极性溶剂对LDS750分子内电荷转移过程的影响
摘要
在本文中,我们主要是利用飞秒瞬态吸收方法来研究LDS750分子在不同极性溶液中的超快动力学过程。把采集的数据进行三指数拟合后得到三个不同的弛豫过程,第一个过程是在数百飞秒量级上快弛豫过程,我们认为第一激发态分子内振动弛豫再分布是导致这一过程的主要原因;第二个过程是在数皮秒量级上的慢弛豫过程,我们通过与先前研究实验结果和理论计算相比较后得出结论,认为被激发LDS750分子存在分子内扭转电荷转移(TICT)过程,即TICT态。从而我们把这一过程归因于粒子从第一激发态的低振动态向TICT弛豫的过程;第三个过程是在数十皮秒量级上的更慢弛豫过程,对于导致这一过程主要因素我们认为是ICT态的寿命及溶剂化过程的共同作用的结果,并且整个慢过程都会受到溶剂粘度系数的影响。
In recent years, with the rapid development of femtosecond lasers, several optical techniques are used to characterize the ultrafast solvation dynamics of the dye molecules in solution, for example, femtosecond time-resolved fluorescence depletion spectroscopy, fluorescence up- conversion and femtosecond transient absorption spectroscopy and so on. In the solution system, a molecular system is excited by an intense, polarized and ultrashort pulse of light, while several ultrafast dynamical processes such as the intramolecular vibrational energy redistribution (IVR), electron transfer between solute and solutions, twisted intra-molecular charge transfer (TICT), the diffusive solvent relaxation etc. will take place. So the equilibrium distribution of molecular orientations can be disturbed and the system is in a high-energy configuration. With the increase of time, the orientation holes rearrange themselves to the best accommodation to minimize the total free energy.
In our experient, ultrafast dynamics studies using femtosecond transient absorption pump-probe technique were performed on LDS750 in polar solvents. The experimental decays of LDS750 in various solvents that include the one fast and two slow processes have been fitted by the tri-exponential function, The fast process on a scale of hundreds of J. L. femtoseconds are assigned to intramolecular vibrational energy redistribution (IVR), and the first slower process on the order of picosecond are contributed to a relaxation from locally excited (LE) state to a twisted intramolecular charge transfer (TICT) state, the second slower process is mainly attributed to the life of the TICT state and solvation relaxation, and the slow process is all effected on the viscosity of the solvents and dipole moment.
In recent years, with the rapid development of femtosecond lasers, several optical techniques are used to characterize the ultrafast solvation dynamics of the dye molecules in solution, for example, femtosecond time-resolved fluorescence depletion spectroscopy, fluorescence up- conversion and femtosecond transient absorption spectroscopy and so on. In the solution system, a molecular system is excited by an intense, polarized and ultrashort pulse of light, while several ultrafast dynamical processes such as the intramolecular vibrational energy redistribution (IVR), electron transfer between solute and solutions, twisted intra-molecular charge transfer (TICT), the diffusive solvent relaxation etc. will take place. So the equilibrium distribution of molecular orientations can be disturbed and the system is in a high-energy configuration. With the increase of time, the orientation holes rearrange themselves to the best accommodation to minimize the total free energy.
In our experient, ultrafast dynamics studies using femtosecond transient absorption pump-probe technique were performed on LDS750 in polar solvents. The experimental decays of LDS750 in various solvents that include the one fast and two slow processes have been fitted by the tri-exponential function, The fast process on a scale of hundreds of J. L. femtoseconds are assigned to intramolecular vibrational energy redistribution (IVR), and the first slower process on the order of picosecond are contributed to a relaxation from locally excited (LE) state to a twisted intramolecular charge transfer (TICT) state, the second slower process is mainly attributed to the life of the TICT state and solvation relaxation, and the slow process is all effected on the viscosity of the solvents and dipole moment.
引文
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[6] K. Prater, W.L. Freund, and R.M. Bowman, Ultrafast investigations of the photophysics of 4-phenylbenzophenone in solution. Chem. Phys. Lett. 1998, 295(1-2), 82.
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[11] H. Ye, G.W. Wicks, and P.M. Fauchet, Hot electron relaxation time in GaN. Appl. Phys. Lett. 1999, 74(5), 711.
[12] A.A. Voityuk, M. Michel-Beyerle, and N. Rosch, Structure and rotation barriers for ground and excited states of the isolated chromophore of the green fluorescent protein. Chem. Phys. Lett. 1998, 296(3-4), 269.
[13] E.J.G. Peterman, R. Monshouwer, I.H.M. Stokkum, R.van Grondelle and H.van Amerongen, Ultrafast singlet excitation transfer from carotenoids to chlorophylls via different pathways in light-harvesting complex II of higher plants. Chem. Phys. Lett. 1997, 264(3-4), 279.
[14] A. Freiberg, K. Timpmann, S. Liu, and N.W. Woodbury, Exciton Relaxation and Transfer in the LH2 Antenna Network of Photosynthetic Bacteria. J. Phys. Chem. B 1998, 102(52), 10974.
[15] T. Ditmire, J.W.G. Tisoh, E. Springate, M.B. Mason, N. Hay, R.A. Smith, J. Marangos, and M.H.R. Hutchinson, High-energy ions preduced in explosions of superheated atomic clusters. Nature 1997, 386, 54.
[16] D. vonder Linde, J. Kuhl and H. Klingenberg, Raman Scattering from Nonequilibrium LO Phonons with Picosecond Resolution. Phys. Rev. Lett. 1980, 44(23), 1505.
[17] R.Z.B. Desamero, V. Chynwat, I. van der Hoef, F.J. Jansen, J. Lugtenburg, D. Gosztola, M.R. Wasielewski, A. Cua, D.F. Bocian, and H.A. Frank, Mechanism of Energy Transfer from Carotenoids to Bacteriochlorophyll: Light-Harvesting by Carotenoids Having Different Extents of -Electron Conjugation Incorporated into the B850 Antenna Complex from the Carotenoidless Bacterium Rhodobacter sphaeroides R-26.1. J. Phys. Chem. B 1998, 102(42), 8151.
[18] T. Elsaesser, M. Woerner, Femtosecond infrared spectroscopy of semiconductors and semiconductor nanostructures. Physics Reports 1999, 321(6), 253.
[19] M. Dantus. Ultrafast probing and control of molecular dynamics: Beyond the Pump-probe Method in Femtochemistry. De Schryver, De Feyter, Schweitzer Eds. Wiley-VCH, 2002, 169.
[20] K.Y. Tseng, K.S. Wong, G.K.L. Wong, Femtosecond time-resolved Z-scan investigations of optical nonlinearities in ZnSe. Optics Letters 1996, 21(3), 180.
[21] Q.H. Zhong, Z.H. Wang, Y. Sun, Q.H. Zhu, F.A. Kong. Vibrational relaxation of dye molecules in solution studied by femtosecond time-resolved stimulated emission pumping fluorescence depletion. Chem. Phys. Lett. 1996, 248, 277-282.
[22] J.Y. Liu, W.H. Fan, K.L. Han, W.Q. Deng, D.L. Xu, N.Q. Lou. Ultrafast vibrational and thermal relaxation of dye molecules in solutions. J. Phys. Chem. A 2003, 107(50), 10857-10861.
[23] L.C. Zhou, J.Y. Liu, G.J. Zhao, Y Shi, X.J. Peng, K.L. Han. The ultrafast dynamics of near-infrared heptamethine cyanine dye in alcoholic and aprotic solvents. Chem. Phys. 2007, 333, 179-185.
[24] K Rotkiewicz, J Herbich, F Pérez Salgado, W Rettig. TICT states in p-cyano-N,N-dimethylaniline derivatives. The structural and environmental effects. Proc. Indian. Acad. Sci. (Chem Sci) 1992, 104(2), 105-115.
[25] JA Bautista, RE Connors, B Bangar Raju, RG Hiller, FP Sharples, Gosztola D, Wasielewski MR, Frank HA. Excited state properties of peridinin: observation of a solvent dependence of the lowest excited singlet state lifetime and spectral behavior unique amongcarotenoids. J. Phys. Chem. B 1999, 103(41), 8751-8758.
[26] DK Palit, AK Singh, AC Bhasikuttan, JP Mittal. Relaxation dynamics in the excited states of LDS-821 in solution. J. Phys. Chem. A 2001, 105(26), 6294-6304.
[27]D Zigmantas, T Polvka, RG Hiller, A Yartsev, V Sundstrm. Spectroscopic and dynamic properties of the peridinin lowest singlet excited states. J. Phys. Chem. A 2001, 105(45), 10296-10306.
[28] XM Guo, AD Xia. Ultrafast excited states relaxation dynamics in solution investigated by stimulated emission from a styryl dye. Journal of Luminescence 2007, 122–123, 532–535.
[29] PW Zhou, P Song, JY Liu, Y Shi, KL Han, GZ He. Rotational reorientation dynamics of oxazine 750 in polar solvents. J. Phys. Chem. A 2008, 112(16), 3646-3655.
[30] PK Singh, S Nath, AC Bhasikuttan, M Kumbhakar, J Mohanty, SK Sarkar, T Mukherjee, H Pal. Effect of donor orientation on ultrafast intermolecular electron transfer in coumarin-amine systems. J. Chem. Phys. 2008, 129, 114504-114511.
[31]BG Liu, MX Jin, H Liu et al. Femtosecond time-resolved measurement of LDS698 molecular processes under high pressure Appl. Phys. Lett. 2008, 92, 241916-241619.
[32] Tianquan Lian,+Yuriy Kholodenko, Robin M. Hochstrasser, Infrared Probe of the Solvent Response to Ultrafast Solvation Processes, J.Phys. Chem., 1995, 99 (9), 2546-2551
[33] D. Bingemann, N.P. Ernsting, Femtosecond solvation dynamics determining the band shape of stimulated emission from a polar styryl dye, J. Chem. Phys.1995.102(7) 2691-2700.
[34] N A. Smith, S R Meech, I V Rubtsov, K Yoshihara, LDS-750 as a probe of solvation dynamics: a femtosecond time-resolved fluorescence study in liquid aniline. Chemical Physics Letters 303_1999.209–217
[35] M. R. Dreizler, E. K. U. Gross(Eds.), Density Functional Theory, Springer Verlag: Heidelberg, Germany, 1990.
[36] C. Lee, W. Yang, R. G. Parr, Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density, Phys. Rev. B 37 (1988) 785-789.
[37] E. K. U. Gross, W. Kohn, Local density-functional theory of frequency-dependent linear response, Phys. Rev. Lett. 55 (1985) 2850-2852.
[38] M. J. Frisch, G. W. Trucks, H. B. Schlegel, G. E. Scuseria, M. A. Robb, J. R. Cheeseman, G. Scalmani, V. Barone, B. Mennucci, G. A. Petersson, H. Nakatsuji, M. Caricato, X. Li, H. P. Hratchian, A. F. Izmaylov, J. Bloino, G. Zheng, J. L. Sonnenberg, M. Hada, M. Ehara, K. Toyota, R. Fukuda, J. Hasegawa, M. Ishida, T. Nakajima, Y. Honda, O. Kitao, H. Nakai, T. Vreven, J. A. Montgomery, Jr., J. E.Peralta, F. Ogliaro, M. Bearpark, J. J. Heyd, E. Brothers, K. N. Kudin, V. N. Staroverov, R. Kobayashi, J. Normand, K. Raghavachari, A. Rendell, J. C. Burant, S. S. Iyengar, J. Tomasi, M. Cossi, N. Rega, J. M. Millam, M. Klene, J. E. Knox, J. B. Cross, V. Bakken, C. Adamo, J. Jaramillo, R. Gomperts, R. E. Stratmann, O. Yazyev, A. J. Austin, R. Cammi, C. Pomelli, J. W. Ochterski, R. L. Martin, K. Morokuma, V. G. Zakrzewski, G. A. Voth, P. Salvador, J. J. Dannenberg, S. Dapprich, A. D. Daniels, O. Farkas, J. B. Foresman, J. V. Ortiz, J. Cioslowski, and D. J. Fox, Gaussian 09, Revision A.02, Gaussian, Inc., Wallingford CT, 2009.
[39] David M Jonas, Matthew J Lang, Yutaka Nagasawa, Taiha Joo, Graham R Fleming, Pump-Probe Polarization Anisotropy Study of Femtosecond Energy Transfer within the Photosynthetic Reaction Center of Rhodobacter sphaeroides R26. J. Phys. Chem. 1996, 100(30), 12660.
[40] Lewis D Book, David C Arnett, Hanbo Hu, Norbert F Scherer, Ultrafast Pump-Probe Studies of Excited-State Charge-Transfer Dynamics in Blue Copper Proteins. J. Phys. Chem. A 1998, 102(23), 4350.
[41] V.M. Kenkre, A. Toknakoff, M.D. Fayer, Theory of vibrational relaxation of polyatomic molecules in liquids. J. Chem. Phys. 1994, 101(12), 10618.
[42] A.J. Taylor, D.J. Erskine and C.L. Tang, Femtosecond vibrational relaxation of large organic molecules. Chem. Phys. Lett. 1984, 103(5), 430.
[43] A.M. Wemer and E.P. Ippen, Femtosecond excited state relaxation of dye molecules in solution. Chem. Phys. Lett. 1985, 114(5-6), 456.
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