2020 New's Items

Autocorrected off-axis holography of two-dimensional materials

Felix Kern
Martin Linck
Daniel Wolf
Nasim Alem
Himani Arora
Sibylle Gemming
Artur Erbe
Alex Zettl
Bernd Buchner
Axel Lubk
2020

The reduced dimensionality in two-dimensional materials leads to a wealth of unusual properties, which are currently explored for both fundamental and applied sciences. In order to study the crystal structure, edge states, the formation of defects and grain boundaries, or the impact of adsorbates, high-resolution microscopy techniques are indispensable. Here we report on the development of an electron holography (EH) transmission electron microscopy (TEM) technique, which facilitates high spatial resolution by an automatic correction of geometric aberrations. Distinguished features...

The Reticular Chemist

Yaghi OM
2020

A new chemist is emerging to extend chemistry from the atom and the molecule to the framework and to meet the new intellectual and practical challenges of the 21st centur.

Competition between magnetic order and charge localization in Na 2 IrO 3 thin crystal devices

Rodriguez J
Lopez G
Ramirez F
Breznay NP
Kealhofer R
Nagarajan V
Latzke D
Wilson S
Marrufo N
Santiago P
Lara J
Diego A
Molina E
Rosser D
Tavassol H
Lanzara A
Analytis JG
Ojeda-Aristizabal C
2020

Spin orbit assisted Mott insulators such as sodium iridate (Na2IrO3) have been an important subject of study in recent years. In these materials, the interplay of electronic correlations, spin-orbit coupling, crystal field effects, and a honeycomb arrangement of ions bring exciting ground states, predicted in the frame of the Kitaev model....

Sequencing of metals in multivariate metal-organic frameworks

Ji Z
Li T
Yaghi OM
2020

We mapped the metal sequences within crystals of metal-oxide rods in multivariate metal-organic framework-74 containing mixed combinations of cobalt (Co), cadmium (Cd), lead (Pb), and manganese (Mn). Atom probe tomography of these crystals revealed the presence of heterogeneous spatial sequences of metal ions that we describe, depending on the metal and synthesis temperature used, as random (Co, Cd, 120°C), short duplicates (Co, Cd, 85°C), long duplicates (Co, Pb, 85°C), and insertions (Co, Mn, 85°C). Three crystals were examined for each sequence type, and the molar fraction of Co among...

Two-Dimensional Electronic–Vibrational Spectroscopy Reveals Cross-Correlation between Solvation Dynamics and Vibrational Spectral Diffusion

Cho M
Fleming GR
2020

Two-dimensional electronic–vibrational spectroscopy (2DEVS) is a useful technique for studying the structure and dynamics of photoexcited molecules via monitoring of the vibrational spectrum in real-time. However, quantitative modeling or prediction of experimental spectra has been hampered by the lack of a firm theoretical basis for this quantity. Here, we develop a useful theory of 2DEVS and show that the time-dependent line shape of the 2DEVS spectrum provides invaluable information on the cross-correlation function of the solvation dynamics and vibrational spectral diffusion. The...

The role of mixed vibronic Qy-Qx states in green light absorption of light-harvesting complex II

Arsenault EA
Yoneda Y
Iwai M
Niyogi K
Fleming GR
2020

The importance of green light for driving natural photosynthesis has long been underappreciated, however, under the presence of strong illumination, green light actually drives photosynthesis more efficiently than red light. This green light is absorbed by mixed vibronic Qy-Qx states, arising from chlorophyll (Chl)-Chl interactions, although almost nothing is known about these states. Here, we employ polarization-dependent two-dimensional electronic-vibrational spectroscopy to study the origin and dynamics of the mixed vibronic Q...

Structural and spectral dynamics of single-crystalline Ruddlesden-Popper phase halide perovskite blue light-emitting diodes

Chen H
Lin J
Kang J
Kong Q
Lu D
Kang J
Lai M
Quan Li N
Lin Z
Jin J
Wang L-w
Toney Michael F
Yang P
2020

Achieving perovskite-based high–color purity blue-emitting light-emitting diodes (LEDs) is still challenging. Here, we report successful synthesis of a series of blue-emissive two-dimensional Ruddlesden-Popper phase single crystals and their high–color purity blue-emitting LED demonstrations. Although this approach successfully achieves a series of bandgap emissions based on the different layer thicknesses, it still suffers from a conventional temperature-induced device degradation mechanism during high-voltage operations. To understand the underlying mechanism, we further elucidate...

Two-Step Patterning of Scalable All-Inorganic Halide Perovskite Arrays

Lin C-K
Zhao Q
Zhang Y
Cestellos-Blanco S
Kong Q
Lai M
Kang J
Yang P
2020

Halide perovskites have many important optoelectronic properties, including high emission efficiency, high absorption coefficients, color purity, and tunable emission wavelength, which makes these materials promising for optoelectronic applications. However, the inability to precisely control large-scale patterned growth of halide perovskites limits their potential toward various device applications. Here, we report a patterning method for the growth of a cesium lead halide perovskite single crystal array. Our approach consists of two steps: (1) cesium halide salt arrays patterning...

High-Performance Pt–Co Nanoframes for Fuel-Cell Electrocatalysis

Chen S
Li M
Gao M
Jin J
Van Spronsen MA
Salmeron MB
Yang P
2020

Pt-based alloy catalysts are promising candidates for fuel-cell applications, especially for cathodic oxygen reduction reaction (ORR) and anodic methanol oxidation reaction (MOR). The rational design of composition and morphology is crucial to promoting catalytic performances. Here, we report the synthesis of Pt–Co nanoframes via chemical etching of Co from solid rhombic dodecahedra. The obtained Pt–Co nanoframes exhibit excellent ORR mass activity in acidic electrolyte, which is as high as 0.40 A mgPt–1 initially and 0.34 A mgPt...

Morphology-controlled transformation of Cu@Au core-shell nanowires into thermally stable Cu3Au intermetallic nanowires

Niu Z
Chen S
Yu Y
Lei T
Dehestani A
Schierle-Arndt K
Yang P
2020

Multimetallic nanowires with long-range atomic ordering hold the promise of unique physicochemical properties in many applications. Here we demonstrate the synthesis and study the stability of Cu3Au intermetallic nanowires. The synthesis is achieved by using Cu@Au core-shell nanowires as precursors. With appropriate Cu/Au stoichiometry, the Cu@Au core-shell nanowires are transformed into fully ordered Cu3Au nanowires under thermal annealing. Thermally-driven atom diffusion accounts for this transformation as revealed by X-ray...