The optimal deposition condition of chlorophyll a (Chl a) Langmuir-Blodgett (LB) film were investigated based on pi-a isotherms, absorption spectrum and scanning tunneling microscopy (STM) observation. The pi-a isotherms of Chl a LB film at various air temperatures and subphase pHs were obtained. Optimum temperature and pH for dense packing of Chl a LB layers are 25 degreesC and 7.0, respectively. The formation of J- and H-aggregations of the ordered chlorophyll a molecules was confirmed by absorption spectrum measurements. The well-ordered structure of Chl a LB layer was observed by STM. Thus, the densely packed Chl a LB layer could be fabricated by the proposed optimal deposition condition. (C) 2003 Elsevier B.V. All rights reserved.