127 research outputs found
Photoexcitation dynamics in regioregular and regiorandom polythiophene films
Journal ArticleUsing a variety of optical probes techniques we studied the photoexcitation dynamics in thin films of poly-3-hexyl thiophene with regioregular order that forms lamellae structures with increased interchain interaction, as well as regiorandom order that keeps a chainlike morphology. In regiorandom films we found that intrachain excitons with correlated induced absorption and stimulated emission bands are the primary excitations; they give rise to a moderately strong photoluminescence band. In regioregular films, on the contrary, we found that the primary excitations are excitons with a much larger interchain component; this results in lack of stimulated emission, vanishing intersystem crossing, and very weak photoluminescence band. In regioregular films we also measured photogenerated geminate polaron pairs with ultrafast dynamics that are precursor to long-lived polaron excitations
Ultrafast spectroscopy of excitons in single-walled carbon nanotubes
Journal ArticleWe studied the femtosecond dynamics of photoexcitations in films containing semiconducting and metallic single-walled carbon nanotubes (SWNTs), using various pump-probe wavelengths and intensities.We found that confined excitons and charge carriers with subpicosecond dynamics dominate the ultrafast response in semiconducting and metallic SWNTs, respectively. Surprisingly, we also found from the exciton excited state absorption bands and multiphoton absorption resonances in the semiconducting nanotubes that transitions between subbands are allowed; this unravels the important role of electron-electron interaction in SWNT optics
Ultrafast dynamics of excitons and solitons in disubstituted polyacetylene
Journal ArticleWe studied the ultrafast photoexcitation dynamics in disubstituted polyacetylene (DPA). We found two distinctively different relaxation channels for the photogenerated excitons; ionic and covalent pathways. In DPA films the photogenerated odd-parity (Bu) excitons that are responsible for the high photoluminescence quantum efficiency follow the ionic relaxation pathway. During the hot exciton thermalization process, however, a fraction of the Bu excitons undergo a phonon-assisted transition to the covalent 2Ag state, which consequently decomposes into two neutral soliton-antisoliton pairs that are subject to ultrafast recombination or dissociate into stable neutral solitons. In DPA solutions the ionic channel remains unchanged, however, the covalent channel becomes ineffective due to the different hot exciton thermalization pathways
Investigating the retention of intermediate-mass black holes in star clusters using N-body simulations
Contrary to supermassive and stellar-mass black holes (SBHs), the existence
of intermediate-mass black holes (IMBHs) with masses ranging between 10^{2-5}
Msun has not yet been confirmed. The main problem in the detection is that the
innermost stellar kinematics of globular clusters (GCs) or small galaxies, the
possible natural loci to IMBHs, are very difficult to resolve. However, if
IMBHs reside in the centre of GCs, a possibility is that they interact
dynamically with their environment. A binary formed with the IMBH and a compact
object of the GC would naturally lead to a prominent source of gravitational
radiation, detectable with future observatories. We use N-body simulations to
study the evolution of GCs containing an IMBH and calculate the gravitational
radiation emitted from dynamically formed IMBH-SBH binaries and the possibility
that the IMBH escapes the GC after an IMBH-SBH merger. We run for the first
time direct-summation integrations of GCs with an IMBH including the dynamical
evolution of the IMBH with the stellar system and relativistic effects, such as
energy loss in gravitational waves (GWs) and periapsis shift, and gravitational
recoil. We find in one of our models an intermediate mass-ratio inspiral
(IMRI), which leads to a merger with a recoiling velocity higher than the
escape velocity of the GC. The GWs emitted fall in the range of frequencies
that a LISA-like observatory could detect, like the European eLISA or in
mission options considered in the recent preliminary mission study conducted in
China. The merger has an impact on the global dynamics of the cluster, as an
important heating source is removed when the merged system leaves the GC. The
detection of one IMRI would constitute a test of GR, as well as an irrefutable
proof of the existence of IMBHs.Comment: Accepted for publication by A&A, minor modification
Ultrafast Pulse Radiolysis Using a Terawatt Laser Wakefield Accelerator
We report the first ultrafast pulse radiolysis transient absorption
spectroscopy measurements from the Terawatt Ultrafast High Field Facility
(TUHFF) at Argonne National Laboratory. TUHFF houses a 20 TW Ti:sapphire laser
system that generates 2.5 nC sub-picosecond pulses of multi-MeV electrons at 10
Hz using laser wakefield acceleration. The system has been specifically
optimized for kinetic measurements in a pump-probe fashion. This requires
averaging over many shots which necessitates stable, reliable generation of
electron pulses. The latter were used to generate excess electrons in pulse
radiolysis of liquid water and concentrated solutions of perchloric acid. The
hydronium ions in the acidic solutions react with the hydrated electrons
resulting in the rapid decay of the transient absorbance at 800 nm on the
picosecond time scale. Time resolution of a few picoseconds has been
demonstrated. The current time resolution is determined primarily by the
physical dimensions of the sample and the detection sensitivity. Subpicosecond
time resolution can be achieved by using thinner samples, more sensitive
detection techniques and improved electron beam quality.Comment: submitted to J. Appl. Phys. 5 figures, 23 page
Structure, Photophysics and the Order-Disorder Transition to the Beta Phase in Poly(9,9-(di -n,n-octyl)fluorene)
X-ray diffraction, UV-vis absorption and photoluminescence (PL) spectroscopy
have been used to study the well-known order-disorder transition (ODT) to the
beta phase in poly(9,9-(di n,n-octyl)fluorene)) (PF8) thin film samples through
combination of time-dependent and temperature-dependent measurements. The ODT
is well described by a simple Avrami picture of one-dimensional nucleation and
growth but crystallization, on cooling, proceeds only after molecular-level
conformational relaxation to the so called beta phase. Rapid thermal quenching
is employed for PF8 studies of pure alpha phase samples while extended
low-temperature annealing is used for improved beta phase formation. Low
temperature PL studies reveal sharp Franck-Condon type emission bands and, in
the beta phase, two distinguishable vibronic sub-bands with energies of
approximately 199 and 158 meV at 25 K. This improved molecular level structural
order leads to a more complete analysis of the higher-order vibronic bands. A
net Huang-Rhys coupling parameter of just under 0.7 is typically observed but
the relative contributions by the two distinguishable vibronic sub-bands
exhibit an anomalous temperature dependence. The PL studies also identify
strongly correlated behavior between the relative beta phase 0-0 PL peak
position and peak width. This relationship is modeled under the assumption that
emission represents excitons in thermodynamic equilibrium from states at the
bottom of a quasi-one-dimensional exciton band. The crystalline phase, as
observed in annealed thin-film samples, has scattering peaks which are
incompatible with a simple hexagonal packing of the PF8 chains.Comment: Submitted to PRB, 12 files; 1 tex, 1 bbl, 10 eps figure
Triplet Exciton Generation in Bulk-Heterojunction Solar Cells based on Endohedral Fullerenes
Organic bulk-heterojunctions (BHJ) and solar cells containing the trimetallic
nitride endohedral fullerene 1-[3-(2-ethyl)hexoxy
carbonyl]propyl-1-phenyl-Lu3N@C80 (Lu3N@C80-PCBEH) show an open circuit voltage
(VOC) 0.3 V higher than similar devices with [6,6]-phenyl-C[61]-butyric acid
methyl ester (PC61BM). To fully exploit the potential of this acceptor molecule
with respect to the power conversion efficiency (PCE) of solar cells, the short
circuit current (JSC) should be improved to become competitive with the state
of the art solar cells. Here, we address factors influencing the JSC in blends
containing the high voltage absorber Lu3N@C80-PCBEH in view of both
photogeneration but also transport and extraction of charge carriers. We apply
optical, charge carrier extraction, morphology, and spin-sensitive techniques.
In blends containing Lu3N@C80-PCBEH, we found 2 times weaker photoluminescence
quenching, remainders of interchain excitons, and, most remarkably, triplet
excitons formed on the polymer chain, which were absent in the reference
P3HT:PC61BM blends. We show that electron back transfer to the triplet state
along with the lower exciton dissociation yield due to intramolecular charge
transfer in Lu3N@C80-PCBEH are responsible for the reduced photocurrent
Charge transfer dynamics in conjugated polymer/MoS2 organic/2D heterojunctions
Heterojunctions between organic and two-dimensional (2D) semiconductors show promising applications in ultrathin electronic and optoelectronic devices, including field-effect transistors, light-emitting diodes, and photovoltaics. These organic/2D heterojunctions form ideal interfaces due to the lack of dangling bonds at the surfaces of the neat (i.e., individual) materials and their propensity to interact via van der Waals forces. Despite this, organic/2D heterojunction devices have had relatively low quantum efficiencies, suggesting limitations on the charge transport within these devices. Understanding the charge transfer dynamics across organic/2D semiconductor interfaces at fundamental time scales is an important part of overcoming these limitations. In this work, we investigate the photoexcited charge carrier dynamics in organic/2D heterojunctions comprised of large-area monolayer MoS2 and solution-deposited organic semiconducting conjugated polymer thin-films. Using photoluminescence and femtosecond transient absorption spectroscopy, we compare the efficiencies of charge transfer for three different conjugated polymer/MoS2 heterojunctions: P3HT, PCDTBT, and PTB7. We show that electron transfer occurs from MoS2 to P3HT in under 9 ps, and from MoS2 to PCDTBT or PTB7 in under 120 fs. Despite this, we demonstrate that the P3HT/MoS2 heterojunction is the most efficient because the transferred charges have an order-of-magnitude increase in their lifetimes, giving rise to enhanced photoluminescence. This work will help guide designs of future organic/2D heterojunctions using scalable fabrication technologies
Carbon nanotubes for ultrafast fibre lasers
Carbon nanotubes (CNTs) possess both remarkable optical properties and high potential for integration in various photonic devices. We overview, here, recent progress in CNT applications in fibre optics putting particular emphasis on fibre lasers. We discuss fabrication and characterisation of different CNTs, development of CNT-based saturable absorbers (CNT-SA), their integration and operation in fibre laser cavities putting emphasis on state-of-the-art fibre lasers, mode locked using CNT-SA. We discuss new design concepts of high-performance ultrafast operation fibre lasers covering ytterbium (Yb), bismuth (Bi), erbium (Er), thulium (Tm) and holmium (Ho)-doped fibre lasers
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