TY - JOUR
T1 - Proton-coupled energy transfer in molecular triads
AU - Rimgard, Belinda Pettersson
AU - Tao, Zhen
AU - Parada, Giovanny A.
AU - Cotter, Laura F.
AU - Hammes-Schiffer, Sharon
AU - Mayer, James M.
AU - Hammarström, Leif
N1 - Publisher Copyright:
© 2022 American Association for the Advancement of Science. All rights reserved.
PY - 2022/8/12
Y1 - 2022/8/12
N2 - 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 ~400 nanometers (nm), which led to fluorescence around 550 nm from the phenol-pyridine unit. Direct excitation of phenol-pyridine would have required ~330-nm light, but the coupled proton transfer within the phenol-pyridine 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.
AB - 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 ~400 nanometers (nm), which led to fluorescence around 550 nm from the phenol-pyridine unit. Direct excitation of phenol-pyridine would have required ~330-nm light, but the coupled proton transfer within the phenol-pyridine 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.
UR - http://www.scopus.com/inward/record.url?scp=85136339645&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85136339645&partnerID=8YFLogxK
U2 - 10.1126/science.abq5173
DO - 10.1126/science.abq5173
M3 - Article
C2 - 35862490
AN - SCOPUS:85136339645
SN - 0036-8075
VL - 377
SP - 742
EP - 747
JO - Science
JF - Science
IS - 6607
ER -