Studying Molecular Rearrangement of P1 Dye at a Passivating Alumina Surface Using Vibrational Sum‐Frequency Generation Spectroscopy: Effect of Atomic‐Level Roughness

GND
1310156980
ORCID
0000-0002-5125-5252
Affiliation
Department of Functional Interfaces Leibniz Institute of Photonic Technology Jena Albert-Einstein-Strasse 9 07745 Jena Germany
De, Ratnadip;
GND
1331485541
Affiliation
Department of Functional Interfaces Leibniz Institute of Photonic Technology Jena Albert-Einstein-Strasse 9 07745 Jena Germany
Bera, Anupam;
GND
1331486041
Affiliation
Department of Functional Interfaces Leibniz Institute of Photonic Technology Jena Albert-Einstein-Strasse 9 07745 Jena Germany
Schmidt, Heiner;
GND
1214845479
ORCID
0000-0002-3598-7656
Affiliation
Institute of Physical Chemistry Friedrich Schiller University Jena Helmholtzweg 4 07743 Jena Germany
Neumann, Christof;
GND
123088747
Affiliation
Department of Functional Interfaces Leibniz Institute of Photonic Technology Jena Albert-Einstein-Strasse 9 07745 Jena Germany
Paa, Wolfgang;
Affiliation
Department of Functional Interfaces Leibniz Institute of Photonic Technology Jena Albert-Einstein-Strasse 9 07745 Jena Germany
Gawlik, Annett;
GND
1213543223
ORCID
0000-0003-2388-1042
Affiliation
Institute of Physical Chemistry Friedrich Schiller University Jena Helmholtzweg 4 07743 Jena Germany
Turchanin, Andrey;
GND
131343971
Affiliation
Department of Functional Interfaces Leibniz Institute of Photonic Technology Jena Albert-Einstein-Strasse 9 07745 Jena Germany
Dietzek‐Ivanšić, Benjamin

Abstract The effect of roughness and thickness of alumina layers, mimicking the passivation layer commonly used in dye‐sensitized photoelectrodes, on the molecular adsorption of P1 dye, 4‐(bi(4‐(2,2‐dicyano‐vinyl)‐thiophene‐2‐yl]‐phenyl]‐aminobenzoic acid) has been studied using surface‐sensitive vibrational sum frequency generation(VSFG) spectroscopy. The VSFG spectra reveal the formation of poorly ordered dye layers on relatively rough surfaces where XPS measures a higher dye loading. Furthermore, these poorly ordered dye molecules are responsible for the generation of trapped electronic states as probed by successive photoluminescence (PL) measurements. Surface sensitive VSFG spectroscopy in combination with XPS and PL measurements provide complementary spectral information on ordering of the adsorbed dyes, their density on the surface and electronic states of the adsorbed monolayer which are prerequisite for improving our understanding of molecularly functionalized photoelectrodes and their further development.

A combined experimental method involving vibrational‐sum frequency generation spectroscopy, X‐ray photoelectron spectroscopy and photoluminescent measurements is employed to investigate the molecular ordering and packing density at the surface of a molecularly functionalized model photoelectrode. Poorly ordered molecular assembly on atomically rough surfaces is observed, which is responsible for the formation of trapped electronic states at the dye‐electrode interface. image

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