovskites have drawn tremendous attention as promisingmultifunctional materials. Herein, by incorporating ortho, metaand para-chlorine substitution in the benzylamine structure, we firstlyreport theinfluence of positional isomerism on the crystal structures of chlorobenzylammonium copper (II) chloride perovskites A2CuCl4. 2Dpolar ferromagnets (3-ClbaH)2CuCl4 and (4-ClbaH)2CuCl4(ClbaH+ = chlorobenzylammonium) are successfully obtained. They bothadopt a polar monoclinic space group Cc at room temperature, displayingsignificant differences in crystal structures. In contrast, (2-ClbaH)2CuCl4adopts a centrosymmetric space group P21/c at roomtemperature. This associated structural evolution successfullyenhances the physical properties of the two polar compounds with high thermalstability, discernible second harmonic generation (SHG) signals, ferromagnetism,and narrowoptical band gaps.These findings demonstrate that theintroduction of chlorine atoms into the inter-layer organicspecies is a powerful tool to tune crystalsymmetries and physical properties, and this inspires further exploration of designinghigh-performance multifunctional copper-based materials. Publisher PDF

Financial support from the National Council of Science and Technology (Conacyt) Mexico. Funding from the Foundation of Polish Science (First TEAM/2017-3/30). Perylene diimide derivatives with different functional groups (OR) in the bay position were synthesised (PDI-1, OR = OC6H4OMe; PDI-2, OR = OC6H4CH2CH2NHBoc; PDI-3, OR = OC6H4CO2Me) and their optoelectronical properties were characterised. The derivatives were applied as alternative electron transport materials (ETMs) to replace the commonly used PCBM in inverted perovskite solar cells (PSCs). Devices with the structure ITO/PTAA/Cs0.04(MA0.17FA0.83)0.96Pb(I0.83Br0.17)3/ETM/Ag (ETM = PCBM or PDI-1, -2 or -3) were fabricated through solution processing techniques. A competitive power conversion efficiency (PCE) of 16.8% was obtained for the PDI-3-based device, which was comparable to the PCBM-based device with PCE of 17.3%. It was found that the electronic nature of the functional groups plays an important role in the charge extraction and band alignment of these small molecular semiconductors. Publisher PDF

F.J., A.P.M., and C.W.H. acknowledge the financial support of the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) TRR 288-422213477 (Project A10). A.P. acknowledges support by the Alexander von Humboldt Foundation through a Feodor Lynen fellowship during his work at UCLA. N.K. is supported by KAKENHI Grants-in-Aids for Scientific Research (Grants No. 18K04715, No. 21H01033, and No. 22K19093), Core-to-Core Program (No. JPJSCCA20170002) from the Japan Society for the Promotion of Science (JSPS), and the JST-Mirai Program (Grant No. JPMJMI18A3). A.C. is grateful for support from the Julian Schwinger Foundation for Physics Research. The work at University of California, Los Angeles, was supported by NSF Grant No. 2004553. In-plane uniaxial pressure has been shown to strongly tune the superconducting state of Sr2RuO4 by approaching a Lifshitz transition and associated Van Hove singularity (VHS) in the density of states. At the VHS, Tc and the in- and out-of-plane upper critical fields are all strongly enhanced, and the latter has changed its curvature as a function of temperature from convex to concave. However, due to strain inhomogeneity it has not been possible so far to determine how the upper critical fields change with strain. Here, we show the strain dependence of both upper critical fields, which was achieved due to an improved sample preparation. We find that the in-plane upper critical field is mostly linear in Tc. On the other hand, the out-of-plane upper critical field varies with a higher power in Tc, and peaks strongly at the VHS. The strong increase in magnitude and the change in form of Hc2||c occur very close to the Van Hove strain, and point to a strong enhancement of both the density of states and the gap magnitude at the Lifshitz transition. Publisher PDF

Funding: Open access funded by Max Planck Society. The authors acknowledge the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany’s Excellence Strategy-EXC-2123 Quantum Frontiers - 390837967; Core program PC2-PN23080202 and the PN-III-P2-2.1-PED-2021-0378 (contract no. 575PED/2022) granted projects, financed by the Romanian Ministry of Research, Innovation and Digitalization/UEFISCDI; and the generous allocation of computer time at the computing center of Donostia International Physics Center and at the Red Española de Supercomputación (project QHS-2021-2-0019). A.A. acknowledges support from Project No. PID2019-103910GB-I00, funded by MCIN/AEI/10.13039/501100011033/ and FEDER Una manera de hacer Europa, and Project No. IT-1527-22 funded by the Basque Government. The changes of properties and preferential interactions based on subtle energetic differences are important characteristics of organic molecules, particularly for their functionalities in biological systems. Only slightly energetically favored interactions are important for the molecular adsorption and bonding to surfaces, which define their properties for further technological applications. Here, prochiral tetracenothiophene molecules are adsorbed on the Cu(111) surface. The chiral adsorption configurations are determined by Scanning Tunneling Microscopy studies and confirmed by first-principles calculations. Remarkably, the selection of the adsorption sites by chemically different moieties of the molecules is dictated by the arrangement of the atoms in the first and second surface layers. Furthermore, we have investigated the thermal effects on the direct desulfurization reaction that occurs under the catalytic activity of the Cu substrate. This reaction leads to a product that is covalently bound to the surface in chiral configurations. Publisher PDF

Funding: This work was financially supported by the European Union's Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant (agreement no. 764837) and NCN Opus grant no. 2019/35/B/ST4/03280. We are also grateful to the Engineering and Physical Sciences Research Council of the UK for financial support from grants EP/R511778/1 and EP/L015110/1. Antimicrobial photodynamic therapy (APDT) is a promising approach to fight the growing problem of antimicrobial resistance that threatens health care, food security and agriculture. APDT uses light to excite a light-activated chemical (photosensitiser), leading to the generation of reactive oxygen species (ROS). Many APDT studies confirm its efficacy in vitro and in vivo against bacteria, fungi, viruses and parasites. However, the development of the field is focused on exploring potential targets and developing new photosensitisers. The role of light, a crucial element for ROS production, has been neglected. What are the main parameters essential for effective photosensitiser activation? Does an optimal light radiant exposure exist? And finally, which light source is best? Many reports have described the promising antibacterial effects of APDT in vitro, however, its application in vivo, especially in clinical settings remains very limited. The restricted availability may partially be due to a lack of standard conditions or protocols, arising from the diversity of selected photosensitising agents (PS), variable testing conditions including light sources used for PS activation and methods of measuring anti-bacterial activity and their effectiveness in treating bacterial infections. We thus sought to systematically review and examine the evidence from existing studies on APDT associated with the light source used. We show how the reduction of pathogens depends on the light source applied, radiant exposure and irradiance of light used, and type of pathogen, and so critically appraise the current state of development of APDT and areas to be addressed in future studies. We anticipate that further standardisation of the experimental conditions will help the field advance, and suggest key optical and biological parameters that should be reported in all APDT studies. More in vivo and clinical studies are needed and are expected to be facilitated by advances in light sources, leading to APDT becoming a sustainable, alternative therapeutic option for bacterial and other microbial infections in the future. Publisher PDF

Funding: This project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska Curie grant agreement No 838885 (NarrowbandSSL). S.M.S. acknowledges support from the Marie Skłodowska-Curie Individual Fellowship (grant agreement No 838885 NarrowbandSSL). We would like to thank the Leverhulme Trust (RPG-2016-047) for financial support. E.Z-C. and I.D.W.S acknowledge support from EPSRC (EP/L017008, EP/P010482/1). Computational resources have been provided by the Consortium des Équipements de Calcul Intensif (CÉCI), funded by the Fonds de la Recherche Scientifiques de Belgique (F. R. S.-FNRS) under Grant No. 2.5020.11, as well as the Tier-1 supercomputer of the Fédération Wallonie-Bruxelles, infrastructure funded by the Walloon Region under the grant agreement n1117545. Y.O. acknowledges funding by the Fonds de la Recherche Scientifique-FNRS under Grant n° F.4534.21 (MIS-IMAGINE). G. R. acknowledges a grant from the ‘‘Fonds pour la formation a la Recherche dans l’Industrie et dans l’Agriculture’’ (FRIA) of the FRS-FNRS. We present a p- and n-doped nonacene compound, NOBNacene, that represents a rare example of a linearly extended ladder-type multiresonant thermally activated delayed fluorescence (MR-TADF) emitter. This compound shows efficient narrow deep blue emission, with a λPL of 410 nm, full width at half maximum, FWHM, of 38 nm, photoluminescence quantum yield, ΦPL of 71 %, and a delayed lifetime, τd of 1.18 ms in 1.5 wt % TSPO1 thin film. The organic light-emitting diode (OLED) using this compound as the emitter shows a comparable electroluminescence spectrum peaked at 409 nm (FWHM=37 nm) and a maximum external quantum efficiency (EQEmax) of 8.5 % at Commission Internationale de l’Éclairage (CIE) coordinates of (0.173, 0.055). The EQEmax values were increased to 11.2 % at 3 wt % doping of the emitter within the emissive layer of the device. At this concentration, the electroluminescence spectrum broadened slightly, leading to CIE coordinates of (0.176, 0.068). Publisher PDF

H.L. would like to thank the University of St. Andrews for financial support via a St. Leonard’s scholarship. The authors acknowledge facilities access made possible through support from the EPSRC Light Element Analysis facility Grant EP/T019298/1 and the EPSRC Strategic Equipment Resource Grant EP/R023751/1. Vacancy-ordered halide perovskites have received great interest in optoelectronic applications. In this work, we report the novel inorganic halide Cs10MnSb6Cl30 with a distinctive 10H (10-layer hexagonal) perovskite polytype structure with (hcccc)2 stacking. Cs10MnSb6Cl30 has 30% B-site vacancies ordered at both corner- and face-sharing sites, resulting in [MnSb6Cl30]10–n columns, i.e., a reduction of octahedral connectivity to 1D. This results in enhanced photoluminescence in comparison to the previously reported 25% vacancy-ordered 3C polytype Cs4MnSb2Cl12 with 2D connectivity. This demonstrates not only the existence of the 10H perovskite structure in halides but also demonstrates the degree of B-site deficiency and stacking sequence variation as a direction to tune the optical properties of perovskite polytypes via vacancy rearrangements. Publisher PDF

Funding: We gratefully acknowledge support from the Engineering and Physical Sciences Research Council (Grant Nos. EP/T02108X/1 and EP/R031924/1), the European Research Council (through the QUESTDO project, 714193), and the Leverhulme Trust (Grant No. RL-2016-006). E.A.M., A.Z., and I.M. gratefully acknowledge studentship support from the International Max-Planck Research School for Chemistry and Physics of Quantum Materials. N.K. is supported by a KAKENHI Grants-in-Aids for Scientific Research (Grant Nos.18K04715, and 21H01033), and Core-to-Core Program (No. JPJSCCA20170002) from the Japan Society for the Promotion of Science (JSPS) and by a JST-Mirai Program (Grant No. JPMJMI18A3). APM and CWH acknowledge support from the Deutsche Forschungsgemeinschaft - TRR 435 288 - 422213477 (project A10). We thank Diamond Light Source for access to Beamline I05 (Proposals SI27471 and SI28412), which contributed to the results presented here. We report the evolution of the electronic structure at the surface of the layered perovskite Sr2RuO4 under large in-plane uniaxial compression, leading to anisotropic B1g strains of εxx − εyy = −0.9 ± 0.1%. From angle-resolved photoemission, we show how this drives a sequence of Lifshitz transitions, reshaping the low-energy electronic structure and the rich spectrum of van Hove singularities that the surface layer of Sr2RuO4 hosts. From comparison to tight-binding modelling, we find that the strain is accommodated predominantly by bond-length changes rather than modifications of octahedral tilt and rotation angles. Our study sheds new light on the nature of structural distortions at oxide surfaces, and how targeted control of these can be used to tune density of states singularities to the Fermi level, in turn paving the way to the possible realisation of rich collective states at the Sr2RuO4 surface. Postprint

Funding: The St Andrews team is grateful to the Engineering and Physical Sciences Research Council (EPSRC) for support from grants EP/P010482/1, EP/R035164/1 and EP/L017008/1. Kyushu team would like to acknowledge Kyulux inc and JSPS Core-to-Core Program (grant number: JPJSCCA20180005) for the support of this project. Three new 1,2,4,5-tetraphenylimidazole derivatives, 9,9-dimethyl-10-(4-(2,4,5-triphenyl-1H-imidazol-1-yl)phenyl)-9,10-dihydroacridine ( DMAC - TPI ), 10-(4-(2,4,5-triphenyl-1H-imidazol-1-yl)phenyl)-10H-phenoxazine ( PXZ-TPI ), and 10-(4-(2,4,5-triphenyl-1H-imidazol-1-yl)phenyl)-10H-phenothiazine ( PTZ - TPI ), bearing different electron donors at the N1 position of the imidazole were synthesised and characterised. DMAC - TPI and PXZ - TPI showed narrow emission at λPL of 388 and 418 nm in toluene, and in doped films in Zeonex polymer (1 wt.%) at λPL 381 and 407 nm, respectively, with a full width at half maximum (FWHM) ranging 0.42-0.44 eV. DMAC - TPI and PXZ - TPI are predicted to show very low oscillator strength for the low-energy transitions, which aligns to the observed low photoluminescence quantum yields. Both molecules showed a singlet-triplet energy gap (ΔEST of around 1.2 eV) that is much too large to enable reverse intersystem crossing and thermally activated delayed fluorescence. Connecting a donor group to TPI at the N1 position can lead to room temperature phosphorescence (RTP), as the example of PTZ - TPI showed. Publisher PDF

The quest to improve transparent conductors balances two key goals: increasing electrical conductivity and increasing optical transparency. To improve both simultaneously is hindered by the physical limitation that good metals with high electrical conductivity have large carrier densities that push the plasma edge into the ultra-violet range. Technological solutions reflect this trade-off, achieving the desired transparencies only by reducing the conductor thickness or carrier density at the expense of a lower conductance. Here we demonstrate that highly anisotropic crystalline conductors offer an alternative solution, avoiding this compromise by separating the directions of conduction and transmission. We demonstrate that slabs of the layered oxides Sr2RuO4 and Tl2Ba2CuO6+δ are optically transparent even at macroscopic thicknesses >2 μm for c-axis polarized light. Underlying this observation is the fabrication of out-of-plane slabs by focused ion beam milling. This work provides a glimpse into future technologies, such as highly polarized and addressable optical screens., Nature Communications, 14 (1), ISSN:2041-1723

Kagome materials have emerged as a setting for emergent electronic phenomena that encompass different aspects of symmetry and topology. It is debated whether the XV$_6$Sn$_6$ kagome family (where X is a rare earth element), a recently discovered family of bilayer kagome metals, hosts a topologically non-trivial ground state resulting from the opening of spin-orbit coupling gaps. These states would carry a finite spin-Berry curvature, and topological surface states. Here, we investigate the spin and electronic structure of the XV$_6$Sn$_6$ kagome family. We obtain evidence for a finite spin-Berry curvature contribution at the center of the Brillouin zone, where the nearly flat band detaches from the dispersing Dirac band because of spin-orbit coupling. In addition, the spin-Berry curvature is further investigated in the charge density wave regime of ScV$_6$Sn$_6$, and it is found to be robust against the onset of the temperature-driven ordered phase. Utilizing the sensitivity of angle resolved photoemission spectroscopy to the spin and orbital angular momentum, our work unveils the spin-Berry curvature of topological kagome metals, and helps to define its spectroscopic fingerprint., Comment: 21 pages, 4 figures

The single-layered ruthenate Sr$_2$RuO$_4$ is one of the most enigmatic unconventional superconductors. While for many years it was thought to be the best candidate for a chiral $p$-wave superconducting ground state, desirable for topological quantum computations, recent experiments suggest a singlet state, ruling out the original $p$-wave scenario. The superconductivity as well as the properties of the multi-layered compounds of the ruthenate perovskites are strongly influenced by a van Hove singularity in proximity of the Fermi energy. Tiny structural distortions move the van Hove singularity across the Fermi energy with dramatic consequences for the physical properties. Here, we determine the electronic structure of the van Hove singularity in the surface layer of Sr$_2$RuO$_4$ by quasiparticle interference imaging. We trace its dispersion and demonstrate from a model calculation accounting for the full vacuum overlap of the wave functions that its detection is facilitated through the octahedral rotations in the surface layer., 13 pages, 6 figures, and supplementary information

We report the first experimental realization of the prime number quantum potential $V_N(x)$, defined as the potential entering the single-particle Schr\"{o}dinger Hamiltonian with eigenvalues given by the first $N$ prime numbers. We use holographic optical traps and, in particular, a spatial light modulator to tailor the potential to the desired shape. As a further application, we also implement a potential with lucky numbers, a sequence of integers generated by a different sieve than the familiar Eratosthenes's sieve used for the primes. Our results pave the way towards the realization of quantum potentials with arbitrary sequences of integers as energy levels and show, in perspective, the possibility to set up quantum systems for arithmetic manipulations or mathematical tests involving prime numbers., Comment: 12 pages, 6 ifgures

Funding: A.P. acknowledges support by the Alexander von Humboldt Foundation through the Feodor Lynen Fellowship. A.C. acknowledges support from the Julian Schwinger Foundation. This work was supported by the National Science Foundation under grant numbers 1709304, 2004553. Work at Los Alamos was supported by the Los Alamos National Laboratory LDRD Program. N.K. is supported by a KAKENHI Grants-in-Aids for Scientific Research (Grant Nos. 17H06136, 18K04715, and 21H01033), and Core-to-Core Program (No. JPJSCCA20170002) from the Japan Society for the Promotion of Science and by a JST-Mirai Program grant (No. JPMJMI18A3). J.M. acknowledges funding by the Slovenian Research Agency (ARRS) under Program No. P1-0044, J1-1696, and J1-2458. The work at Dresden was funded by the Deutsche Forschungsgemeinschaft-TRR 288-422213477 (projects A10 and B01). The Flatiron Institute is a division of the Simons Foundation. We perform nuclear magnetic resonance (NMR) measurements of the oxygen-17 Knight shifts for Sr2RuO4, while subjected to uniaxial stress applied along [100] direction. The resulting strain is associated with a strong variation of the temperature and magnetic field dependence of the inferred magnetic response. A quasiparticle description based on density-functional theory calculations, supplemented by many-body renormalizations, is found to reproduce our experimental results, and highlights the key role of a van-Hove singularity. The Fermi-liquid coherence scale is shown to be tunable by strain, and driven to low values as the associated Lifshitz transition is approached. Publisher PDF

Funding: We acknowledge the financial support of the Max Planck Society. A.P.M. and C.W.H. acknowledge support from the Deutsche Forschungsgemeinschaft through SFB 1143 (Project ID 247310070). M.K. acknowledges financial support from ANR LABEX Grant No. ANR-10-LABX-0039-PALM. We probe the effect on Tc of in-plane uniaxial stress applied to the high-temperature superconductor YBa2Cu3O6.67. We find a highly anisotropic response. Under compression along the b axis, which reduces the orthorhombicity of the CuO2 planes, Tc is broadly flat for stresses up to at least 1.7 GPa. Under compression along the a axis, Tc decreases steeply. For stresses beyond ≈1 GPa the decrease is quasilinear. We hypothesize that superconductivity is suppressed by competition with uniaxial charge density wave order, which has been found to onset at ≈1 GPa. Publisher PDF

Funding: S. W. thanks the China Scholarship Council (201906250199). A. K. G. is grateful to the Royal Society for Newton International Fellowship NF171163. EZ-C and IDWS acknowledge support from EPSRC (EP/L017008, EP/P010482/1). We are also grateful for financial support from the University of St Andrews Restarting Research Funding Scheme (SARRF) which is funded through the Scottish Funding Council grant reference SFC/AN/08/020. EZ-C is a Royal Society Leverhulme Trust Senior Research fellow (SRF\R1\201089). We would also like to thank the Leverhulme Trust (RPG-2016-047) for financial support. Herein, we demonstrate how judicious selection of donor decorating a central multi-resonant thermally activated delayed fluorescence (MR-TADF) core based on DiKTa can lead to very high-performance OLEDs. Decorating the DiKTa core with triphenylamine (TPA) and diphenylamine (DPA), 3TPA-DiKTa and 3DPA-DiKTa exhibit bright, narrowband green and red emission in doped films, respectively. The OLEDs based on these emitters showed record-high performance with maximum external quantum efficiencies (EQEmax) for this family of emitters, with a EQEmax of 30.8% for 3TPA-DiKTa at λEL of 551 nm and 16.7% for 3DPA-DiKTa at λEL of 613 nm. The efficiency roll-off in the OLEDs was improved significantly by using 4CzIPN as an assistant dopant in hyperfluorescence (HF) devices. The outstanding device performance has been attributed to preferential horizontal orientation of the transition dipole moments of 3TPA-DiKTa and 3DPA-DiKTa. Publisher PDF

We study how polariton condensation modifies charge transport in organic materials. In typical organic materials, charge transport proceeds via incoherent hopping. We therefore provide an approach to determine how the rate and final state of this hopping process is affected by strong matter-light coupling and polariton condensation. We show how the hopping process may create excitations when starting from a state with a finite excitation density. That is, how hopping can change the state of a lower polariton condensate by creating upper polaritons, optically inactive excitonic dark states, or by exciting vibrational sidebands. While the matrix elements for these processes can be large, for typical materials at room temperature, such excitations are suppressed by thermal factors, and ground state processes dominate. We thus study how the ground state hopping rate depends on condensate density, matter-light coupling, and cavity photon detuning. All these factors change the vibrational configuration associated with the optically active molecules, which can enhance or suppress hopping by increasing or decreasing the vibrational overlap with the state of a charged molecule. We show that hopping rates can be exponentially sensitive to detuning and condensate density, allowing an increase or decrease of hopping rate by two orders of magnitude., Comment: 21 pages, 8 figures

Magnonic devices operating at terahertz frequencies offer intriguing prospects for high-speed electronics with minimal energy dissipation However, guiding and manipulating terahertz magnons via external parameters present formidable challenges. Here we report the results of magnetic Raman scattering experiments on the antiferromagnetic spin-orbit Mott insulator Sr2IrO4 under uniaxial stress. We find that the energies of zone-center magnons are extremely stress sensitive: lattice strain of 0.1% increases the magnon energy by 40%. The magnon response is symmetric with respect to the sign of the applied stress (tensile or compressive), but depends strongly on its direction in the IrO2 planes. A theory based on coupling of the spin-orbit-entangled iridium magnetic moments to lattice distortions provides a quantitative explanation of the Raman data and a comprehensive framework for the description of magnon-lattice interactions in magnets with strong spin-orbit coupling. The possibility to efficiently manipulate the propagation of terahertz magnons via external stress opens up multifold design options for reconfigurable magnonic devices.

We study the dynamics of multimode polariton lasing in organic microcavities by using a second-order cumulant equation approach. By inspecting the time evolution of the photon mode occupations, we show that if multiple lasing peaks are observed in time-integrated mode occupations, the reason can be either bi-modal lasing or temporal switching between several modes. The former takes place within a narrow range of parameters while the latter occurs more widely. We find that the origin of the temporal switching is different in the weak- and strong-coupling regimes. At weak coupling slope efficiency is the determining factor, while for strong coupling it is changes in the eigenmodes and gain spectrum upon pumping. This difference is revealed by investigating the photoluminescence and momentum-resolved gain spectra. Our results underscore the importance of understanding the time evolution of the populations when characterizing the lasing behaviour of a multimode polariton system, and show how these features differ between weak and strong coupling., Comment: 15 pages, 13 figures

Tracing out the environmental degrees of freedom is a necessary procedure when simulating open quantum systems. While being an essential step in deriving a tractable master equation it represents a loss of information. In situations where there is strong interplay between the system and environmental degrees of freedom this loss makes understanding the dynamics challenging. These dynamics, when viewed in isolation, have no time-local description: they are non-Markovian and memory effects induce complex features that are difficult to interpret. To address this problem, we here show how to use system correlations, calculated by any method, to infer any correlation function of a Gaussian environment, so long as the coupling between system and environment is linear. This not only allows reconstruction of the full dynamics of both system and environment, but also opens avenues into studying the effect of a system on its environment. In order to obtain accurate bath dynamics, we exploit a numerically exact approach to simulating the system dynamics, which is based on the construction and contraction of a tensor network that represents the process tensor of this open quantum system. Using this we are able to find any system correlation function exactly. To demonstrate the applicability of our method we show how heat moves between different modes of a bosonic bath when coupled to a two-level system that is subject to an off-resonant drive., Comment: 11+8 pages, 4+2 figures

Funding: M. K. would like to thank 2214-A International Research Fellowship Programme for Ph.D. students (1059B141900585). This project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska Curie grant agreement No 838885 (NarrowbandSSL). S.M.S. acknowledges support from the Marie Skłodowska-Curie Individual Fellowship (grant agreement No 838885 NarrowbandSSL). A. K. G. is grateful to the Royal Society for Newton International Fellowship NF171163. L.M acknowledges that the project who gave rise to these results received support from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme Grant agreement No. 834431, the Spanish Ministry of Science, Innovation and Universities (MICIU, RTI2018-095362-A-I00, and EQC2018-004888-P) and the Comunitat Valenciana (IDIFEDER/2020/063 and PROMETEU/2020/077). D.T. acknowledges support from the Comunitat Valenciana (CIGE/2021/0). We designed and synthesized two new ionic thermally activated delayed fluorescent (TADF) emitters that are charged analogues of a known multiresonant TADF (MR-TADF) compound, DiKTa . The emission of the charged derivatives is red-shifted compared to the parent compound. For instance, DiKTa-OBuIm emits in the green (λPL = 499 nm, 1 wt % in mCP) while DiKTa-DPA-OBuIm emits in the red (λPL = 577 nm, 1 wt % in mCP). In 1 wt % mCP films, both emitters showed good photoluminescence quantum yields of 71% and 61%, and delayed lifetimes of 316.6 μs and 241.7 μs, respectively, for DiKTa-OBuIm and DiKTa-DPA-OBuIm , leading to reverse intersystem crossing rates of 2.85 × 103 s−1 and 3.04 × 103 s−1. Light-emitting electrochemical cells were prepared using both DiKTa-OBuIm and DiKTa-DPA-OBuIm as active emitters showing green (λmax = 534 nm) and red (λmax = 656 nm) emission, respectively. Publisher PDF

JMS acknowledges the Coordenação de Aperfeiçoamento de Pessoal de Nível Superior – Brasil (CAPES) – Finance Code 001 for PhD funding. LKJ acknowledges support from the Marie Skłodowska-Curie Individual Fellowship (European Commission) (MCIF: no. 745776) and funding from UKRI-FLF through MR/T022094/1. GC thanks the EPSRC (EP/E036244/1) for funding. BODIPY-based materials are well known for their outstanding chemical and photo-stability as well as their ease of synthesis and tunability of their frontier molecular orbitals. These are attractive features for hole transporting materials (HTMs) for perovskite solar cells (PSCs) that could help improve device stability and cost. In this paper, we report the straightforward synthesis of a new BODIPY small molecule, PTZ-PTZ-BDP , functionalised with phenothiazine moieties in both the meso and α positions giving rise to a Y-shaped structure. As estimated by DFT calculations, and confirmed by electrochemical and ambient photoemission spectroscopy studies, PTZ-PTZ-BDP presents appropriate energy levels suitable for its use as a HTM in PSCs. Electrochemical measurements also reveal several redox processes with excellent reversibility. Systematic evaluation of its performance as HTM in n–i–p PSC with and without dopants was conducted and the device parameters compared with commonly used HTMs of spiro-OMeTAD and PTAA. The CH3NH3PbI3 based PSCs incorporating simple solution processed PTZ-PTZ-BDP as HTM demonstrated a champion power conversion efficiency of 14.6%, matched in performance and shelf-life stability to complex and expensive state-of-the-art HTMs, showing that BODIPY based HTMs are a promising direction for perovskite solar cells. Publisher PDF

Funding: We acknowledge funding from the Physics of Quantum Materials department and the research group “Physics of Unconventional Metals and Superconductors (PUMAS)” of the Max Planck Society. C.G. and E.H. acknowledge support from the German Science Foundation (DFG) through grant GE 602/4-1 Fermi-NESt. P.M.R.B. was supported by the Marsden Fund Council from Government funding, managed by Royal Society Te Apārangi. R.K. is supported by the DFG through project. no. KU 3287/1-1. D.F.A. was supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering, under award DE-SC0021971. Materials with multiple superconducting phases are rare. Here, we report the discovery of two-phase unconventional superconductivity in CeRh2As2 Using thermodynamic probes, we establish that the superconducting critical field of its high-field phase is as high as 14 tesla, even though the transition temperature is only 0.26 kelvin. Furthermore, a transition between two different superconducting phases is observed in a c axis magnetic field. Local inversion-symmetry breaking at the cerium sites enables Rashba spin-orbit coupling alternating between the cerium sublayers. The staggered Rashba coupling introduces a layer degree of freedom to which the field-induced transition and high critical field seen in experiment are likely related. Postprint Postprint

Funding: This work was primarily supported by the U.S. Department of Energy, Office of Basic Sciences, Division of Materials Sciences and Engineering, under Award No. DE-SC0002334. Single-crystal delafossite PdCoO2 is known to have an extremely low intrinsic impurity concentration of ~0.001%, demonstrating extraordinarily high conductivity with a mean free path of ~20 microns at low temperatures. However, when grown as thin films, the resistivity at room temperature increases by a factor of 3 to 80 times, depending on the film thickness. Using scanning transmission electron microscopy, we identify different classes of defects for the single crystal vs epitaxial thin film. The dominant defect for single-crystal PdCoO2 is found to be ribbon-like defects. For the thin films, we identify different types of defects arising in epitaxial thin films mainly due to substrate termination that disrupt the lateral connectivity of the conducting planes. Our results are consistent with the high conductivity of single crystals and increased electrical resistivity of the thin films compared to that of single crystals, suggesting that selecting a proper substrate, improving surface quality, and reducing the step density are the keys to enhance the film quality for utilizing PdCoO2 as a platform for future applications. Postprint

Van-der-Waals (vdW) ferromagnets have enabled the development of heterostructures assembled from exfoliated monolayers with spintronics functionalities, making it important to understand and ultimately tune their magnetic properties at the microscopic level. Information about the magnetic properties of these systems comes so far largely from macroscopic techniques, with little being known about the microscopic magnetic properties. Here, we combine spin-polarized scanning tunneling microscopy and quasi-particle interference imaging with neutron scattering to establish the magnetic and electronic properties of the metallic vdW ferromagnet Fe3GeTe2. By imaging domain walls at the atomic scale, we can relate the domain wall width to the exchange interaction and magnetic anisotropy extracted from the magnon dispersion as measured in inelastic neutron scattering, with excellent agreement between the two techniques. From comparison with Density Functional Theory calculations we can assign the quasi-particle interference to be dominated by spin-majority bands. We find a dimensional dichotomy of the bands at the Fermi energy: bands of minority character are predominantly two-dimensional in character, whereas the bands of majority character are three-dimensional. We expect that this will enable new design principles for spintronics devices., 18 pages main manuscript with 5 figures plus 12 pages supplementary

Funding: F.J., A.P.M., and C.W.H. acknowledge the financial support of the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) - TRR 288 - 422213477 (project A10). H.S.R. and S.H.S. acknowledge the financial support of the Engineering and Physical Sciences Research Council (UK). H.S.R. acknowledges support from the Aker Scholarship. T.S. acknowledges the support of the Natural Sciences and Engineering Research Council of Canada (NSERC), in particular the Discovery Grant [RGPIN-2020-05842], the Accelerator Supplement [RGPAS-2020-00060], and the Discovery Launch Supplement [DGECR-2020-00222]. N.K. is supported by a KAKENHI Grants-in-Aids for Scientific Research (Grant Nos.17H06136, 18K04715, and 21H01033), and Core-to-Core Program (No. JPJSCCA20170002) from the Japan Society for the Promotion of Science (JSPS) and by a JST-Mirai Program (Grant No. JPMJMI18A3). Applying in-plane uniaxial pressure to strongly correlated low-dimensional systems has been shown to tune the electronic structure dramatically. For example, the unconventional superconductor Sr2RuO4 can be tuned through a single Van Hove point, resulting in strong enhancement of both Tc and Hc2. Out-of-plane (c axis) uniaxial pressure is expected to tune the quasi-two-dimensional structure even more strongly, by pushing it towards two Van Hove points simultaneously. Here, we achieve a record uniaxial stress of 3.2 GPa along the c axis of Sr2RuO4. Hc2 increases, as expected for increasing density of states, but unexpectedly Tc falls. As a first attempt to explain this result, we present three-dimensional calculations in the weak interaction limit. We find that within the weak-coupling framework there is no single order parameter that can account for the contrasting effects of in-plane versus c-axis uniaxial stress, which makes this new result a strong constraint on theories of the superconductivity of Sr2RuO4. Publisher PDF

Funding information: B.J.R. and S.G. acknowledge support from the Office of Basic Energy Sciences of the U.S. Department of Energy under award No. DE-SC0020143. B.J.R. and S.G. acknowledge support from the Cornell Center for Materials Research with funding from the Materials Research Science and Engineering Centers program of the National Science Foundation (cooperative agreement No. DMR-1719875). T.G.K. acknowledges support from the National Science Foundation under Grant No. PHY-2110250. N.K. acknowledges support from Japan Society for the Promotion of Science (JSPS) KAKENHI (Grants No. JP17H06136, No. JP18K04715, and No. 21H01033) and Japan Science and Technology Agency Mirai Program (JPMJMI18A3) in Japan. Recent experiments suggest that Sr2RuO4 has a two-component superconducting order parameter (OP). A two-component OP has multiple degrees of freedom in the superconducting state that can result in low-energy collective modes or the formation of domain walls—a possibility that would explain a number of experimental observations including the smallness of the signature of time reversal symmetry breaking at Tc and telegraph noise in critical current experiments. We use resonant ultrasound spectroscopy to perform ultrasound attenuation measurements across the superconducting Tc of Sr2RuO4. We find that compressional sound attenuation increases by a factor of 7 immediately below Tc , in sharp contrast with what is found in both conventional (s-wave) and high-Tc (d-wave) superconductors. Our observations are most consistent with the presence of domain walls that separate different configurations of the superconducting OP. The fact that we only observe an increase in sound attenuation for compressional strains, and not for shear strains, suggests an inhomogeneous superconducting state formed of two distinct, accidentally degenerate superconducting OPs that are not related to each other by symmetry. Whatever the mechanism, a factor of 7 increase in sound attenuation is a singular characteristic that must be reconciled with any potential theory of superconductivity in Sr2RuO4. Publisher PDF

The strong nonlinearities of exciton-polariton condensates in lattices make them suitable candidates for neuromorphic computing and physical simula- tions of complex problems. So far, all room temperature polariton condensate lattices have been achieved by nanoimprinting microcavities, which by nature lacks the crucial tunability required for realistic reconfigurable simulators. Here, we report the observation of a quantised oscillating nonlinear quantum fluid in 1D and 2D potentials in an organic microcavity at room temperature, achieved by an on-the-fly fully tuneable optical approach. Remarkably, the condensate is delocalised from the excitation region by macroscopic dis- tances, leading both to longer coherence and a threshold one order of mag- nitude lower than that with a conventional Gaussian excitation profile. We observe different mode selection behaviour compared to inorganic materials, which highlights the anomalous scaling of blueshift with pump intensity and the presence of sizeable energy-relaxation mechanisms. Our work is a major step towards a fully tuneable polariton simulator at room temperature. Ministry of Education (MOE) Published version M.W., G.A.T., and I.D.W.S. acknowledge financial support from the Engineering and Physical Sciences Research Council (EPSRC) programme grant Hybrid Polaritonics (EP/M025330/1), and from the Scottish Funding Council. W.V. and T.L. were supported by the Ministry of Education (Singapore) Tier 2 grant MOE2019-T2-004. H.O. acknowledges EPSRC through a grant (EP/S014403/1). K.O. acknowledges EPSRC for PhD studentship support through a grant (EP/L015110/1).

We introduce a numerical method to determine the Hamiltonian of Mean Force (HMF) Gibbs state for a quantum system strongly coupled to a reservoir. The method adapts the Time Evolving Matrix Product Operator (TEMPO) algorithm to imaginary time propagation. By comparing the real-time and imaginary-time propagation for a generalized spin-boson model, we confirm that the HMF Gibbs state correctly predicts the steady state. We show that the numerical dynamics match the polaron master equation at strong coupling. We illustrate the potential of the imaginary-time TEMPO approach by exploring reservoir-induced entanglement between qubits., Comment: 8 pages, 7 figures

AKG is grateful to the Royal Society for Newton International Fellowship NF171163. We acknowledge support from the Engineering and Physical Sciences Research Council of the UK (grants EP/P010482/1 and EP/L017008/1). We thank the EPSRC UK National Mass Spectrometry Facility at Swansea University for analytical services. We thank Umicore for providing palladium (II) acetate. We report an organic emitter containing a β-triketone electron acceptor core and phenoxazine as the electron donors ( TPXZBM ) for solution-processed organic light-emitting diodes (OLEDs). The resulting molecule is very unusual because it shows both thermally activated delayed fluorescence (TADF) and intramolecular proton transfer. We compare its performance with the previously reported diketone analogue PXZPDO . Solution-processed OLEDs of PXZPDO and TPXZBM show maximum external quantum efficiencies of 20.1% and 12.7%, respectively. The results obtained for the solution-processed PXZPDO -based device are as good as the previously reported evaporated device. At a very high luminance of 10,000 cd/m2 the efficiency of the OLEDs was 10.6% for PXZPDO and 4.7% for TPXZBM , demonstrating relatively low efficiency roll-off for TADF materials. The low efficiency roll-off was rationalized on the basis of the short delayed lifetimes of 1.35 μs for PXZPDO and 1.44 μs for TPXZBM . Our results suggest that intramolecular proton transfer may be useful for the design of OLED materials with low efficiency roll-off. Postprint

GC acknowledges the EPSRC for funding (EP/E036244/1). JMS acknowledges the Coordenação de Aperfeiçoamento de Pessoal de Nível Superior – Brasil (CAPES) – Finance Code 001 for PhD funding. JMS also acknowledges Dr Nor Basid Adiwibawa Prasetya for helpful advice. Dr L. K. Jagadamma acknowledges support from a Marie Skłodowska-Curie Individual Fellowship (European Commission) (MCIF: No. 745776). Thiophene-based semiconductors are amongst the most successful materials in organic electronics. In this contribution, we present the synthesis and characterisation of two thiophene-based macrocycles as well as their evaluation in organic-electronic devices. McT-1 is composed of ten thiophene moieties, whereas in McT-2, four additional electron-deficient benzothiadiazole moieties are incorporated to form a donor–acceptor (D–A) π-system. Red-shifted and broadened absorption spectra as well as more positive redox potentials are observed in McT-2, whereas McT-1 displays a sharper absorption band with a higher extinction coefficient. Macrocycle McT-1 shows emission in the yellow region whereas McT-2 displays emission in the red wavelength region. DFT calculations predict the macrocycles to comprise of mainly the E,E isomers with a near-planar structure, which is further supported by the single crystal X-ray structure for McT-1. Their charge transporting properties are determined by fabricating thin-film OFETs. The photovoltaic properties of McT-1 and McT-2 are also investigated by fabricating bulk heterojunction (BHJ) devices and their potential as photodetectors has been evaluated. Publisher PDF

This work was carried out within the framework of a Max-Planck independent research group on strongly correlated systems. We acknowledge financial support from the Deutsche Forschungsgemeinschaft through SFB 1143 (Project No. 247310070) and Cluster of Excellence ct.qmat (EXC 2147, Project No. 390858490), EPSRC (EP/T028637/1), ShanghaiTech University, Agencia Nacional de Promoción Científica y Tecnológica through PICT 2017-2347, and Consejo Nacional de Investigaciones Científicas y Técnicas through PIP 0446. Metamagnetic transitions are analogs of a pressure-driven gas-liquid transition in water. In insulators, they are marked by a superlinear increase in the magnetization that occurs at a field strength set by the spin exchange interactions. Here we study topological metamagnets, in which the magnetization is itself a topological quantity and for which we find a single transition line for two materials with substantially different magnetic interactions: the spin ices Dy2Ti2O7 and Ho2Ti2O7. We study single crystals under magnetic field and stress applied along the [001] direction and show that this transition, of the Kasteleyn type, has a magnetization versus field curve with upward convexity and a distinctive asymmetric peak in the susceptibility. We also show that the dynamical response of Ho2Ti2O7 is sensitive to changes in the Ho3+ environment induced by compression along [001]. Uniaxial compression may open up experimental access to equilibrium properties of spin ice at lower temperatures. Publisher PDF

S.W. thanks the China Scholarship Council (201906250199). EZ-C and IDWS acknowledge support from EPSRC (EP/L017008, EP/P010482/1). We are also grateful for financial support from the University of St Andrews Restarting Research Funding Scheme (SARRF) which is funded through the Scottish Funding Council grant reference SFC/AN/08/020. EZ-C is a Royal Society Leverhulme Trust Senior Research fellow (SRF\R1\201089). We would also like to thank the Leverhulme Trust (RPG-2016-047) for financial support. This project has received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska Curie grant agreement No 838885 (NarrowbandSSL). S.M.S. acknowledges support from the Marie Skłodowska-Curie Individual Fellowship. Computational resources have been provided by the Consortium des Équipements de Calcul Intensif (CÉCI), funded by the Fonds de la Recherche Scientifiques de Belgique (F.R.S.-FNRS) under Grant No. 2.5020.11, as well as the Tier-1 supercomputer of the Fédération Wallonie-Bruxelles, infrastructure funded by the Walloon Region under the grant agreement n1117545. Y.O. acknowledges funding by the Fonds de la Recherche Scientifique-FNRS under Grant n° F.4534.21 (MIS-IMAGINE). D.B. is a FNRS Research Director. Strategies to tune the emission of multiresonant thermally activated delayed fluorescence (MR-TADF) emitters remain rare. Here, we explore the effect of donor substitution about a MR-TADF core on the emission energy and the nature of the excited state. We decorate different numbers and types of electron-donors about a central MR-TADF core, DiKTa. Depending on the identity and number of donor groups, the excited state either remains short-range charge transfer (SRCT) and thus characteristic of an MR-TADF emitter or becomes a long-range charge transfer (LRCT) that is typically observed in donor–acceptor TADF emitters. The impact is that in three examples that emit from a SRCT state, Cz-DiKTa, Cz-Ph-DiKTa, and 3Cz-DiKTa, the emission remains narrow, while in four examples that emit via a LRCT state, TMCz-DiKTa, DMAC-DiKTa, 3TMCz-DiKTa, and 3DMAC-DiKTa, the emission broadens significantly. Through this strategy, the organic light-emitting diodes fabricated with the three MR-TADF emitters show maximum electroluminescence emission wavelengths, λEL, of 511, 492, and 547 nm with moderate full width at half-maxima (fwhm) of 62, 61, and 54 nm, respectively. Importantly, each of these devices show high maximum external quantum efficiencies (EQEmax) of 24.4, 23.0, and 24.4%, which are among the highest reported with ketone-based MR-TADF emitters. OLEDs with D–A type emitters, DMAC-DiKTa and TMCz-DiKTa, also show high efficiencies, with EQEmax of 23.8 and 20.2%, but accompanied by broad emission at λEL of 549 and 527 nm, respectively. Notably, the DMAC-DiKTa-based OLED shows very small efficiency roll-off, and its EQE remains 18.5% at 1000 cd m–2. Therefore, this work demonstrates that manipulating the nature and numbers of donor groups decorating a central MR-TADF core is a promising strategy for both red-shifting the emission and improving the performance of the OLEDs. Publisher PDF

npj quantum materials 7(1), 98 (2022). doi:10.1038/s41535-022-00508-9, Reducing the thickness of a material to its two-dimensional (2D) limit can have dramatic consequences for its collective electronic states, including magnetism, superconductivity, and charge and spin ordering. An extreme case is $TiTe_2$, where a charge density wave (CDW) emerges in the single-layer, which is absent for the bulk compound, and whose origin is still poorly understood. Here, we investigate the electronic band structure evolution across this CDW transition using temperature-dependent angle-resolved photoemission spectroscopy. Our study reveals an orbital-selective band hybridisation between the backfolded conduction and valence bands occurring at the CDW phase transition, which in turn leads to a significant electronic energy gain, underpinning the CDW transition. For the bulk compound, we show how this energy gain is almost completely suppressed due to the three-dimensionality of the electronic band structure, including via a kz-dependent band inversion which switches the orbital character of the valence states. Our study thus sheds new light on how control of the electronic dimensionality can be used to trigger the emergence of new collective states in 2D materials., Published by Nature Publishing Group, [London]

A chiral quantum Hall (QH) edge state placed in proximity to an s-wave superconductor experiences induced superconducting correlations. Recent experiments have observed the effect of proximity-coupling in QH edge states through signatures of the mediating process of Andreev reflection. We present the microscopic theory behind this effect by modeling the system with a many-body Hamiltonian, consisting of an s-wave superconductor, subject to spin-orbit coupling and a magnetic field, which is coupled by electron tunneling to a QH edge state. By integrating out the superconductor we obtain an effective pairing Hamiltonian in the QH edge state. We clarify the qualitative appearance of nonlocal superconducting correlations in a chiral edge state and analytically predict the suppression of electron-hole conversion at low energies (Pauli blocking) and negative resistance as experimental signatures of Andreev reflection in this setup. In particular, we show how two surface phenomena of the superconductor, namely Rashba spin-orbit coupling and a supercurrent due to the Meissner effect, are essential for the Andreev reflection. Our work provides a promising pathway to the realization of Majorana zero-modes and their parafermionic generalizations., 16 pages, 9 figures. Published version

The authors are highly thankful for the financial support of Higher Education Commission (HEC) Pakistan through the equipment/research grants (6976/Federal/NRPU/R&D/HEC/2017), (20-3071/NRPU/R&D/HEC/13). Author ZS acknowledges HEC for indigenous PhD Fellowship Phase-II, Batch-II, 2013, PIN 213-66018-2PS2-127 and International Research Support Initiative Programme (IRSIP). Author LKJ acknowledges support from a Marie Skłodowska-Curie Individual Fellowship (European Commission) (MCIF: No. 745776). This work demonstrates a route to making mixed halide perovskite powders at room temperature by the anti-solvent-assisted crystallization method. Although, mixed halide CH3NH3PbBr3−xClx perovskites have been prepared by different methods, however, to the best of our knowledge the anti-solvent-assisted crystallization method is employed here for the first time to prepare mixed halide CH3NH3PbBr3−xClx perovskite powders. Solution-processed methyl ammonium lead tribromide CH3NH3PbBr3 (x = 0) and different amounts of chloride (Cl) containing mixed halide perovskites (CH3NH3PbBr3−xClx) were prepared for compositions of x = 0.5, 1, 1.25, 1.75. It reveals that bulk CH3NH3PbBr3−xClx samples are highly crystalline and exists in pure single cubic phase with an increased tolerance factor as compared to pure CH3NH3PbBr3. The CH3NH3PbBr3 perovskite has space-group Pm-3 m and a cell parameter of 5.930 Å (volume = 206 Å). The synthesis route adopted here gives access to hybrid perovskites powders with high Cl content and hence enables the band gap to be precisely tuned over a range from 2.26 to 2.49 eV. The powder samples display the subtle shifts in the emission spectra and the photoluminescence kinetics exhibits a decrease in average lifetime by increasing the Cl contents due to the presence of trap states in the structures that encourage non-radiative recombination of charge carrier. Conventionally, the CH3NH3PbBr3-based inverted solar cell architecture is prepared via mixing of the CH3NH3Br and PbBr2 precursors. In contrast, herein, the precursor solutions are directly prepared from the CH3NH3PbBr3 powder and the active layer of the inverted perovskite solar cells are then spin coated using this solution. The high Voc value of the fabricated solar cells potentially makes it a promising candidate for tandem photovoltaic, photocatalytic water splitting, and semi-transparent photovoltaic applications. Postprint Postprint

Interacting Bosons, loaded in artificial lattices, have emerged as a modern platform to explore collective manybody phenomena, quantum phase transitions and exotic phases of matter as well as to enable advanced on chip simulators. Such experiments strongly rely on well-defined shaping the potential landscape of the Bosons, respectively Bosonic quasi-particles, and have been restricted to cryogenic, or even ultra-cold temperatures. On chip, the GaAs-based exciton-polariton platform emerged as a promising system to implement and study bosonic non-linear systems in lattices, yet demanding cryogenic temperatures. In our work, we discuss the first experiment conducted on a polaritonic lattice at ambient conditions: We utilize fluorescent proteins as an excitonic gain material, providing ultra-stable Frenkel excitons. We directly take advantage of their soft nature by mechanically shaping them in the photonic one-dimensional lattice. We demonstrate controlled loading of the condensate in distinct orbital lattice modes of different symmetries, and finally explore, as an illustrative example, the formation of a gap solitonic mode, driven by the interplay of effective interaction and negative effective mass in our lattice. The observed phenomena in our open dissipative system are comprehensively scrutinized by a nonequilibrium model of polariton condensation. We believe, that this work is establishing the organic polariton platform as a serious contender to the well-established GaAs platform for a wide range of applications relying on coherent Bosons in lattices, given its unprecedented flexibility, cost effectiveness and operation temperature., 19 pages, 4 figures