I05-ARPES
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Alfred J. H.
Jones
,
Ryan
Muzzio
,
Paulina
Majchrzak
,
Sahar
Pakdel
,
Davide
Curcio
,
Klara
Volckaert
,
Deepnarayan
Biswas
,
Jacob
Gobbo
,
Simranjeet
Singh
,
Jeremy T.
Robinson
,
Kenji
Watanabe
,
Takashi
Taniguchi
,
Timur K.
Kim
,
Cephise
Cacho
,
Nicola
Lanata
,
Jill A.
Miwa
,
Philip
Hofmann
,
Jyoti
Katoch
,
Soeren
Ulstrup
Diamond Proposal Number(s):
[24072]
Abstract: The possibility of triggering correlated phenomena by placing a singularity
of the density of states near the Fermi energy remains an intriguing avenue toward engineering the properties of quantum materials. Twisted bilayer gra- phene is a key material in this regard because the superlattice produced by the rotated graphene layers introduces a van Hove singularity and flat bands near the Fermi energy that cause the emergence of numerous correlated phases, including superconductivity. Direct demonstration of electrostatic control of the superlattice bands over a wide energy range has, so far, been critically missing. This work examines the effect of electrical doping on the electronic band structure of twisted bilayer graphene using a back-gated device archi- tecture for angle-resolved photoemission measurements with a nano-focused light spot. A twist angle of 12.2° is selected such that the superlattice Brillouin zone is sufficiently large to enable identification of van Hove singularities and flat band segments in momentum space. The doping dependence of these fea- tures is extracted over an energy range of 0.4 eV, expanding the combinations of twist angle and doping where they can be placed at the Fermi energy and thereby induce new correlated electronic phases in twisted bilayer graphene.
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Jun 2020
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I09-Surface and Interface Structural Analysis
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Diamond Proposal Number(s):
[23159]
Open Access
Abstract: The coupling of nickel‐rich LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes with high‐capacity silicon–graphite (Si–Gr) anodes is one promising route to further increase the energy density of lithium‐ion batteries. Practically, however, the cycle life of such cells is seriously hindered due to continuous electrolyte degradation on the surfaces of both electrodes. In this study, tris(trimethylsilyl) phosphite (TMSPi) is introduced as an electrolyte additive to improve the electrochemical performance of the NMC811/Si–Gr full cells through formation of protective surface layers at the electrode/electrolyte interfaces. This is thought to prevent the surface fluorination of the active materials and enhance interfacial stability. Notably, TMSPi is shown to significantly reduce the overpotential and operando X‐ray diffraction (XRD) confirms that an irreversible “two‐phase” transition reaction caused by the formed adventitious Li2CO3 layer on the surface of NMC811 can transfer to a solid‐solution reaction mechanism with TMSPi‐added electrolyte. Moreover, influences of TMSPi on the cathode electrolyte interphase (CEI) on the NMC811 and solid electrolyte interphase (SEI) on the Si–Gr are systematically investigated by electron microscopy and synchrotron‐based X‐ray photoelectron spectroscopy which allows for the nondestructive depth‐profiling analysis of chemical compositions and oxidation states close to the electrode surfaces.
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Jun 2020
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I05-ARPES
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Junzhang
Ma
,
Han
Wang
,
Simin
Nie
,
Changjiang
Yi
,
Yuanfeng
Xu
,
Hang
Li
,
Jasmin
Jandke
,
Wulf
Wulfhekel
,
Yaobo
Huang
,
Damien
West
,
Pierre
Richard
,
Alla
Chikina
,
Vladimir N.
Strocov
,
Joël
Mesot
,
Hongming
Weng
,
Shengbai
Zhang
,
Youguo
Shi
,
Tian
Qian
,
Ming
Shi
,
Hong
Ding
Diamond Proposal Number(s):
[17080]
Abstract: Parity‐time symmetry plays an essential role for the formation of Dirac states in Dirac semimetals. So far, all of the experimentally identified topologically nontrivial Dirac semimetals (DSMs) possess both parity and time reversal symmetry. The realization of magnetic topological DSMs remains a major issue in topological material research. Here, combining angle‐resolved photoemission spectroscopy with density functional theory calculations, it is ascertained that band inversion induces a topologically nontrivial ground state in EuCd2As2. As a result, ideal magnetic Dirac fermions with simplest double cone structure near the Fermi level emerge in the antiferromagnetic (AFM) phase. The magnetic order breaks time reversal symmetry, but preserves inversion symmetry. The double degeneracy of the Dirac bands is protected by a combination of inversion, time‐reversal, and an additional translation operation. Moreover, the calculations show that a deviation of the magnetic moments from the c‐axis leads to the breaking of C3 rotation symmetry, and thus, a small bandgap opens at the Dirac point in the bulk. In this case, the system hosts a novel state containing three different types of topological insulator: axion insulator, AFM topological crystalline insulator (TCI), and higher order topological insulator. The results provide an enlarged platform for the quest of topological Dirac fermions in a magnetic system.
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Feb 2020
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I16-Materials and Magnetism
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Han Gyeol
Lee
,
Lingfei
Wang
,
Liang
Si
,
Xiaoyue
He
,
Daniel G.
Porter
,
Jeong Rae
Kim
,
Eun Kyo
Ko
,
Jinkwon
Kim
,
Sung Min
Park
,
Bongju
Kim
,
Andrew Thye Shen
Wee
,
Alessandro
Bombardi
,
Zhicheng
Zhong
,
Tae Won
Noh
Diamond Proposal Number(s):
[22181]
Abstract: The metal–insulator transition (MIT) in transition‐metal‐oxide is fertile ground for exploring intriguing physics and potential device applications. Here, an atomic‐scale MIT triggered by surface termination conversion in SrRuO3 ultrathin films is reported. Uniform and effective termination engineering at the SrRuO3(001) surface can be realized via a self‐limiting water‐leaching process. As the surface termination converts from SrO to RuO2, a highly insulating and nonferromagnetic phase emerges within the topmost SrRuO3 monolayer. Such a spatially confined MIT is corroborated by systematic characterizations on electrical transport, magnetism, and scanning tunneling spectroscopy. Density functional theory calculations and X‐ray linear dichroism further suggest that the surface termination conversion breaks the local octahedral symmetry of the crystal field. The resultant modulation in 4d orbital occupancy stabilizes a nonferromagnetic insulating surface state. This work introduces a new paradigm to stimulate and tune exotic functionalities of oxide heterostructures with atomic precision.
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Dec 2019
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B18-Core EXAFS
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Celeste A. M.
Van Den Bosch
,
Andrea
Cavallaro
,
Roberto
Moreno
,
Giannantonio
Cibin
,
Gwilherm
Kerherve
,
José M.
Caicedo
,
Thomas K.
Lippert
,
Max
Doebeli
,
José
Santiso
,
Stephen J.
Skinner
,
Ainara
Aguadero
Diamond Proposal Number(s):
[13530, 16839]
Abstract: Understanding the effects of lattice strain on oxygen surface and diffusion kinetics in oxides is a controversial subject that is critical for developing efficient energy storage and conversion materials. In this work, high‐quality epitaxial thin films of the model perovskite La0.5Sr0.5Mn0.5Co0.5O3−δ (LSMC), under compressive or tensile strain, are characterized with a combination of in situ and ex situ bulk and surface‐sensitive techniques. The results demonstrate a nonlinear correlation of mechanical and chemical properties as a function of the operation conditions. It is observed that the effect of strain on reducibility is dependent on the “effective strain” induced on the chemical bonds. In‐plain strain, and in particular the relative BO length bond, is the key factor controlling which of the B‐site cation can be reduced preferentially. Furthermore, the need to use a set of complimentary techniques to isolate different chemically induced strain effects is proven. With this, it is confirmed that tensile strain favors the stabilization of a more reduced lattice, accompanied by greater segregation of strontium secondary phases and a decrease of oxygen exchange kinetics on LSMC thin films.
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Dec 2019
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I07-Surface & interface diffraction
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Diamond Proposal Number(s):
[17223]
Open Access
Abstract: Halide perovskites are emerging as valid alternatives to conventional photovoltaic active materials owing to their low cost and high device performances. This material family also shows exceptional tunability of properties by varying chemical components, crystal structure, and dimensionality, providing a unique set of building blocks for new structures. Here, highly stable self‐assembled lead–tin perovskite heterostructures formed between low‐bandgap 3D and higher‐bandgap 2D components are demonstrated. A combination of surface‐sensitive X‐ray diffraction, spatially resolved photoluminescence, and electron microscopy measurements is used to reveal that microstructural heterojunctions form between high‐bandgap 2D surface crystallites and lower‐bandgap 3D domains. Furthermore, in situ X‐ray diffraction measurements are used during film formation to show that an ammonium thiocyanate additive delays formation of the 3D component and thus provides a tunable lever to substantially increase the fraction of 2D surface crystallites. These novel heterostructures will find use in bottom cells for stable tandem photovoltaics with a surface 2D layer passivating the 3D material, or in energy‐transfer devices requiring controlled energy flow from localized surface crystallites to the bulk.
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Nov 2019
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I07-Surface & interface diffraction
|
Zahra
Andaji-garmaroudi
,
Mojtaba
Abdi-jalebi
,
Dengyang
Guo
,
Stuart
Macpherson
,
Aditya
Sadhanala
,
Elizabeth M.
Tennyson
,
Edoardo
Ruggeri
,
Miguel
Anaya
,
Krzysztof
Galkowski
,
Ravichandran
Shivanna
,
Kilian
Lohmann
,
Kyle
Frohna
,
Sebastian
Mackowski
,
Tom J.
Savenije
,
Richard H.
Friend
,
Samuel D.
Stranks
Diamond Proposal Number(s):
[17223]
Open Access
Abstract: Mixed‐halide lead perovskites have attracted significant attention in the field of photovoltaics and other optoelectronic applications due to their promising bandgap tunability and device performance. Here, the changes in photoluminescence and photoconductance of solution‐processed triple‐cation mixed‐halide (Cs0.06MA0.15FA0.79)Pb(Br0.4I0.6)3 perovskite films (MA: methylammonium, FA: formamidinium) are studied under solar‐equivalent illumination. It is found that the illumination leads to localized surface sites of iodide‐rich perovskite intermixed with passivating PbI2 material. Time‐ and spectrally resolved photoluminescence measurements reveal that photoexcited charges efficiently transfer to the passivated iodide‐rich perovskite surface layer, leading to high local carrier densities on these sites. The carriers on this surface layer therefore recombine with a high radiative efficiency, with the photoluminescence quantum efficiency of the film under solar excitation densities increasing from 3% to over 45%. At higher excitation densities, nonradiative Auger recombination starts to dominate due to the extremely high concentration of charges on the surface layer. This work reveals new insight into phase segregation of mixed‐halide mixed‐cation perovskites, as well as routes to highly luminescent films by controlling charge density and transfer in novel device structures.
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Sep 2019
|
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E01-JEM ARM 200CF
|
Diamond Proposal Number(s):
[16854]
Abstract: 2D crystals are typically uniform and periodic in‐plane with stacked sheet‐like structure in the out‐of‐plane direction. Breaking the in‐plane 2D symmetry by creating unique lattice structures offers anisotropic electronic and optical responses that have potential in nanoelectronics. However, creating nanoscale‐modulated anisotropic 2D lattices is challenging and is mostly done using top‐down lithographic methods with ≈10 nm resolution. A phase transformation mechanism for creating 2D striated lattice systems is revealed, where controlled thermal annealing induces Se loss in few‐layered PdSe2 and leads to 1D sub‐nm etched channels in Pd2Se3 bilayers. These striated 2D crystals cannot be described by a typical unit cells of 1–2 Å for crystals, but rather long range nanoscale periodicity in each three directions. The 1D channels give rise to localized conduction states, which have no bulk layered counterpart or monolayer form. These results show how the known family of 2D crystals can be extended beyond those that exist as bulk layered van der Waals crystals by exploiting phase transformations by elemental depletion in binary systems.
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Sep 2019
|
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Xiyang
Li
,
Shilei
Zhang
,
Hang
Li
,
Diego
Alba Venero
,
Jonathan S
White
,
Robert
Cubitt
,
Qingzhen
Huang
,
Jie
Chen
,
Lunhua
He
,
Gerrit
Van Der Laan
,
Wenhong
Wang
,
Thorsten
Hesjedal
,
Fangwei
Wang
Open Access
Abstract: A biskyrmion consists of two bound, topologically stable, skyrmion spin textures. These coffee‐bean‐shaped objects are observed in real space in thin plates using Lorentz transmission electron microscopy (LTEM). From LTEM imaging alone, it is not clear whether biskyrmions are surface‐confined objects, or, analogous to skyrmions in non-centrosymmetric helimagnets, 3D tube‐like structures in a bulk sample. Here, the biskyrmion form factor is investigated in single‐ and polycrystalline‐MnNiGa samples using small‐angle neutron scattering. It is found that biskyrmions are not long‐range ordered, not even in single crystals. Surprisingly all of the disordered biskyrmions have their in‐plane symmetry axis aligned along certain directions, governed by the magneto-crystalline anisotropy. This anisotropic nature of biskyrmions may be further exploited to encode information.
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Mar 2019
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I03-Macromolecular Crystallography
|
Diamond Proposal Number(s):
[7146]
Abstract: The development of extracellular matrix mimetics that imitate niche stem cell microenvironments and support cell growth for technological applications is intensely pursued. Specifically, mimetics are sought that can enact control over the self‐renewal and directed differentiation of human pluripotent stem cells (hPSCs) for clinical use. Despite considerable progress in the field, a major impediment to the clinical translation of hPSCs is the difficulty and high cost of large‐scale cell production under xeno‐free culture conditions using current matrices. Here, a bioactive, recombinant, protein‐based polymer, termed ZTFn, is presented that closely mimics human plasma fibronectin and serves as an economical, xeno‐free, biodegradable, and functionally adaptable cell substrate. The ZTFn substrate supports with high performance the propagation and long‐term self‐renewal of human embryonic stem cells while preserving their pluripotency. The ZTFn polymer can, therefore, be proposed as an efficient and affordable replacement for fibronectin in clinical grade cell culturing. Further, it can be postulated that the ZT polymer has significant engineering potential for further orthogonal functionalization in complex cell applications.
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Mar 2019
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