318 research outputs found
Ultrafast heterogeneous electron transfer reactions Comparative theoretical studies on time and frequency domain data
Recent theoretical studies on linear absorption spectra of dye semiconductor systems perylene attached to nanostructured TiO2, L. Wang et al., J. Phys. Chem. B 109, 9589 2005 are extended here in different respects. Since the systems show ultrafast photoinduced heterogeneous electron transfer the time dependent formulation used to compute the absorbance is also applied to calculate the temporal evolution of the sub 100 fs charge injection dynamics after a 10 fs laser pulse excitation. These studies complement our recent absorption spectra fit for two perylene bridge anchor group TiO2 systems. Moreover, the time dependent formulation of the absorbance is confronted with a frequency domain description. The latter underlines the central importance of the self energy caused by the coupling of the dye levels to the semiconductor band continuum. The used model is further applied to study the effect of different parameters such as 1 the dependence on the reorganization energies of the involved intramolecular transitions, 2 the effect of changing the transfer integral which couples the excited dye state with the band continuum, and 3 the effect of the concrete form of the semiconductor band density of states. Emphasis is also put on the case where the charge injection level of the dye is near or somewhat below the band edge. This nicely demonstrates the change from a structureless absorption to a well resolved vibrational progression including characteristic shifts of the absorption lines which are a direct measure for the dye semiconductor couplin
An optical quasimonomer
A comprehensive investigation of the luminescent properties of carbon nitride
polymers, based on tri-s-triazine units, has been conducted. Steady-state
temperature- and excitation-power-dependent as well as time-resolved
measurements with near-UV excitation (λ=325 nm and 405 nm) yield strong
photoluminescence, covering the visible spectrum. The spectral, thermal, and
temporal features of the photoluminescence can be satisfactorily described by
the excitation and radiative recombination of molecular excitons, localized at
single tri-s-triazine units. The discussed model is in accordance with the
recently reported absorption features of carbon nitride polymers. Thus, from
the point of view of optical spectroscopy, the material effectively behaves as
a monomer
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Photophysics of polymeric carbon nitride: An optical quasimonomer
A comprehensive investigation of the luminescent properties of carbon nitride polymers, based on tri-s-triazine units, has been conducted. Steady-state temperature- and excitation-power-dependent as well as time-resolved measurements with near-UV excitation (λ=325 nm and 405 nm) yield strong photoluminescence, covering the visible spectrum. The spectral, thermal, and temporal features of the photoluminescence can be satisfactorily described by the excitation and radiative recombination of molecular excitons, localized at single tri-s-triazine units. The discussed model is in accordance with the recently reported absorption features of carbon nitride polymers. Thus, from the point of view of optical spectroscopy, the material effectively behaves as a monomer
Generalized Modeling of Photoluminescence Transients
Time resolved photoluminescence TRPL measurements and the extraction of meaningful parameters involve four key ingredients a suitable sample such as a semiconductor double heterostructure, a state of the art measurement setup, a kinetic model appropriate for the description of the sample behavior, and a general analysis method to extract the model parameters of interest from the measured TRPL transients. Until now, the last ingredient is limited to single curve fits, which are mostly based on simple models and least squares fits. These are often insufficient for the parameter extraction in real world applications. The goal of this article is to give the community a universal method for the analysis of TRPL measurements, which accounts for the Poisson distribution of photon counting events. The method can be used to fit multiple TRPL transients simultaneously using general kinematic models, but should also be used for single transient fits. To demonstrate this approach, multiple TRPL transients of a GaAs AlGaAs heterostructure are fitted simultaneously using coupled rate equations. It is shown that the simultaneous fits of several TRPL traces supplemented by systematic error estimations allow for a more meaningful and more robust parameter determination. The statistical methods also quantify the quality of the description by the underlying physical mode
On the benchmarking of multi-junction photoelectrochemical fuel generating devices
We discuss benchmarking considerations for multi-junction solar fuel absorbers and investigate the effects of spectral shaping by catalyst nanoparticles on design criteria.MMM acknowledges funding from the fellowship programme of the German National Academy of Sciences Leopoldina, grant LPDS 2015-09
Generalized Method to Extract Carrier Diffusion Length from Photoconductivity Transients Cases of BiVO4, Halide Perovskites, and Amorphous and Crystalline Silicon
Long diffusion lengths of photoexcited charge carriers are crucial for high power conversion efficiencies of photoelectrochemical and photovoltaic devices. Time resolved photoconductance measurements are often used to determine diffusion lengths in conventional semiconductors. However, effects such as polaron formation or multiple trapping can lead to time varying mobilities and lifetimes that are not accounted for in the conventional calculation of the diffusion length. Here, a generalized analysis is presented that is valid for time dependent mobilities and time dependent lifetimes. The diffusion length is determined directly from the integral of a photoconductivity transient and can be applied regardless of the nature of carrier relaxation. To demonstrate our approach, photoconductivity transients are measured from 100 fs to 1 s by the combination of time resolved terahertz and microwave spectroscopy for BiVO4, one of the most studied metal oxide photoanodes for photoelectrochemical water splitting. The temporal evolution of charge carrier displacement is monitored and converges after about 100 ns to a diffusion length of about 15 nm, which rationalizes the photocurrent loss in the corresponding photoelectrochemical device. The presented method is further validated on a amp; 8722;Si H, c amp; 8722;Si, and halide perovskite, which underlines its potential to determine the diffusion length in a wide range of semiconductors, including disordered material
3.9 day orbital modulation in the TeV gamma-ray flux and spectrum from the X-ray binary LS 5039
New observations of LS 5039, a High Mass X-ray Binary comprising a massive
star and compact object, were carried out with the High Energy Stereoscopic
System of Cherenkov Telescopes (H.E.S.S.) in 2005 at very high energy (VHE)
gamma-ray energies. These observations reveal that its flux and energy spectrum
are modulated with the 3.9 day orbital period of the binary system. This is the
first time in gamma-ray astronomy that orbital modulation has been observed,
and periodicity clearly established using ground-based gamma-ray detectors. The
VHE gamma-ray emission is largely confined to half of the orbit, peaking around
the inferior conjunction epoch of the compact object. For this epoch, there is
also a hardening of the energy spectrum in the energy range between 0.2 TeV and
a few TeV. The flux vs. orbital phase profile provides the first clear
indication of gamma-ray absorption via pair production within an astrophysical
source, a process which is expected to occur if the gamma-ray production site
is situated within ~1 AU of the compact object. Moreover the production region
size must be not significantly greater than the binary separation (~0.15 AU).
Notably, these constraints are also considerably smaller than the collimated
outflows or jets (extending out to ~1000 AU) observed in LS 5039. The spectral
hardening could arise from variations with phase in the maximum electron
energies, and/or the dominant VHE gamma-ray production mechanism.Comment: 8 pages, 8 figures, accepted for publication in Astronomy &
Astrophysic
H.E.S.S. observations of gamma-ray bursts in 2003-2007
Very-high-energy (VHE; >~100 GeV) gamma-rays are expected from gamma-ray
bursts (GRBs) in some scenarios. Exploring this photon energy regime is
necessary for understanding the energetics and properties of GRBs. GRBs have
been one of the prime targets for the H.E.S.S. experiment, which makes use of
four Imaging Atmospheric Cherenkov Telescopes (IACTs) to detect VHE gamma-rays.
Dedicated observations of 32 GRB positions were made in the years 2003-2007 and
a search for VHE gamma-ray counterparts of these GRBs was made. Depending on
the visibility and observing conditions, the observations mostly start minutes
to hours after the burst and typically last two hours. Results from
observations of 22 GRB positions are presented and evidence of a VHE signal was
found neither in observations of any individual GRBs, nor from stacking data
from subsets of GRBs with higher expected VHE flux according to a
model-independent ranking scheme. Upper limits for the VHE gamma-ray flux from
the GRB positions were derived. For those GRBs with measured redshifts,
differential upper limits at the energy threshold after correcting for
absorption due to extra-galactic background light are also presented.Comment: 9 pages, 4 tables, 3 figure
Discovery of VHE gamma-rays from the high-frequency-peaked BL Lac object RGB J0152+017
Aims: The BL Lac object RGB J0152+017 (z=0.080) was predicted to be a very
high-energy (VHE; > 100 GeV) gamma-ray source, due to its high X-ray and radio
fluxes. Our aim is to understand the radiative processes by investigating the
observed emission and its production mechanism using the High Energy
Stereoscopic System (H.E.S.S.) experiment. Methods: We report recent
observations of the BL Lac source RGB J0152+017 made in late October and
November 2007 with the H.E.S.S. array consisting of four imaging atmospheric
Cherenkov telescopes. Contemporaneous observations were made in X-rays by the
Swift and RXTE satellites, in the optical band with the ATOM telescope, and in
the radio band with the Nancay Radio Telescope. Results: A signal of 173
gamma-ray photons corresponding to a statistical significance of 6.6 sigma was
found in the data. The energy spectrum of the source can be described by a
powerlaw with a spectral index of 2.95+/-0.36stat+/-0.20syst. The integral flux
above 300 GeV corresponds to ~2% of the flux of the Crab nebula. The source
spectral energy distribution (SED) can be described using a two-component
non-thermal synchrotron self-Compton (SSC) leptonic model, except in the
optical band, which is dominated by a thermal host galaxy component. The
parameters that are found are very close to those found in similar SSC studies
in TeV blazars. Conclusions: RGB J0152+017 is discovered as a source of VHE
gamma-rays by H.E.S.S. The location of its synchrotron peak, as derived from
the SED in Swift data, allows clearly classification it as a
high-frequency-peaked BL Lac (HBL).Comment: Accepted for publication in A&A Letters (5 pages, 4 figures
The exceptionally powerful TeV gamma-ray emitters in the Large Magellanic Cloud
The Large Magellanic Cloud, a satellite galaxy of the Milky Way, has been
observed with the High Energy Stereoscopic System (H.E.S.S.) above an energy of
100 billion electron volts for a deep exposure of 210 hours. Three sources of
different types were detected: the pulsar wind nebula of the most energetic
pulsar known N 157B, the radio-loud supernova remnant N 132D and the largest
non-thermal X-ray shell - the superbubble 30 Dor C. The unique object SN 1987A
is, surprisingly, not detected, which constrains the theoretical framework of
particle acceleration in very young supernova remnants. These detections reveal
the most energetic tip of a gamma-ray source population in an external galaxy,
and provide via 30 Dor C the unambiguous detection of gamma-ray emission from a
superbubble.Comment: Published in Science Magazine (Jan. 23, 2015). This ArXiv version has
the supplementary online material incorporated as an appendix to the main
pape
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