title: Unraveling Surface Plasmon Decay in Core-Shell Nanostructures toward Broadband Light-Driven Catalytic Organic Synthesis.
abstract: Harnessing surface plasmon of metal nanostructures to promote catalytic organic synthesis holds great promise in solar-to-chemical energy conversion. High conversion efficiency relies not only on broadening the absorption spectrum but on coupling the harvested energy into chemical reactions. Such coupling undergoes hot-electron transfer and photothermal conversion during the decay of surface plasmon; however, the two plasmonic effects are unfortunately entangled, making their individual roles still under debate. Here, we report that in a model system of bimetallic Au-Pd core-shell nanostructures the two effects can be disentangled through tailoring the shell thickness at atomic-level precision. As demonstrated by our ultrafast absorption spectroscopy characterizations, the achieved tunability of the two effects in a model reaction of Pd-catalyzed organic hydrogenation offers a knob for enhancing energy coupling. In addition, the two intrinsic plasmonic modes at 400-700 and 700-1000 nm in the bar-shaped nanostructures allow for utilizing photons to a large extent in full solar spectrum. This work establishes a paradigmatic guidance toward designing plasmonic-catalytic nanomaterials for enhanced solar-to-chemical energy conversion.
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), Synergetic Innovation Center of Quantum Information & Quantum Physics, and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, People's Republic of China.
authors.forename: Hao
authors.initials: H
authors.lastname: Huang
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), Synergetic Innovation Center of Quantum Information & Quantum Physics, and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, People's Republic of China.
authors.forename: Lei
authors.initials: L
authors.lastname: Zhang
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), Synergetic Innovation Center of Quantum Information & Quantum Physics, and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, People's Republic of China.
authors.forename: Zhiheng
authors.initials: Z
authors.lastname: Lv
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), Synergetic Innovation Center of Quantum Information & Quantum Physics, and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, People's Republic of China.
authors.forename: Ran
authors.initials: R
authors.lastname: Long
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, People's Republic of China.
authors.forename: Chao
authors.initials: C
authors.lastname: Zhang
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), Synergetic Innovation Center of Quantum Information & Quantum Physics, and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, People's Republic of China.
authors.forename: Yue
authors.initials: Y
authors.lastname: Lin
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), Synergetic Innovation Center of Quantum Information & Quantum Physics, and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, People's Republic of China.
authors.forename: Kecheng
authors.initials: K
authors.lastname: Wei
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), Synergetic Innovation Center of Quantum Information & Quantum Physics, and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, People's Republic of China.
authors.forename: Chengming
authors.initials: C
authors.lastname: Wang
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), Synergetic Innovation Center of Quantum Information & Quantum Physics, and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, People's Republic of China.
authors.forename: Lu
authors.initials: L
authors.lastname: Chen
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, People's Republic of China.|College of Physics and Optoelectronics, South China University of Technology , Guangzhou, Guangdong 510641, China.
authors.forename: Zhi-Yuan
authors.initials: ZY
authors.lastname: Li
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), Synergetic Innovation Center of Quantum Information & Quantum Physics, and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, People's Republic of China.
authors.forename: Qun
authors.initials: Q
authors.lastname: Zhang
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), Synergetic Innovation Center of Quantum Information & Quantum Physics, and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, People's Republic of China.
authors.forename: Yi
authors.initials: Y
authors.lastname: Luo
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), Synergetic Innovation Center of Quantum Information & Quantum Physics, and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, People's Republic of China.
authors.forename: Yujie
authors.initials: Y
authors.lastname: Xiong