551 research outputs found
Correlated-electron description of the photophysics of thin films of -conjugated polymers
We extend Mulliken's theory of ground state charge transfer in a
donor-acceptor complex to excited state charge transfer between pairs of
identical -conjugated oligomers, one of which is in the optically excited
state and the other in the ground state, leading to the formation of a
charge-transfer exciton. Within our theory, optical absorptions from the
charge-transfer exciton should include a low energy intermolecular
charge-transfer excitation, as well as distinct intramolecular excitations from
both the neutral delocalized exciton component and the Coulombically bound
polaron-pair component of the charge-transfer exciton. We report high order
configuration-interaction calculations for pairs of oligomers of
poly-paraphenylenevinylene (PPV) that go beyond our previous single
configuration-interaction calculation and find all five excited state
absorptions predicted using heuristic arguments based on the Mulliken concept.
Our calculated excited state absorption spectrum exhibits strong qualitative
agreement with the complete wavelength-dependent ultrafast photoinduced
absorption in films of PPV derivatives, suggesting that a significant fraction
of the photoinduced absorption here is from the charge-transfer exciton. We
make detailed comparisons to experiments, and a testable experimental
prediction
Effect of interchain coupling on conducting polymer luminescence: excimers in derivatives of poly(phenylene vinylene)
Optical excitation of a chain in a polymer film may result in formation of an
excimer, a superposition of on-chain excitons and charge-transfer excitons on
the originally excited chain and a neighboring chain. The excimer emission is
red-shifted compared to that of an on-chain exciton by an amount depending on
the interchain coupling . Setting up the excimer wavefunction and
calculating the red shift, we determine average values, referred to a
monomer, of 0.52 eV and 0.16 eV for poly(2,5-hexyloxy -phenylene
cyanovinylene), CN-PPV, and poly[2-methoxy, 5-(2'-ethyl-hexyloxy)-1, 4
p-phenylene vinylene], MEH-PPV, respectively, and use them to determine the
effect of interchain distance on the emission.Comment: 10 pages, RevTeX, 1 PS figure, replaced version of cond-mat/9707095,
accepted for publication in Phys. Rev. B, Rapid Communicatio
Differentiated thyroid carcinoma associated with histological features of Hashimoto's thyroiditis
Evidence for Excimer Photoexcitations in an Ordered {\pi}-Conjugated Polymer Film
We report pressure-dependent transient picosecond and continuous-wave
photomodulation studies of disordered and ordered films of
2-methoxy-5-(2-ethylhexyloxy) poly(para-phenylenevinylene). Photoinduced
absorption (PA) bands in the disordered film exhibit very weak pressure
dependence and are assigned to intrachain excitons and polarons. In contrast,
the ordered film exhibits two additional transient PA bands in the midinfrared
that blueshift dramatically with pressure. Based on high-order configuration
interaction calculations we ascribe the PA bands in the ordered film to
excimers. Our work brings insight to the exciton binding energy in ordered
films versus disordered films and solutions. The reduced exciton binding energy
in ordered films is due to new energy states appearing below the continuum band
threshold of the single strand.Comment: 5.5 pages, 5 figure
Quantum inelastic conductance through molecular wires
We calculate non-perturbatively the inelastic effects on the conductance
through a conjugated molecular wire-metal heterojunction, including realistic
electron-phonon coupling. We show that at sub-band-gap energies the current is
dominated by quantum coherent transport of virtual polarons through the
molecule. In this regime, the tunneling current is strongly increased relative
to the case of elastic scattering. It is essential to describe the full quantum
coherence of the polaron formation and transport in order to obtain correct
physics. Our results are generally applicable to one-dimensional atomic or
molecular wires.Comment: 4 pages, 4 figures, accepted for publication in Physical Review
Letter
Mesoscopic Cooperative Emission From a Disordered System
We study theoretically the cooperative light emission from a system of classical oscillators confined within a volume with spatial scale, , much
smaller than the radiation wavelength, . We assume
that the oscillators frequencies are randomly distributed around a central
frequency, , with some characteristic width, . In
the absence of disorder, that is , the cooperative emission spectrum
is composed of a narrow subradiant peak superimposed on a wide superradiant
band. When , we demonstrate that if is large enough, the
subradiant peak is not simply broadened by the disorder but rather splits into
a system of random narrow peaks. We estimate the spectral width of these peaks
as a function of , and . We also estimate the
amplitude of this mesoscopic structure in the emission spectrum.Comment: 25 pages including 6 figure
Fluctuation-Facilitated Charge Migration along DNA
We propose a model Hamiltonian for charge transfer along the DNA double helix
with temperature driven fluctuations in the base pair positions acting as the
rate limiting factor for charge transfer between neighboring base pairs. We
compare the predictions of the model with the recent work of J.K. Barton and
A.H. Zewail (Proc.Natl.Acad.Sci.USA, {\bf 96}, 6014 (1999)) on the unusual
two-stage charge transfer of DNA.Comment: 4 pages, 2 figure
Quality of Life in Chronic Pancreatitis is Determined by Constant Pain, Disability/Unemployment, Current Smoking, and Associated Co-Morbidities
OBJECTIVES: Chronic pancreatitis (CP) has a profound independent effect on quality of life (QOL). Our aim was to identify factors that impact the QOL in CP patients. METHODS: We used data on 1,024 CP patients enrolled in the three NAPS2 studies. Information on demographics, risk factors, co-morbidities, disease phenotype, and treatments was obtained from responses to structured questionnaires. Physical and mental component summary (PCS and MCS, respectively) scores generated using responses to the Short Form-12 (SF-12) survey were used to assess QOL at enrollment. Multivariable linear regression models determined independent predictors of QOL. RESULTS: Mean PCS and MCS scores were 36.7+/-11.7 and 42.4+/-12.2, respectively. Significant (P \u3c 0.05) negative impact on PCS scores in multivariable analyses was noted owing to constant mild-moderate pain with episodes of severe pain or constant severe pain (10 points), constant mild-moderate pain (5.2), pain-related disability/unemployment (5.1), current smoking (2.9 points), and medical co-morbidities. Significant (P \u3c 0.05) negative impact on MCS scores was related to constant pain irrespective of severity (6.8-6.9 points), current smoking (3.9 points), and pain-related disability/unemployment (2.4 points). In women, disability/unemployment resulted in an additional 3.7 point reduction in MCS score. Final multivariable models explained 27% and 18% of the variance in PCS and MCS scores, respectively. Etiology, disease duration, pancreatic morphology, diabetes, exocrine insufficiency, and prior endotherapy/pancreatic surgery had no significant independent effect on QOL. CONCLUSIONS: Constant pain, pain-related disability/unemployment, current smoking, and concurrent co-morbidities significantly affect the QOL in CP. Further research is needed to identify factors impacting QOL not explained by our analyses
A Shot in the Dark: Failing to Recognize the Link Between Physical and Mental Illness
A 74-year-old widowed white man with chronic rheumatoid arthritis presented with nausea and weight loss. He was diagnosed with failure to thrive and admitted for hydration. Misoprostol was determined to be the etiology of his symptoms and he was discharged home. Three days later, he killed himself with a gunshot to the head. Clinicians often fail to recognize those at high risk for suicide. Suicidal risk is increased in both psychiatric and physical illness, and particularly when both are present. Psychiatric illness, particularly depression, often underlies chronic medical illness. The purpose of this case report is to remind health care providers of the strong association between depression and chronic medical illness, and to consider this in all patients, including those who present solely with physical symptoms. Recognizing this association and screening for it, as recommended by the U.S. Preventive Services Task Force, may prevent the unnecessary tragedy of suicide
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