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Singlet fission (SF), a spin-allowed multiexciton generation process, experienced renewed interest in the last decade due to its potential to increase the efficiency of photovoltaic devices. The hurdles now lie in the limited range of SF-capable materials and demanding morphology requirement for an efficient fission process. Although primary fission to yield triplet pair (1TT) can occur independently of film morphology in intramolecular singlet fission (iSF) materials, the separation of the 1TT state has been shown to be highly dependent on the packing motif and morphologies. In this work, we have demonstrated that both iSF and triplet pair separation processes took place irrelevant of molecular order and/or film morphology in a series of pentalene compounds. With the >180% fission efficiency, the suitable triplet energy levels, and the long lifetime of the triplet excitons, these iSF systems can be integrated into practical photovoltaic application. [ABSTRACT FROM AUTHOR]

We have developed an integrated instrument combining deep ultraviolet laser ionization mass spectrometry (DUV-LIMS) and infrared multiphoton dissociation (IR-MPD) spectroscopy, abbreviated as DUV-IR. The 177.3 nm DUV laser (7 eV single-photon energy) has short pulse duration (15 ps) and appropriate pulse energy (∼20 µJ), which is found to be highly efficient for low-fragment photoionization of neutral metal clusters and molecules. A home-made cluster source is designed with an adjustable formation channel suitable for the generation of different cluster series. The well-aligned components of the reflection time-of-flight mass spectrometer, as well as the coaxial design of DUV laser and molecular beam, bring forth high sensitivity and high resolution of the DUV-LIMS. Taking these advantages, well-resolved neutral Vn (n = 1–43) and (Benzene)n (n = 1–25) clusters have been generated free of fragmentation. In addition to the generation and detection of neutral clusters, a fast-flow reaction tube is also designed downstream of the cluster source allowing to study their reactivity. In particular, a broad-range tunable IR laser (1.3–16 µm) is coupled with the DUV laser to attain IR-MPD spectroscopic analysis. This integrated system offers a general protocol to prepare various clusters to study their gas-phase reactivity and to determine their structures. [ABSTRACT FROM AUTHOR]

We report here the development of a reflectron time-of-flight mass spectrometer utilizing singlephoton ionization based on an all-solid-state deep ultraviolet (DUV) laser system. The DUV laser was achieved from the second harmonic generation using a novel nonlinear optical crystal KBe2BO3F2 under the condition of high-purity N2 purging. The unique property of this laser system (177.3-nm wavelength, 15.5-ps pulse duration, and small pulse energy at ~15 μJ) bears a transient low power density but a high single-photon energy up to 7 eV, allowing for ionization of chemicals, especially organic compounds free of fragmentation. Taking this advantage, we have designed both pulsed nanospray and thermal evaporation sources to form supersonic expansion molecular beams for DUV single-photon ionization mass spectrometry (DUV-SPI-MS). Several aromatic amine compounds have been tested revealing the fragmentation-free performance of the DUV-SPI-MS instrument, enabling applications to identify chemicals from an unknown mixture. [ABSTRACT FROM AUTHOR]