1 3
Topics in Current Chemistry (2018) 376:35
In conclusion, multi-VCS is now established as one of the state-of-the-art nonlinear spectroscopy techniques for the investigation of ultrafast photoreactivity in
molecules. More specifically, it is a technique of choice for monitoring vibrational
dynamics in excited states with unparalleled time resolution. It is our belief that the
combination of multi-VCS methods with recent and rapid theoretical developments
will further enhance the impact of multi-VCS in unraveling ultrafast photoreaction
mechanisms.
References
1. Joo TH, Albrecht AC (1993) Vibrational frequencies and dephasing times in excited electronic
states by femtosecond time-resolved 4-wave-mixing. Chem Phys 173(1):17–26
2. Weiner AM, Desilvestri S, Ippen EP (1985) 3-Pulse scattering for femtosecond dephasing studies—theory and experiment. J Opt Soc Am B 2(4):654–662
3. Hwang H, Rossky PJ (2004) Electronic decoherence induced by intramolecular vibrational motions
in a betaine dye molecule. J Phys Chem B 108(21):6723–6732. https ://doi.org/10.1021/jp037 031b
4. Vos MH, Jones MR, Martin JL (1998) Vibrational coherence in bacterial reaction centers: spectroscopic characterisation of motions active during primary electron transfer. Chem Phys 233(2–
3):179–190. https ://doi.org/10.1016/S0301 -0104(97)00355 -8
5. Collini E, Wong CY, Wilk KE, Curmi PMG, Brumer P, Scholes GD (2010) Coherently wired lightharvesting in photosynthetic marine algae at ambient temperature. Nature 463(7281):U644–U669.
https ://doi.org/10.1038/natur e0881 1
6. Fuller FD, Pan J, Gelzinis A, Butkus V, Senlik SS, Wilcox DE, Yocum CF, Valkunas L, Abramavicius D, Ogilvie JP (2014) Vibronic coherence in oxygenic photosynthesis. Nat Chem 6(8):706–
711. https ://doi.org/10.1038/nchem .2005
7. Huelga SF, Plenio MB (2013) Vibrations, quanta and biology. Contemp Phys 54(4):181–207. https
://doi.org/10.1080/00405 000.2013.82968 7
8. Romero E, Augulis R, Novoderezhkin VI, Ferretti M, Thieme J, Zigmantas D, van Grondelle R
(2014) Quantum coherence in photosynthesis for efficient solar-energy conversion. Nat Phys
10(9):677–683. https ://doi.org/10.1038/nphys 3017
9. Scholes GD, Fleming GR, Olaya-Castro A, van Grondelle R (2011) Lessons from nature about
solar light harvesting. Nat Chem 3(10):763–774. https ://doi.org/10.1038/nchem .1145
10. Gueye M, Manathunga M, Agathangelou D, Orozco Y, Paolino M, Fusi S, Haacke S, Olivucci
M, Leonard J (2018) Engineering the vibrational coherence of vision into a synthetic molecular
device. Nat Commun 9:313. https ://doi.org/10.1038/s4146 7-017-02668 -w
11. Scholes GD, Fleming GR, Chen LX, Aspuru-Guzik A, Buchleitner A, Coker DF, Engel GS, van
Grondelle R, Ishizaki A, Jonas DM, Lundeen JS, McCusker JK, Mukamel S, Ogilvie JP, OlayaCastro A, Ratner MA, Spano FC, Whaley KB, Zhu XY (2017) Using coherence to enhance function in chemical and biophysical systems. Nature 543(7647):647–656. https ://doi.org/10.1038/
natur e2142 5
12. Rose TS, Rosker MJ, Zewail AH (1989) Femtosecond real-time probing of reactions. IV. The reactions of alkali halides. J Chem Phys 91(12):7415–7436
13. Pollard WT, Fragnito HL, Bigot JY, Shank CV, Mathies RA (1990) Quantum-mechanical theory for 6 fs dynamic absorption spectroscopy and its application to Nile blue. Chem Phys Lett
168(3):239–245. https ://doi.org/10.1016/0009-2614(90)85603 -A
14. Fragnito HL, Bigot JY, Becker PC, Shank CV (1989) Evolution of the vibronic absorption spectrum in a molecule following impulsive excitation with a 6 fs optical pulse. Chem Phys Lett
160(2):101–104. https ://doi.org/10.1016/0009-2614(89)87564 -5
15. Dhar L, Rogers JA, Nelson KA (1994) Time-resolved vibrational spectroscopy in the impulsive
limit. Chem Rev 94(1):157–193. https ://doi.org/10.1021/cr000 25a00 6
16. Ruhman S, Kosloff R (1990) Application of chirped ultrashort pulses for generating large-amplitude ground-state vibrational coherence: a computer simulation. J Opt Soc Am B 7(8):1748–1752.
https ://doi.org/10.1364/josab .7.00174 8
237
Reprinted from the journal
Topics in Current Chemistry (2018) 376:35
In conclusion, multi-VCS is now established as one of the state-of-the-art nonlinear spectroscopy techniques for the investigation of ultrafast photoreactivity in
molecules. More specifically, it is a technique of choice for monitoring vibrational
dynamics in excited states with unparalleled time resolution. It is our belief that the
combination of multi-VCS methods with recent and rapid theoretical developments
will further enhance the impact of multi-VCS in unraveling ultrafast photoreaction
mechanisms.
References
1. Joo TH, Albrecht AC (1993) Vibrational frequencies and dephasing times in excited electronic
states by femtosecond time-resolved 4-wave-mixing. Chem Phys 173(1):17–26
2. Weiner AM, Desilvestri S, Ippen EP (1985) 3-Pulse scattering for femtosecond dephasing studies—theory and experiment. J Opt Soc Am B 2(4):654–662
3. Hwang H, Rossky PJ (2004) Electronic decoherence induced by intramolecular vibrational motions
in a betaine dye molecule. J Phys Chem B 108(21):6723–6732. https ://doi.org/10.1021/jp037 031b
4. Vos MH, Jones MR, Martin JL (1998) Vibrational coherence in bacterial reaction centers: spectroscopic characterisation of motions active during primary electron transfer. Chem Phys 233(2–
3):179–190. https ://doi.org/10.1016/S0301 -0104(97)00355 -8
5. Collini E, Wong CY, Wilk KE, Curmi PMG, Brumer P, Scholes GD (2010) Coherently wired lightharvesting in photosynthetic marine algae at ambient temperature. Nature 463(7281):U644–U669.
https ://doi.org/10.1038/natur e0881 1
6. Fuller FD, Pan J, Gelzinis A, Butkus V, Senlik SS, Wilcox DE, Yocum CF, Valkunas L, Abramavicius D, Ogilvie JP (2014) Vibronic coherence in oxygenic photosynthesis. Nat Chem 6(8):706–
711. https ://doi.org/10.1038/nchem .2005
7. Huelga SF, Plenio MB (2013) Vibrations, quanta and biology. Contemp Phys 54(4):181–207. https
://doi.org/10.1080/00405 000.2013.82968 7
8. Romero E, Augulis R, Novoderezhkin VI, Ferretti M, Thieme J, Zigmantas D, van Grondelle R
(2014) Quantum coherence in photosynthesis for efficient solar-energy conversion. Nat Phys
10(9):677–683. https ://doi.org/10.1038/nphys 3017
9. Scholes GD, Fleming GR, Olaya-Castro A, van Grondelle R (2011) Lessons from nature about
solar light harvesting. Nat Chem 3(10):763–774. https ://doi.org/10.1038/nchem .1145
10. Gueye M, Manathunga M, Agathangelou D, Orozco Y, Paolino M, Fusi S, Haacke S, Olivucci
M, Leonard J (2018) Engineering the vibrational coherence of vision into a synthetic molecular
device. Nat Commun 9:313. https ://doi.org/10.1038/s4146 7-017-02668 -w
11. Scholes GD, Fleming GR, Chen LX, Aspuru-Guzik A, Buchleitner A, Coker DF, Engel GS, van
Grondelle R, Ishizaki A, Jonas DM, Lundeen JS, McCusker JK, Mukamel S, Ogilvie JP, OlayaCastro A, Ratner MA, Spano FC, Whaley KB, Zhu XY (2017) Using coherence to enhance function in chemical and biophysical systems. Nature 543(7647):647–656. https ://doi.org/10.1038/
natur e2142 5
12. Rose TS, Rosker MJ, Zewail AH (1989) Femtosecond real-time probing of reactions. IV. The reactions of alkali halides. J Chem Phys 91(12):7415–7436
13. Pollard WT, Fragnito HL, Bigot JY, Shank CV, Mathies RA (1990) Quantum-mechanical theory for 6 fs dynamic absorption spectroscopy and its application to Nile blue. Chem Phys Lett
168(3):239–245. https ://doi.org/10.1016/0009-2614(90)85603 -A
14. Fragnito HL, Bigot JY, Becker PC, Shank CV (1989) Evolution of the vibronic absorption spectrum in a molecule following impulsive excitation with a 6 fs optical pulse. Chem Phys Lett
160(2):101–104. https ://doi.org/10.1016/0009-2614(89)87564 -5
15. Dhar L, Rogers JA, Nelson KA (1994) Time-resolved vibrational spectroscopy in the impulsive
limit. Chem Rev 94(1):157–193. https ://doi.org/10.1021/cr000 25a00 6
16. Ruhman S, Kosloff R (1990) Application of chirped ultrashort pulses for generating large-amplitude ground-state vibrational coherence: a computer simulation. J Opt Soc Am B 7(8):1748–1752.
https ://doi.org/10.1364/josab .7.00174 8
237
Reprinted from the journal