Polycrystalline tetracene films have been explored using weak ∼ 30 fs visible laser pulses that excite the lowest singlet exciton as well as coherent vibrational motion. Transient difference spectra show a triplet absorption which arises following singlet fission (SF) and persists for 1.6 ns without decay. Adaptive pulse shaping identifies multipulse optimal fields which maximize this absorption feature by ∼ 20%. These are comprised of subpulses separated by time delays well correlated with the period of lattice vibrations suggesting such modes control the yield of SF photochemistry.
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http://dx.doi.org/10.1103/PhysRevLett.105.257403 | DOI Listing |
J Phys Chem Lett
April 2023
Graduate School of Science and Technology, Niigata University, 2-8050 Ikarashi, Nishi-ku, Niigata 950-2181, Japan.
A triplet-triplet pair is a key intermediate in singlet fission (SF), which has the potential to overcome the theoretical limit of solar cell efficiency. Here, we report a new spectroscopy to directly detect a short-lived triplet-triplet pair via the effects of radio-wave (RF) irradiation near zero magnetic field at room temperature. The fluorescence of polycrystalline powder of tetracene is reduced by RF irradiation at zero field, which is caused by a quasi-static RF field effect on spin mixing and electron-spin resonance among zero-field-splitting sublevels of the triplet-triplet pair.
View Article and Find Full Text PDFJ Chem Phys
December 2020
Department of Chemistry, University of California Riverside, Riverside, California 92521, USA.
The temperature-dependent fluorescence spectrum, decay rate, and spin quantum beats are examined in single tetracene crystals to gain insight into the mechanism of singlet fission. Over the temperature range of 250 K-500 K, the vibronic lineshape of the emission indicates that the singlet exciton becomes localized at 400 K. The fission process is insensitive to this localization and exhibits Arrhenius behavior with an activation energy of 550 ± 50 cm.
View Article and Find Full Text PDFMater Sci Eng C Mater Biol Appl
January 2020
Department of Bionanosystem Engineering, Graduate School, Chonbuk National University, Jeonju, 561-756, Republic of Korea; College of Medical and Dental Sciences, Sir Robert Aitken Institute for Medical Research, University of Birmingham, Edgbaston, Birmingham, UK. Electronic address:
A promising candidate for the development of controlled and targeted nanoscale drug delivery system but less studied so far is calcium carbonate (CaCO) in the form of porous polycrystalline vaterite spheres. Vaterite has been shown to exhibit various beneficial properties such as excellent biocompatibility, high drug loading capacity, and pH-sensitive decomposition under mild conditions. However, fabricating vaterite particles with improved porosity, high surface area and loading a payload into the common synthesis method is still a challenge.
View Article and Find Full Text PDFPhys Chem Chem Phys
May 2019
Department of Chemistry, Western Washington University, 516 High St., Bellingham, WA 98225, USA.
A model is introduced for treating early-stage nucleation, growth kinetics, and mesoscale domain structure in submonolayer polycrystalline films prepared by solution-phase processing methods such as spin casting, dip coating, liquid-based printing, and related techniques. The model combines a stochastic treatment of nucleation derived from classical nucleation theory with deterministic computation of the spatiotemporal dynamics of the monomer concentration landscape by numerical solution of the two-dimensional diffusion equation, treating nuclei as monomer sinks. Results are compared to experimental measurements of solution-processed submonolayer tetracene films prepared using a vapor-liquid-solid deposition technique.
View Article and Find Full Text PDFACS Nano
January 2019
Nanoscale Device Characterization Division , National Institute of Standards and Technology, 100 Bureau Drive , Gaithersburg , Maryland 20899 , United States.
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