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- W3112450417 abstract "Two-photon excitation is an attractive means for controlling chemistry in both space and time. Isoenergetic one- and two-photon excitations (OPE and TPE) in non-centrosymmetric molecules are often assumed to reach the same excited state and, hence, to produce similar excited-state reactivity. We compare the solvent-to-solute excited-state proton transfer of the super photobase FR0-SB following isoenergetic OPE and TPE. We find up to 62 % increased reactivity following TPE compared to OPE. From steady-state spectroscopy, we rule out the involvement of different excited states and find that OPE and TPE spectra are identical in non-polar solvents but not in polar ones. We propose that differences in the matrix elements that contribute to the two-photon absorption cross sections lead to the observed enhanced isoenergetic reactivity, consistent with the predictions of our high-level coupled-cluster-based computational protocol. We find that polar solvent configurations favor greater dipole moment change between ground and excited states, which enters the probability for two-photon excitations as the absolute value squared. This, in turn, causes a difference in the Franck-Condon region reached via TPE compared to OPE. We conclude that a new method has been found for controlling chemical reactivity via the matrix elements that affect two-photon cross sections, which may be of great utility for spatial and temporal precision chemistry." @default.
- W3112450417 created "2020-12-21" @default.
- W3112450417 creator A5001291968 @default.
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- W3112450417 date "2020-12-14" @default.
- W3112450417 modified "2023-10-13" @default.
- W3112450417 title "Isoenergetic two-photon excitation enhances solvent-to-solute excited-state proton transfer" @default.
- W3112450417 cites W1695379209 @default.
- W3112450417 cites W1844067222 @default.
- W3112450417 cites W1907088169 @default.
- W3112450417 cites W1943394565 @default.
- W3112450417 cites W1965848428 @default.
- W3112450417 cites W1968765476 @default.
- W3112450417 cites W1969874566 @default.
- W3112450417 cites W1972357461 @default.
- W3112450417 cites W1973357698 @default.
- W3112450417 cites W1982164127 @default.
- W3112450417 cites W1984139317 @default.
- W3112450417 cites W1985175271 @default.
- W3112450417 cites W1985793906 @default.
- W3112450417 cites W1986570904 @default.
- W3112450417 cites W1989274860 @default.
- W3112450417 cites W2003668889 @default.
- W3112450417 cites W2007849368 @default.
- W3112450417 cites W2009442202 @default.
- W3112450417 cites W2011215428 @default.
- W3112450417 cites W2012458244 @default.
- W3112450417 cites W2012718683 @default.
- W3112450417 cites W2019394610 @default.
- W3112450417 cites W2030976617 @default.
- W3112450417 cites W2035312164 @default.
- W3112450417 cites W2037061986 @default.
- W3112450417 cites W2038122764 @default.
- W3112450417 cites W2043325406 @default.
- W3112450417 cites W2044945447 @default.
- W3112450417 cites W2046031057 @default.
- W3112450417 cites W2046412723 @default.
- W3112450417 cites W2048834113 @default.
- W3112450417 cites W2050065698 @default.
- W3112450417 cites W2059645026 @default.
- W3112450417 cites W2060711224 @default.
- W3112450417 cites W2062192056 @default.
- W3112450417 cites W2062852634 @default.
- W3112450417 cites W2063070241 @default.
- W3112450417 cites W2064375314 @default.
- W3112450417 cites W2066481445 @default.
- W3112450417 cites W2068517321 @default.
- W3112450417 cites W2069736521 @default.
- W3112450417 cites W2070574667 @default.
- W3112450417 cites W2075701819 @default.
- W3112450417 cites W2075723505 @default.
- W3112450417 cites W2076940601 @default.
- W3112450417 cites W2079053731 @default.
- W3112450417 cites W2079790823 @default.
- W3112450417 cites W2089682437 @default.
- W3112450417 cites W2090391132 @default.
- W3112450417 cites W2090572943 @default.
- W3112450417 cites W2091723156 @default.
- W3112450417 cites W2093171685 @default.
- W3112450417 cites W2094642658 @default.
- W3112450417 cites W2102945356 @default.
- W3112450417 cites W2109931506 @default.
- W3112450417 cites W2118997899 @default.
- W3112450417 cites W2128583282 @default.
- W3112450417 cites W2135618296 @default.
- W3112450417 cites W2136006749 @default.
- W3112450417 cites W2147607085 @default.
- W3112450417 cites W2164318957 @default.
- W3112450417 cites W2167460696 @default.
- W3112450417 cites W2202808915 @default.
- W3112450417 cites W2230728100 @default.
- W3112450417 cites W2331608584 @default.
- W3112450417 cites W2331840255 @default.
- W3112450417 cites W2407448655 @default.
- W3112450417 cites W2467607937 @default.
- W3112450417 cites W2501886121 @default.
- W3112450417 cites W2511344474 @default.
- W3112450417 cites W2564756703 @default.
- W3112450417 cites W2582615419 @default.
- W3112450417 cites W2765237238 @default.
- W3112450417 cites W2888899123 @default.
- W3112450417 cites W2889722145 @default.
- W3112450417 cites W2972821904 @default.
- W3112450417 cites W2973790612 @default.
- W3112450417 cites W3017260797 @default.
- W3112450417 cites W3048872476 @default.
- W3112450417 cites W4211056227 @default.
- W3112450417 doi "https://doi.org/10.1063/5.0020282" @default.