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Roles of Plasmonic Excitation and Protonation on Photoreactions of p-Aminobenzenethiol on Ag Nanoparticles
KTH, Skolan för bioteknologi (BIO), Teoretisk kemi och biologi.ORCID-id: 0000-0002-3282-0711
KTH, Skolan för bioteknologi (BIO), Teoretisk kemi och biologi.
KTH, Skolan för bioteknologi (BIO), Teoretisk kemi och biologi.ORCID-id: 0000-0003-0007-0394
2014 (Engelska)Ingår i: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 118, nr 13, s. 6893-6902Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

There is increasing evidence that surface plasmons could catalyze photochemical reactions of organic molecules on metal surfaces. However, due to the complex interactions among the substrate, the adsorbate, the environment, and the incident light, the existence and the underlying mechanism of such catalytic processes have been under intense debate. Here we present a systematic first principles study on one of the most studied and controversial systems, namely, p-aminobenzenethiol (PATP) adsorbed on silver nanoparticles. Our calculations have confirmed that the observed surface-enhanced Raman scattering (SERS) bands at 1142, 1391, and 1440 cm(-1) of PATP on silver surfaces belong to its coupling reaction product, 4,4'-dimercaptoazobenzene (DMAB). It is found that the deprotonation or protonation of N atoms is the key initial step for the transformations between PATP and DMAB. The photodecomposition reaction from DMAB to PATP can occur only under the conditions that both proton transfer and plasmonic excitations have taken place. Moreover, in addition to the widely suggested hot-electron injection mechanism of plasmon, a new photochemical channel has been revealed in the decomposition of DMAB molecules under suitable incident light. This may open up an entire new type of chemical reaction in surface chemistry that we call plasmonic photochemistry. Our theoretical calculations provide consistent interpretations for the experimentally observed pH-,wavelength-,and electrode potential dependence of the SERS spectra of PATP/DMAB adsorbed on silver surfaces. Our findings highlight the important role of theoretical investigations for better understanding of complex processes involved in photochemical reaction of surface adsorbates.

Ort, förlag, år, upplaga, sidor
American Chemical Society (ACS), 2014. Vol. 118, nr 13, s. 6893-6902
Nyckelord [en]
Electrode potentials, First-principles study, Photo-decomposition, Silver nanoparticles, Surface adsorbates, Surface enhanced Raman Scattering (SERS), Theoretical calculations, Theoretical investigations
Nationell ämneskategori
Fysikalisk kemi
Identifikatorer
URN: urn:nbn:se:kth:diva-145587DOI: 10.1021/jp500728sISI: 000334258600040Scopus ID: 2-s2.0-84898077395OAI: oai:DiVA.org:kth-145587DiVA, id: diva2:719286
Anmärkning

QC 20140523

Tillgänglig från: 2014-05-23 Skapad: 2014-05-23 Senast uppdaterad: 2017-12-05Bibliografiskt granskad
Ingår i avhandling
1. Theoretical Study on Chemical Structures and Stability of Molecules in Metallic Junctions
Öppna denna publikation i ny flik eller fönster >>Theoretical Study on Chemical Structures and Stability of Molecules in Metallic Junctions
2016 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

In this thesis, we focus on the structural identification of the interface using surface enhanced Raman spectroscopy (SERS) and inelastic electron tunnelling scattering (IETS). Two different molecular junctions, namely gold/ trans-1,2-bis (4-pyridyl) ethylene/gold junction and gold/4,4'-bipyridine/gold junctions in various conditions were studied and the corresponding configurations were determined. The enhancement in SERS was also studied by employing the time-dependent density functional theory. Furthermore, we studied some properties of the interface, such as the stability of the adsorbates and charge transfer properties of molecular junctions. The decrease in the stability of molecules was found when adsorbed on metallic surface and trapped in metallic junctions. Our studies explained several puzzles and by rational design, more stable molecular devices were obtained.

Ort, förlag, år, upplaga, sidor
Stockholm, Sweden: KTH Royal Institute of Technology, 2016. s. 71
Serie
TRITA-BIO-Report, ISSN 1654-2312 ; 2016:12
Nyckelord
SERS, IETS, Interface, Chemical Stability
Nationell ämneskategori
Naturvetenskap Kemi Teoretisk kemi
Forskningsämne
Teoretisk kemi och biologi
Identifikatorer
urn:nbn:se:kth:diva-185947 (URN)978-91-7595-992-4 (ISBN)
Disputation
2016-05-25, FA32, Roslagstullsbacken 21, Stockholm, 10:00 (Engelska)
Opponent
Handledare
Tillgänglig från: 2016-04-29 Skapad: 2016-04-29 Senast uppdaterad: 2016-04-29Bibliografiskt granskad

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Duan, SaiLuo, Yi

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The Journal of Physical Chemistry C
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Totalt: 83 träffar
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