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Full-Text Articles in Physical Sciences and Mathematics
Anisotropic Singlet Fission In Single Crystalline Hexacene, Dezheng Sun, Gang-Hua Deng, Bolei Xu, Enshi Xu, Xia Li, Yajing Wu, Yuqin Qian, Yu Zhong, Colin Nuckolls, Avetik R. Harutyunyan, Hai-Lung Dai, Gugang Chen, Hanning Chen, Yi Rao
Anisotropic Singlet Fission In Single Crystalline Hexacene, Dezheng Sun, Gang-Hua Deng, Bolei Xu, Enshi Xu, Xia Li, Yajing Wu, Yuqin Qian, Yu Zhong, Colin Nuckolls, Avetik R. Harutyunyan, Hai-Lung Dai, Gugang Chen, Hanning Chen, Yi Rao
Chemistry and Biochemistry Faculty Publications
Singlet fission is known to improve solar energy utilization by circumventing the Shockley-Queisser limit. The two essential steps of singlet fission are the formation of a correlated triplet pair and its subsequent quantum decoherence. However, the mechanisms of the triplet pair formation and decoherence still remain elusive. Here we examined both essential steps in single crystalline hexacene and discovered remarkable anisotropy of the overall singlet fission rate along different crystal axes. Since the triplet pair formation emerges on the same timescale along both crystal axes, the quantum decoherence is likely responsible for the directional anisotropy. The distinct quantum decoherence rates …
Diffraction Effects In Single‐ And Two‐Laser Photothermal Lens Spectroscopy, Stephen E. Bialkowski, Agnes Chartier
Diffraction Effects In Single‐ And Two‐Laser Photothermal Lens Spectroscopy, Stephen E. Bialkowski, Agnes Chartier
Stephen E. Bialkowski
A simple method for calculating the effects of optical geometry on photothermal lens signals is shown. This method is based on calculating cumulative electric-field phase shifts produced by a series of Gaussian refractive-index perturbations produced by the photothermal effect. Theoretical results are found for both pulsed-laser and continuous Gaussian laser excitation sources and both single- and two-laser apparatuses commonly employed in photothermal lens spectroscopy. The effects of apparatus geometry on the resulting signal are shown. Analytical time-dependent signal results are found for small signals. Analytical pump–probe focus geometry results allow direct optimization for certain conditions. The calculations indicate that the …
Accounting For Saturation Effects In Pulsed Infrared Laser Excited Photothermal Spectroscopy, Stephen E. Bialkowski
Accounting For Saturation Effects In Pulsed Infrared Laser Excited Photothermal Spectroscopy, Stephen E. Bialkowski
Stephen E. Bialkowski
Equations that relate photothermal lens focal lengths and photothermal deflection angles to saturation absorption coefficients are derived. These equations are derived for two-level absorbers with both homogeneously and inhomogeneously broadened transitions. Initial and time-dependent photothermal lens signals are calculated. Equations describing the zero-time signals are exact to within the simplifying assumptions of the derivation, while the time-dependent signals are approximate. The approximation is performed by the use of a finite series of Gaussian functions to model the temperature change profile distorted by nonlinear absorption. The excitation irradiance-dependent signal behavior for rectangular and exponential excitation pulse time profiles for homogeneously and …
Application Of The Batio3 Beam Fanning Limiter As An Adaptive Spatial Filter For Signal Enhancementin Pulsed Laser Excited Photothermal Spectroscopy, Stephen E. Bialkowski
Application Of The Batio3 Beam Fanning Limiter As An Adaptive Spatial Filter For Signal Enhancementin Pulsed Laser Excited Photothermal Spectroscopy, Stephen E. Bialkowski
Stephen E. Bialkowski
A method for obtaining a high-contrast visible-light signal from infrared absorption in low-absorbance samples is described. This method is based on a beam-fanning optical limiter in photorefractive BaTiO3. The resulting signal is not linear but does exhibit an enhanced signal-to-background ratio that is 4 to 6 orders of magnitude better than that of conventional infrared absorption spectrophotometry in the shot-noise limit. A simple model for the beam-fanning, optical-limiter-based, pulsed-laser-excited photothermal spectroscopy detector is found to describe the experimental data adequately. This technique using photothermal spectroscopy detection may have advantages for rapid signal analysis and for two-dimensional visible imaging …