Based on earlier results on the photocatalytic properties of MoS2, the 1T form of MoSe2, prepared by lithium intercalation and exfoliation of bulk MoSe2, has been employed for the visible-light induced generation of hydrogen. 1T-MoSe2 is found to be superior to both 2H and 1T MoS2 as well as 2H-MoSe2 in producing hydrogen from water, the yield being in the 60–75 mmol h−1 g−1 range with a turn over frequency of 15–19 h−1. First principles calculations reveal that 1T-MoSe2 has a lower work function than 2H-MoSe2 as well as 1T and 2H-MoS2, making it easier to transfer an electron from 1T-MoSe2 for the production of H2.
The recent discovery of non-saturating giant positive magnetoresistance has aroused much interest in Td-WTe(2). We have investigated structural, electronic and vibrational properties of bulk and few-layer Td-WTe(2) experimentally and theoretically. Spin-orbit coupling is found to govern the semi-metallic character of Td-WTe(2) and its structural link with the metallic 1 T form provides an understanding of its structural stability. There is a metal-to-insulator switch-over in the electrical conductivity and a change in the sign of the Seebeck coefficient around 373 K. Lattice vibrations of Td-WTe(2) have been analyzed using first-principles calculations. Out of the 33 possible zone-center Raman active modes, five distinct Raman bands are observed around 112, 118, 134, 165 and 212 cm(-1) in bulk Td-WTe(2). Based on symmetry analysis and calculated Raman tensors, we assign the intense bands at 165 cm(-1) and 212 cm(-1) to the A'(1)and A''(1) modes, respectively. Most of the Raman bands stiffen with decreasing thickness, and the ratio of the integrated intensities of the A''(1) to A'(1) bands decreases in the few-layer sample, while all the bands soften in both the bulk and few-layer samples with increasing temperature.
The nature of the transient species leading to emission from the spin/orbital-forbidden Mn d−d transition in doped semiconductor quantum dots has intrigued scientists for a long time. This understanding is important in the quest for energy efficiency as the energy from the conduction band is transferred efficiently to Mn in the femtosecond time scale overcoming other nonradiative recombination pathways. In this work, we have shown the presence of the transient species using materials with band gaps in resonance with the energy of the Mn emission to understand the nature of the absorbing, transient, and emitting species. Detailed studies lead to the emergence of a transient Mn 3+ state that is further corroborated with spin-dependent density functional theory calculations. This opens up a unique opportunity to realize a reversible photochemical reaction and high radiative efficiency in a semiconductor nanostructure by controlling the spin state of the magnetic ion by external illumination.
REPORT DOCUMENTATION PAGEForm maintaining the data needed, and completing and reviewing this collection of information. Send comments regarding this burden estimate or any other aspect of this collection of information ind udings uggestons for reducin g Ws burden to Department of Defense. Washington Headquarters Services, Directorate for Information Operations and Reports (0704-0188), 1215 Jefferson Davis Highway, Suite 1204, Arlington W 22202-4302 Respondents should be aware that notwithstanding any other provision of law, no person shall be subject to any penalty for failing to comply with a collection of information if ,t does not display a currently valid OMB control number. PLEASE DO NOT RETURN YOUR FORM TO THE ABOVE ADDRESS. 05-05-2000 REPORT DATE (DD-MM-YYYY) REPORT TYPE Journal Article TITLE AND SUBTITLE640x486 Long-Wavelength Two-Color GaAs/AlGaAs Quantum Well Infrared Photodetector (QWIP) Focal Plane Array Camera AUTHOR(S)Gunapala SD, Bandara SV, Singh A, Liu JK, Rafol SB, Luong EM, Mumolo JM, Tran NQ, Ting DZY, Vincent JD, Shott CA, Long J, LeVan PD PERFORMING ORGANIZATION NAME(S) AND ADDRESS(ES)Air Force Research Laboratory 3 55 0 Aberdeen Ave. SE Kirtland AFB, NM 87117-5776 SPONSORING / MONITORING AGENCY NAME(S) AND ADDRESS(ES) DISTRIBUTION /AVAILABILITYSTATEMENTApproved for Public Release; Distribution is Unlimited. SUPPLEMENTARY NOTES DATES COVERED (From SPONSOR/MONITOR'S ACRONYM(S) SPONSOR/MONITOR'S REPORT NUMBER(S) 20021212 120We have designed and fabricated an optimized long-wavelength/very-long-wavelength two-color quantum well infrared photodetector (QWIP) device structure. The device structure was grown on a 3-in semiinsulating GaAs substrate by molecular beam epitaxy (MBE). The wafer was processed into several 640 x 486 format monolithically integrated 8-9 and 14-15 ßm two-color (or dual wavelength) QWIP focal plane arrays (FPA's). These FPA's were then hybridized to 640 x 486 silicon CMOS readout multiplexers. A thinned (i.e., substrate removed) FPA hybrid was integrated into liquid helium cooled dewar for electrical and optical characterization and to demonstrate simultaneous two-color imagery. The 8-9 /im detectors in the FPA have shown background limited performance (BLIP) at 70 K operating temperature for 300 K background with f/2 cold stop. The 14-15 /mi detectors of the FPA reach BLIP at 40 K operating temperature under the same background conditions. In this paper we discuss the performance of this long-wavelength dualband QWIP FPA in terms of quantum efficiency, detectivity, noise equivalent temperature difference (NE A T), uniformity, and operability. Abstract-We have designed and fabricated an optimized long-wavelength/very-long-wavelength two-color quantum well infrared photodetector (QWIP) device structure. The device structure was grown on a 3-in semi-insulating GaAs substrate by molecular beam epitaxy (MBE). The wafer was processed into several 640 x 486 format monolithically integrated 8-9 and 14-15 /im two-color (or dual wavelength) QWIP focal plane arrays (FPA's). Th...
We report high pressure Raman experiments of Black phosphorus (BP) up to 24 GPa. The line widths of first order Raman modes A 1 g , B2g and A 2 g of the orthorhombic phase show a minimum at 1.1 GPa. Our first-principles density functional analysis reveals that this is associated with the anomalies in electron-phonon coupling at the semiconductor to topological insulator transition through inversion of valence and conduction bands marking a change from trivial to nontrivial electronic topology. The frequencies of B2g and A 2 g modes become anomalous in the rhombohedral phase at 7.4 GPa, and new modes appearing in the rhombohedral phase show anomalous softening with pressure. This is shown to originate from unusual structural evolution of black phosphorous with pressure, based on first-principles theoretical analysis.
Among the 1H and 1T structures exhibited by monolayers of transition metal dichalcogenides, the group VI compounds MX 2 (M = Mo, W and X = S, Se) largely occur in the 1H form. Recently, transformation of the 1H form to the 1T form with metallic electronic structure at high temperatures was demonstrated in MoS 2 with Re substitution and electron irradiation by Lin et al (2014 Nat. Nanotechnology 9 391). Here, we use first-principles calculations to determine the energy landscape associated with the 1H to 1T phase transition, predict novel 1T structures and relate the observed by Lin et al (2014 Nat. Nanotechnology 9 391) intermediate structures to structural instabilities of the 1T structure of MX 2 compounds. We show that the metallic centrosymmetric 1T (c 1T ) structure of these compounds is unstable with respect to dimerization or trimerization of metal atoms, leading to a competing metallic 3 1 × 1T form and ferroelectric semiconducting 3 3 × 1T form respectively. While the former is a more stable 1T form of MoSe 2 , WS 2 and WSe 2 , the latter is a more stable 1T form of MoS 2 exhibiting rich ferroelectric dipolar domain structure. In the vicinity of metalsemiconductor transitions, their semiconducting forms are shown to exhibit an anomalous response to electric fields. To facilitate the experimental verification of these subtle features of the 1T forms of MX 2 monolayers, we present comparative analysis of their vibrational properties, and identify their Raman and infra-red spectroscopic signatures.
High pressure Raman spectroscopy of bulk 2H-MoTe 2 upto ∼ 29 GPa is shown to reveal two phase transitions (at ∼ 6 and 16.5 GPa), which are analyzed using first-principles density functional theoretical calculations. The transition at 6 GPa is marked by changes in the pressure coefficients of A 1g and E 1 2g Raman mode frequencies as well as in their relative intensity. Our calculations show that this is an isostructural semiconductor to a semimetal transition. The transition at ∼ 16.5 GPa is identified with the changes in linewidths of the Raman modes as well as in the pressure coefficients of their frequencies. Our theoretical analysis clearly shows that the structure remains the same upto 30 GPa. However, the topology of the Fermi-surface evolves as a function of pressure, and abrupt appearance of electron and hole pockets at P ∼ 20 GPa marks a Lifshitz transition. a electronic mail:asood@physics.iisc.ernet.in
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