B16-Test Beamline
Optics
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Abstract: A high stability Double Crystal Monochromator has been developed at The Diamond Light Source for beamlines I09 and I23. The design specification was a cryogenic, fixed exit, energy scanning monochromator, operating over an energy range of 2.1 – 25 keV using a Si(111) crystal set. The novel design concepts are the direct drive, air bearing Bragg axis, low strain crystal mounts and the cooling scheme. The instrument exhibited superb stability and repeatability on the B16 Test Beamline. A 20 keV Si(555), 1.4 ?rad rocking curve was demonstrated. The DCM showed good stability without any evidence of vibration or Bragg angle nonlinearity.
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Mar 2013
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NONE-No attached Diamond beamline
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Abstract: Zeolites are microporous crystalline materials that find wide application in industry, for example, as catalysts and gas separators, and in our daily life, for example, as adsorbents or as ion exchangers in laundry detergents1. The tetrahedrally coordinated silicon and aluminium atoms in the zeolite unit cell occupy the so-called crystallographic T-sites. Besides their pore size, the occupation of specific T-sites by the aluminium atoms determines the performance of the zeolites2. Despite its importance, the distribution of aluminium over the crystallographic T-sites remains one of the most challenging, unresolved issues in zeolite science. Here, we report how to determine unambiguously and directly the distribution of aluminium in zeolites by means of the X-ray standing wave technique3 using brilliant, focused X-rays from a third-generation synchrotron source. We report in detail the analysis of the aluminium distribution in scolecite, which demonstrates how the aluminium occupancy in zeolites can systematically be determined.
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Jun 2008
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Abstract: The formation of a quasi-2dimensional electron gas at interface of SrTiO3 (STO) and LaAlO3 (LAO) attracted considerable attention in the recent years. The polar LAO layer was expected to cause the build-up of an electric potential. Distortions in the overlayer are discussed as one possible response of the system. The highly sensitive X-ray standing wave (XSW) imaging technique is well suited to study theses films because of its chemical and spacial resolution. LAO thin films below and above the critical thickness for conductivity were studied at the hard X-ray photo electron spectroscopy end station of ID32 at the ESRF. The XSW modulated core level photo electron yield was recorded for the five elements present in film and substrate for seven different Bragg reflections. Subsequent analysis provided for each reflection and element the amplitude and phase of one Fourier coefficient of the elemental atomic distribution function. The three dimensional real space image of the atomic distribution for each of the elements is reconstructed by direct Fourier inversion. The reconstructed 3D images obtained by this model free approach reveal significant atomic displacements.
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Mar 2012
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I09-Surface and Interface Structural Analysis
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P. T. P.
Ryan
,
Z.
Jakub
,
J.
Balajka
,
J.
Hulva
,
M.
Meier
,
J. T.
Kuchle
,
P. J.
Blowey
,
P. K.
Thakur
,
C.
Franchini
,
D. J.
Payne
,
D. P.
Woodruff
,
L. A.
Rochford
,
F.
Allegretti
,
T.-l.
Lee
,
G. S.
Parkinson
,
D. A.
Duncan
Diamond Proposal Number(s):
[16403, 18191, 13817]
Open Access
Abstract: The normal incidence X-ray standing wave (NIXSW) technique has been used to follow the evolution of the adsorption geometry of Ni adatoms on the Fe3O4(001)-(√2 × √2)R45° surface as a function of temperature. Two primary surface region sites are identified: a bulk-continuation tetrahedral site and a sub-surface octahedral site, the latter site being preferred at higher annealing temperatures. The ease of incorporation is linked to the presence of subsurface cation vacancies in the (√2 × √2)R45° reconstruction and is consistent with the preference for octahedral coordination observed in the spinel compound NiFe2O4.
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Jun 2018
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I09-Surface and Interface Structural Analysis
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Sebastian A.
Howard
,
Christopher N.
Singh
,
Galo J.
Paez
,
Matthew
Wahila
,
Linda W.
Wangoh
,
Shawn
Sallis
,
Keith
Tirpak
,
Yufeng
Liang
,
David
Prendergast
,
Mateusz
Zuba
,
Jatinkumar
Rana
,
Alex
Weidenbach
,
Timothy M.
Mccrone
,
Wanli
Yang
,
Tien-lin
Lee
,
Fanny
Rodolakis
,
William
Doolittle
,
Wei-cheng
Lee
,
Louis F. J.
Piper
Diamond Proposal Number(s):
[20647]
Open Access
Abstract: The discovery of analog LixNbO2 memristors revealed a promising new memristive mechanism wherein the diffusion of Li+ rather than O2− ions enables precise control of the resistive states. However, directly correlating lithium concentration with changes to the electronic structure in active layers remains a challenge and is required to truly understand the underlying physics. Chemically delithiated single crystals of LiNbO2 present a model system for correlating lithium variation with spectroscopic signatures from operando soft x-ray spectroscopy studies of device active layers. Using electronic structure modeling of the x-ray spectroscopy of LixNbO2 single crystals, we demonstrate that the intrinsic memristive behavior in LixNbO2 active layers results from field-induced degenerate p-type doping. We show that electrical operation of LixNbO2-based memristors is viable even at marginal Li deficiency and that the analog memristive switching occurs well before the system is fully metallic. This study serves as a benchmark for material synthesis and characterization of future LixNbO2-based memristor devices and suggests that valence change switching is a scalable alternative that circumvents the electroforming typically required for filamentary-based memristors.
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Jul 2019
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I09-Surface and Interface Structural Analysis
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Peter
Deimel
,
Reda M.
Bababrik
,
Bin
Wang
,
Philip
Blowey
,
Luke
Rochford
,
Pardeep K.
Thakur
,
Tien-lin
Lee
,
Marie-laure
Bocquet
,
Johannes V.
Barth
,
Phil
Woodruff
,
David
Duncan
,
Francesco
Allegretti
Diamond Proposal Number(s):
[8940]
Open Access
Abstract: The strong parallels between coordination chemistry and adsorption on metal surfaces, with molecules and ligands forming local bonds to individual atoms within a metal surface, have been established over many years of study. The recently proposed “surface trans-effect” (STE) appears to be a further manifestation of this analogous behaviour, but so far the true nature of the modified molecule–metal surface bonding has been unclear. The STE could play an important role in determining the reactivities of surface-supported metal–organic complexes, influencing the design of systems for future applications. However, the current understanding of this effect is incomplete and lacks reliable structural parameters with which to benchmark theoretical calculations. Using X-ray standing waves, we demonstrate that ligation of ammonia and water to iron phthalocyanine (FePc) on Ag(111) increases the adsorption height of the central Fe atom; dispersion corrected density functional theory calculations accurately model this structural effect. The calculated charge redistribution in the FePc/H2O electronic structure induced by adsorption shows an accumulation of charge along the σ-bonding direction between the surface, the Fe atom and the water molecule, similar to the redistribution caused by ammonia. This apparent σ-donor nature of the observed STE on Ag(111) is shown to involve bonding to the delocalised metal surface electrons rather than local bonding to one or more surface atoms, thus indicating that this is a true surface trans-effect.
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Jun 2016
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I09-Surface and Interface Structural Analysis
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Diamond Proposal Number(s):
[9717, 12044, 11394, 14432, 15455]
Abstract: More than a decade after the discovery of the two-dimensional electron system (2DES) at the interface between the band insulators
LaAlO
3
(LAO) and
SrTiO
3
(STO) its microscopic origin is still under debate. Several explanations have been proposed, the main contenders being electron doping by oxygen vacancies and electronic reconstruction, i.e., the redistribution of electrons to the interface to minimize the electrostatic energy in the polar LAO film. However, no experiment thus far could provide unambiguous information on the microscopic origin of the interfacial charge carriers. Here we utilize a novel experimental approach combining photoelectron spectroscopy (PES) with highly brilliant synchrotron radiation and apply it to a set of samples with varying key parameters that are thought to be crucial for the emergence of interfacial conductivity. Based on microscopic insight into the electronic structure, we obtain results tipping the scales in favor of polar discontinuity as a generic, robust driving force for the 2DES formation. Likewise, other functionalities such as magnetism or superconductivity might be switched in all-oxide devices by polarity-driven charge transfer.
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May 2017
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I09-Surface and Interface Structural Analysis
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Chiara
Bigi
,
Zhenkun
Tang
,
Gian Marco
Pierantozzi
,
Pasquale
Orgiani
,
Pranab Kumar
Das
,
Jun
Fujii
,
Ivana
Vobornik
,
Tommaso
Pincelli
,
Alessandro
Troglia
,
Tien-lin
Lee
,
Regina
Ciancio
,
Goran
Drazic
,
Alberto
Verdini
,
Anna
Regoutz
,
Phil D. C.
King
,
Deepnarayan
Biswas
,
Giorgio
Rossi
,
Giancarlo
Panaccione
,
Annabella
Selloni
Diamond Proposal Number(s):
[16041]
Abstract: Two-dimensional (2D) metallic states induced by oxygen vacancies (
V
O
s
) at oxide surfaces and interfaces provide opportunities for the development of advanced applications, but the ability to control the behavior of these states is still limited. We used angle resolved photoelectron spectroscopy combined with density-functional theory (DFT) to study the reactivity of
V
O
-induced states at the (001) surface of anatase
TiO
2
, where both 2D metallic and deeper lying in-gap states (IGs) are observed. The 2D and IG states exhibit remarkably different evolutions when the surface is exposed to molecular
O
2
: while IGs are almost completely quenched, the metallic states are only weakly affected. DFT calculations indeed show that the IGs originate from surface
V
O
s
and remain localized at the surface, where they can promptly react with
O
2
. In contrast, the metallic states originate from subsurface vacancies whose migration to the surface for recombination with
O
2
is kinetically hindered on anatase
TiO
2
(001), thus making them much less sensitive to oxygen dosing.
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Feb 2020
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I09-Surface and Interface Structural Analysis
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Nan
Yang
,
Alex
Belianinov
,
Evgheni
Strelcov
,
Antonello
Tebano
,
Vittorio
Foglietti
,
Daniele
Di Castro
,
Christoph
Schlueter
,
Tien-lin
Lee
,
Arthur P.
Baddorf
,
Nina
Balke
,
Stephen
Jesse
,
Sergei V.
Kalinin
,
Giuseppe
Balestrino
,
Carmela
Aruta
Diamond Proposal Number(s):
[9221]
Abstract: A systematic study by reversible and hysteretic electrochemical strain microscopy (ESM) in samples of cerium oxide with different Sm content and in several working conditions allows disclosing the microscopic mechanism underlying the difference in electrical conduction mechanism and related surface activity, such as water adsorption and dissociation with subsequent proton liberation. We have measured the behavior of the reversible hysteresis loops by changing temperature and humidity, both in standard ESM configuration and using the first-order reversal curve method. The measurements have been performed in much smaller temperature ranges with respect to alternative measuring techniques. Complementing our study with hard X-ray photoemission spectroscopy and irreversible scanning probe measurements, we find that water incorporation is favored until the doping with Sm is too high to allow the presence of Ce3+. The influence of doping on the surface reactivity clearly emerges from all of our experimental results. We find that at lower Sm concentration, proton conduction is prevalent, featured by lower activation energy and higher electrical conductivity. Defect concentrations determine the type of the prevalent charge carrier in a doping dependent manner.
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Dec 2014
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I09-Surface and Interface Structural Analysis
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N.
Yang
,
E.
Strelcov
,
A.
Belianinov
,
Antonello
Tebano
,
V.
Foglietti
,
Christoph
Schlueter
,
Tien-lin
Lee
,
S.
Jesse
,
S. V.
Kalinin
,
G.
Balestrino
,
Carmela
Aruta
Abstract: Water adsorption, splitting, and proton liberation were investigated on Sm0.1Ce0.9O2-δ thin films by scanning probe microscopy. An irreversible volume expansion was observed by applying a positive bias with increased temperature. The volume expansion is also linearly dependent on the relative humidity. A reversible water adsorption process and its effect on the conductivity were also investigated by electrochemical strain microscopy and first order reversal curve under a number of experiment conditions. The presence of a Ce3+ along with OH groups, detected by hard x-ray photoemission spectroscopy established a clear correlation between the water incorporation and the valence state of Ce.
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Oct 2015
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