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result(s) for
"Harada, Takaaki"
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Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites
2017
The hot-phonon bottleneck effect in lead-halide perovskites (APbX
3
) prolongs the cooling period of hot charge carriers, an effect that could be used in the next-generation photovoltaics devices. Using ultrafast optical characterization and first-principle calculations, four kinds of lead-halide perovskites (A=FA
+
/MA
+
/Cs
+
, X=I
−
/Br
−
) are compared in this study to reveal the carrier-phonon dynamics within. Here we show a stronger phonon bottleneck effect in hybrid perovskites than in their inorganic counterparts. Compared with the caesium-based system, a 10 times slower carrier-phonon relaxation rate is observed in FAPbI
3
. The up-conversion of low-energy phonons is proposed to be responsible for the bottleneck effect. The presence of organic cations introduces overlapping phonon branches and facilitates the up-transition of low-energy modes. The blocking of phonon propagation associated with an ultralow thermal conductivity of the material also increases the overall up-conversion efficiency. This result also suggests a new and general method for achieving long-lived hot carriers in materials.
Slow cooling of hot charge carriers in lead halide perovskite could be used in photovoltaics devices. Here, Yang
et al
. study hot carrier dynamics by transient absorption spectroscopy. They relate the phonon bottleneck to the up-conversion of low-energy phonons, facilitated by the presence of organic cations.
Journal Article
Imaging the motion of electrons across semiconductor heterojunctions
by
Deckoff-Jones, Skylar
,
Krishna, M. Bala Murali
,
Winchester, Andrew
in
147/28
,
639/301/357/1018
,
639/4077/4072/4062
2017
The flow of photoexcited electrons in a type-II heterostructure can be imaged with energy, spatial and temporal resolution.
Technological progress since the late twentieth century has centred on semiconductor devices, such as transistors, diodes and solar cells
1
,
2
,
3
,
4
,
5
,
6
,
7
,
8
. At the heart of these devices is the internal motion of electrons through semiconductor materials due to applied electric fields
3
,
9
or by the excitation of photocarriers
2
,
4
,
5
,
8
. Imaging the motion of these electrons would provide unprecedented insight into this important phenomenon, but requires high spatial and temporal resolution. Current studies of electron dynamics in semiconductors are generally limited by the spatial resolution of optical probes, or by the temporal resolution of electronic probes. Here, by combining femtosecond pump–probe techniques with spectroscopic photoemission electron microscopy
10
,
11
,
12
,
13
, we imaged the motion of photoexcited electrons from high-energy to low-energy states in a type-II 2D InSe/GaAs heterostructure. At the instant of photoexcitation, energy-resolved photoelectron images revealed a highly non-equilibrium distribution of photocarriers in space and energy. Thereafter, in response to the out-of-equilibrium photocarriers, we observed the spatial redistribution of charges, thus forming internal electric fields, bending the semiconductor bands, and finally impeding further charge transfer. By assembling images taken at different time-delays, we produced a movie lasting a few trillionths of a second of the electron-transfer process in the photoexcited type-II heterostructure—a fundamental phenomenon in semiconductor devices such as solar cells. Quantitative analysis and theoretical modelling of spatial variations in the movie provide insight into future solar cells, 2D materials and other semiconductor devices.
Journal Article
Obtaining Cross-Sections of Paint Layers in Cultural Artifacts Using Femtosecond Pulsed Lasers
by
Hamm, James
,
Deckoff-Jones, Skylar
,
Dani, Keshav
in
art conservation
,
Continuous radiation
,
cross-section analysis
2017
Recently, ultrafast lasers exhibiting high peak powers and extremely short pulse durations have created a new paradigm in materials processing. The precision and minimal thermal damage provided by ultrafast lasers in the machining of metals and dielectrics also suggests a novel application in obtaining precise cross-sections of fragile, combustible paint layers in artwork and cultural heritage property. Cross-sections of paint and other decorative layers on artwork provide critical information into its history and authenticity. However, the current methodology which uses a scalpel to obtain a cross-section can cause further damage, including crumbling, delamination, and paint compression. Here, we demonstrate the ability to make controlled cross-sections of paint layers with a femtosecond pulsed laser, with minimal damage to the surrounding artwork. The femtosecond laser cutting overcomes challenges such as fragile paint disintegrating under scalpel pressure, or oxidation by the continuous-wave (CW) laser. Variations in laser power and translational speed of the laser while cutting exhibit different benefits for cross-section sampling. The use of femtosecond lasers in studying artwork also presents new possibilities in analyzing, sampling, and cleaning of artwork with minimal destructive effects.
Journal Article
Ultrafast Intrinsic Photoresponse and Direct Evidence of Sub-gap States in Liquid Phase Exfoliated MoS2Thin Films
2015
2-Dimensional structures with swift optical response have several technological advantages, for example they could be used as components of ultrafast light modulators, photo-detectors and optical switches. Here we report on the fast photo switching behavior of thin films of liquid phase exfoliated MoS
2
, when excited with a continuous laser of λ = 658 nm (E = 1.88 eV), over a broad range of laser power. Transient photo-conductivity measurements, using an optical pump and THz probe (OPTP), reveal that photo carrier decay follows a bi-exponential time dependence, with decay times of the order of picoseconds, indicating that the photo carrier recombination occurs via trap states. The nature of variation of photocurrent with temperature confirms that the trap states are continuously distributed within the mobility gap in these thin film of MoS
2
and play a vital role in influencing the overall photo response. Our findings provide a fundamental understanding of the photo-physics associated with optically active 2D materials and are crucial for developing advanced optoelectronic devices.
Journal Article
Total synthesis of gelsemoxonine
by
Yokoshima, Satoshi
,
Shimokawa, Jun
,
Fukuyama, Tohru
in
Aldehydes
,
alkaloid synthesis
,
Cyanides
2012
The first total synthesis of gelsemoxonine has been accomplished. A divinylcyclopropane–cycloheptadiene rearrangement of the highly functionalized substrate successfully assembled the spiro-quaternary carbon center connected to the bicyclic seven-membered core structure. A one-pot isomerization reaction of the α,β-unsaturated aldehyde to the saturated ester via a trimethylsilyl cyanide–diazabicycloundecene (TMSCN–DBU) reagent combination allowed a facile and diastereoselective introduction of the latent nitrogen functionality in the unique azetidine moiety.
Journal Article
Status of 48 Ca double beta decay search in CANDLES
2021
We study a strategy to reduce veto-time in the search for neutrino-less double-beta decay ( 0υββ ) with CANDLES-III system. We develop a new likelihood analysis and apply it to our new Run010 data. We show that we can increase the un-vetoed live-time by 11.8%. Thanks to this improvements, We expect to increase a limit on the life-time of 0υββ by a factor of three by analyzing both Run009 and Run010 data.
Journal Article
Terahertz frequency magnetoelectric effect in Ni doped CaBaCo\\(_4\\)O\\(_7\\)
by
Dhanasekhar, C
,
Mariserla, Bala M K
,
Deckoff-Jones, Skylar
in
Absorption spectra
,
Dependence
,
Electrons
2017
We present a study of terahertz frequency magnetoelectric effect in ferrimagnetic pyroelectric CaBaCo\\(_4\\)O\\(_7\\) and its Ni-doped variants. The terahertz absorption spectrum of these materials consists of spin excitations and low-frequency infrared-active phonons. We studied the magnetic-field-induced changes in the terahertz refractive index and absorption in magnetic fields up to 17 T. We find that the magnetic field modulates the strength of infrared-active optical phonons near 1.2 and 1.6 THz. We use the Lorentz model of the dielectric function to analyze the measured magnetic-field dependence of the refractive index and absorption. We propose that most of the magnetoelectric effect is contributed by the optical phonons near 1.6 THz and higher-frequency resonances. Our experimental results can be used to construct and validate more detailed theoretical descriptions of magnetoelectricity in CaBaCo\\(_{4-x}\\)Ni\\(_x\\)O\\(_7\\).
A primordial and reversible TCA cycle in a facultatively chemolithoautotrophic thermophile
by
Miyazaki, Masayuki
,
Mori, Koji
,
Shuto, Aya
in
Adenosine triphosphate
,
Anaerobic microorganisms
,
Bacteria
2018
Classically, it is thought that citrate synthase only works in one direction: to catalyze the production of citrate from acetyl coenzyme A and oxaloacetate in the tricarboxylic acid (TCA) cycle. The TCA cycle can run in reverse to cleave citrate and fix carbon dioxide autotrophically, but this was thought to occur only with alternative enzymes, such as citrate lyase. Now Nunoura et al. and Mall et al. have discovered thermophilic bacteria with highly efficient and reversible citrate synthase that requires reduced ferredoxin (see the Perspective by Ragsdale). This function is undetectable by metagenomics, but classical biochemistry filled in the gaps seen between the genome sequences and the phenotypes of the organisms. The direction of catalysis depends on the availability of organic versus inorganic carbon and reflects a flexible bet-hedging strategy for survival in fluctuating environments. In evolutionary terms, this capacity might predate the classical TCA cycle and is likely to occur in a wide range of anaerobic microorganisms. Science , this issue p. 559 , p. 563 ; see also p. 517 Classical biochemistry reveals the occurrence of an unexpected capacity to reverse the tricarboxylic acid cycle in anaerobic microbes. Inorganic carbon fixation is essential to sustain life on Earth, and the reductive tricarboxylic acid (rTCA) cycle is one of the most ancient carbon fixation metabolisms. A combination of genomic, enzymatic, and metabolomic analyses of a deeply branching chemolithotrophic Thermosulfidibacter takaii ABI70S6 T revealed a previously unknown reversible TCA cycle whose direction was controlled by the available carbon source(s). Under a chemolithoautotrophic condition, a rTCA cycle occurred with the reverse reaction of citrate synthase (CS) and not with the adenosine 5′-triphosphate–dependent citrate cleavage reactions that had been regarded as essential for the conventional rTCA cycle. Phylometabolic evaluation suggests that the TCA cycle with reversible CS may represent an ancestral mode of the rTCA cycle and raises the possibility of a facultatively chemolithomixotrophic origin of life.
Journal Article
Cell cycle arrest determines adult neural stem cell ontogeny by an embryonic Notch-nonoscillatory Hey1 module
2021
Quiescent neural stem cells (NSCs) in the adult mouse brain are the source of neurogenesis that regulates innate and adaptive behaviors. Adult NSCs in the subventricular zone are derived from a subpopulation of embryonic neural stem-progenitor cells (NPCs) that is characterized by a slower cell cycle relative to the more abundant rapid cycling NPCs that build the brain. Yet, how slow cell cycle can cause the establishment of adult NSCs remains largely unknown. Here, we demonstrate that Notch and an effector Hey1 form a module that is upregulated by cell cycle arrest in slowly dividing NPCs. In contrast to the oscillatory expression of the Notch effectors Hes1 and Hes5 in fast cycling progenitors, Hey1 displays a non-oscillatory stationary expression pattern and contributes to the long-term maintenance of NSCs. These findings reveal a novel division of labor in Notch effectors where cell cycle rate biases effector selection and cell fate.
Adult neural stem cells are derived from an embryonic population of slowcycling progenitor cells, though how reduced cycling speed leads to establishment of the adult population has remained elusive. Here they show that non-oscillatory Notch-Hey signaling induced by slow-cycling contributes to long term maintenance of neural stem cells.
Journal Article