Proton-coupled energy transfer in molecular triads

被引:19
作者
Rimgard, Belinda Pettersson [1 ]
Tao, Zhen [2 ,4 ]
Parada, Giovanny A. [2 ,3 ]
Cotter, Laura F. [2 ]
Hammes-Schiffer, Sharon [2 ]
Mayer, James M. [2 ]
Hammarstrom, Leif [1 ]
机构
[1] Uppsala Univ, Dept Chem, Angstrom Lab, SE-75120 Uppsala, Sweden
[2] Yale Univ, Dept Chem, New Haven, CT 06520 USA
[3] Coll New Jersey, Dept Chem, Ewing, NJ 08628 USA
[4] Univ Penn, Dept Chem, Philadelphia, PA 19104 USA
基金
瑞典研究理事会;
关键词
ELECTRON-TRANSFER; TRANSFER ESIPT; STATE;
D O I
10.1126/science.abq5173
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
We experimentally discovered and theoretically analyzed a photochemical mechanism, which we term proton-coupled energy transfer (PCEnT). A series of anthracene-phenol-pyridine triads formed a local excited anthracene state after light excitation at a wavelength of similar to 400 nanometers (nm), which led to fluorescence around 550 nm from the phenol-pyridine unit. Direct excitation of phenolpyridine would have required similar to 330-nm light, but the coupled proton transfer within the phenolpyridine unit lowered its excited-state energy so that it could accept excitation energy from anthracene. Singlet-singlet energy transfer thus occurred despite the lack of spectral overlap between the anthracene fluorescence and the phenol-pyridine absorption. Moreover, theoretical calculations indicated negligible charge transfer between the anthracene and phenol-pyridine units. We construe PCEnT as an elementary reaction of possible relevance to biological systems and future photonic devices.
引用
收藏
页码:742 / 746
页数:5
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共 30 条
  • [1] Intraprotein radical transfer during photoactivation of DNA photolyase
    Aubert, C
    Vos, MH
    Mathis, P
    Eker, APM
    Brettel, K
    [J]. NATURE, 2000, 405 (6786) : 586 - 590
  • [2] Activationless Multiple-Site Concerted Proton-Electron Tunneling
    Bowring, Miriam A.
    Bradshaw, Liam R.
    Parada, Giovanny A.
    Pollock, Timothy P.
    Fernandez-Teran, Ricardo J.
    Kolmar, Scott S.
    Mercado, Brandon Q.
    Schlenker, Cody W.
    Gamelin, Daniel R.
    Mayer, James M.
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2018, 140 (24) : 7449 - 7452
  • [3] NEW ULTRAVIOLET STABILIZERS - 3-(2'-HYDROXYPHENYL)PYRAZOLE AND 5-(2'-HYDROXYPHENYL)PYRAZOLE
    CATALAN, J
    FABERO, F
    CLARAMUNT, RM
    MARIA, MDS
    FOCESFOCES, MDC
    CANO, FH
    MARTINEZRIPOLL, M
    ELGUERO, J
    SASTRE, R
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1992, 114 (13) : 5039 - 5048
  • [4] Solvent and Temperature Effects on Photoinduced Proton-Coupled Electron Transfer in the Marcus Inverted Region
    Cotter, Laura F.
    Rimgard, Belinda Pettersson
    Parada, Giovanny A.
    Mayer, James M.
    Hammarstrom, Leif
    [J]. JOURNAL OF PHYSICAL CHEMISTRY A, 2021, 125 (35) : 7670 - 7684
  • [5] Excited-state proton coupled charge transfer modulated by molecular structure and media polarization
    Demchenko, Alexander P.
    Tang, Kuo-Chun
    Chou, Pi-Tai
    [J]. CHEMICAL SOCIETY REVIEWS, 2013, 42 (03) : 1379 - 1408
  • [6] Driving Force Dependence of Rates for Nonadiabatic Proton and Proton-Coupled Electron Transfer: Conditions for Inverted Region Behavior
    Edwards, Sarah J.
    Soudackov, Alexander V.
    Hammes-Schiffer, Sharon
    [J]. JOURNAL OF PHYSICAL CHEMISTRY B, 2009, 113 (44) : 14545 - 14548
  • [7] Analytic derivative couplings between configuration-interaction-singles states with built-in electron-translation factors for translational invariance
    Fatehi, Shervin
    Alguire, Ethan
    Shao, Yihan
    Subotnik, Joseph E.
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2011, 135 (23)
  • [8] PHOTOINDUCED ELECTRON-TRANSFER IN THE SOLID-STATE - RATE VS FREE-ENERGY DEPENDENCE IN FIXED-DISTANCE PORPHYRIN ACCEPTOR MOLECULES
    GAINES, GL
    ONEIL, MP
    SVEC, WA
    NIEMCZYK, MP
    WASIELEWSKI, MR
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1991, 113 (02) : 719 - 721
  • [9] Theory of Coupled Electron and Proton Transfer Reactions
    Hammes-Schiffer, Sharon
    Stuchebrukhov, Alexei A.
    [J]. CHEMICAL REVIEWS, 2010, 110 (12) : 6939 - 6960
  • [10] Enhanced Rigidification within a Double Mutant of Soybean Lipoxygenase Provides Experimental Support for Vibronically Nonadiabatic Proton-Coupled Electron Transfer Models
    Hu, Shenshen
    Soudackov, Alexander V.
    Hammes-Schiffer, Sharon
    Klinman, Judith P.
    [J]. ACS CATALYSIS, 2017, 7 (05): : 3569 - 3574