title: Excitonic Relaxation and Coherent Vibrational Dynamics in Zinc Chlorin Aggregates for Artificial Photosynthetic Systems.
abstract: The excitonic relaxation and coherent vibrational dynamics in stairlike zinc chlorin aggregates prepared for mimicking chlorosome in nature have been studied simultaneously by 6.8 fs real-time vibrational laser spectroscopy. The relaxation from Q-exciton state to the dark nonfluorescent charge-transfer (CT) state is determined to be 850 ± 70 fs. The spectral distribution of the molecular vibrational amplitude has been discussed in terms of the difference in the equilibrium positions of potential curves between the ground state and the excited state. Since the displacement in the coordinate space from the potential minimum of the ground state to that of the excited states is small, coherent oscillations generated by the impulsive excitation are strongest where the slope of the excitonic resonance is largest. Consequently, the probe wavelength dependence of the amplitude modulation follows the first derivative of the excitonic resonance, and π phase jump has been observed. Excitonic transition energy modulation caused by the coherent molecular vibrations has also been studied, and the vibrational mode with a low frequency of 146 cm(-1) is found to play a dominating role in the transition energy shift effect.
authors: State Key Laboratory of High Field Laser Physics, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences , Shanghai 201800, China.
authors: Dongjia
authors: D
authors: Han
authors: State Key Laboratory of High Field Laser Physics, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences , Shanghai 201800, China.
authors: Juan
authors: J
authors: Du
authors: Advanced Ultrafast Laser Research Center, University of Electro-Communications , 1-5-1, Chofugaoka, Chofu, Tokyo 182-8585, Japan.|JST , CREST, K's Gobancho, 7 Gobancho, Chiyoda-ku, Tokyo, 102-0076 Japan.
authors: Takayoshi
authors: T
authors: Kobayashi
authors: Department of Materials Chemistry, Ryukoku University , Otsu, Shiga 520-2194, Japan.
authors: Tomohiro
authors: T
authors: Miyatake
authors: Department of Bioscience and Biotechnology, Ritsumeikan University , Kusatsu, Shiga 525-8577, Japan.
authors: Hitoshi
authors: H
authors: Tamiaki
authors: State Key Laboratory of High Field Laser Physics, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences , Shanghai 201800, China.
authors: Yanyan
authors: Y
authors: Li
authors: State Key Laboratory of High Field Laser Physics, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences , Shanghai 201800, China.|FSA Collaborative Innovation Center, Shanghai Jiao Tong University , Shanghai 200240, China.
authors: Yuxin
authors: Y
authors: Leng
mesh_terms: D007834:Lasers; D008665:Metalloporphyrins / Q000737:chemistry*; D010788:Photosynthesis / Q000502:physiology*; D011789:Quantum Theory; D013057:Spectrum Analysis; D014732:Vibration
chemical_list: D008665:Metalloporphyrins; C558702:zinc chlorin