ELSEVIER Surface Science386 (1997) 245-248
surface science
Deposition of photo-generated mixed-valent Fe(II)-Fe(III)
complexes at the surface of Langmuir monolayers
Nobuo Kimizuka *, Tsutomu Asai, Shinji Ohno, Kunitaka Fujiyoshi, Toyoki Kunitake
Department of Chemical Science and Technology, Faculty of Engineering, Kyushu University, Fukuoka 812, Japan
Received5 November1996;acceptedfor publication 26 February 1997
Abstract
A mixed-valentFe(II) Fe(III) complexwas deposited at the surface of cationic monolayersby photoirradiation of the aqueous
subphase containing equimolar Fe 3÷ and Fe(CN)3- ions. The photo-depositionprocesswas detected in situ by the measurement of
reflectance spectra at the air-water interface at a constant surface pressure. The present technique provides a first example of the
photo-induced mineralizationprocess at the air-water interface. © 1997 ElsevierScienceB.V.
Keywords." Iron; Liquid-gas interfaces; Physical adsorption; Reflectionspectroscopy;Self-assembly
1. Introduction
Biomimetic fabrication of inorganic materials
that are directed by organic molecular assemblies
have been attracting much interest, because they
provide useful approaches to control the inorganic
nanostructures [1,2]. We have reported that
macroscopically oriented self-supporting films
were obtained by casting aqueous dispersions of a
lipid bilayer membrane [3], and these multibilayer
films provide two-dimensional matrices for the
preparation of molecularly controlled polysiloxane
networks [4], metal oxides [5], quantized cadmium
sulfides [6], lead halide clusters [7] and bimetallic
/~-cyano complexes [8]. In these studies, inorganic
nanostructures are regulated by the two-dimen-
sional space of the host multibilayer, as well as by
electrostatic and van der Waals interactions acting
* Correspondingauthor. Tel.: (+ 81) 92 642.3597;fax: (+ 81)
92 642.3611;e-mail: kimitcm@mbox.nc.kyushu-u.ac.jp
0039-6028/97/$17.00© 1997ElsevierScience B.V. All rights reserved.
Pll S0039-6028 (9 7 ) 00322- I
at bilayer surfaces. Langmuir monolayers provide
another class of molecular templates which enable
oriented nucleation of inorganic crystals [9], semi-
conductor particles [10] and electrochemically gen-
erated metal particles [11]. However, there has
been no report on photo-regulation of the mono-
layer-directed mineralization process. In this
paper, we report a novel photo-induced deposition
process of a #-cyano Fe (II)-Fe (III) mixed-valent
complex at the monolayer surface. #-Cyano bime-
tallic complexes are known as catalysts for water
photolysis [12] and were recently highlighted as
photo-responsible molecule-based magnets [13].
2. Experimental
Preparation of ammonium amphiphile 1 (see
Scheme 1) has been described previously [14]. The
pressure-area isotherms of the surface monolayer
(rc-A curve) were measured with a computer-
controlled film balance (USI system, model FSD-