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Optical Nonlinearity in CdSSe Microcrystallites Embedded in Glasses
IEICE TRANSACTIONS on Electronics
Publication Date: 2007/01/01
Online ISSN: 1745-1353
Print ISSN: 0916-8516
Type of Manuscript: Special Section PAPER (Special Section on Microoptomechatronics)
Category: Advanced Nano Technologies
optical nonlinearity, semiconductor microcrystallites, CdSSe, optical non-linear efficiency, σeff, carrier recombination time, τ, energy relaxation time, T1, phase relaxation time, T2,
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We investigate the enhancement of the optical nonlinearity and the limit of the improvement of the response speed in CdSxSe1-x microcrystallites by measuring the effective optical nonlinear cross section (σeff), the energy decay time (T1) and the dephasing time in two kinds of semiconductor microcrystallites of CdS0.12Se0.8 microcrystallites embedded in alkaline multi-component glasses (CdSSeMs) and CdSe microcrystallites embedded in SiO2 thin film (CdSeMs). As the average radius of CdSSeMs decreases from 10 to 1 nm, the values of σeff and T1 gradually change from 2.610-16 to 1.110-16 cm2 and from dozens picoseconds to 4 psec, respectively. The size dependence of CdSSEMs shows that the energy level structure in the microcrystallite with a radius of less than a few nanometers is a two-level system, in which σeff is proportional to T2. The carrier recombination time (τ) of CdSSeMs with the average radius of 1 nm is estimated to 2 psec. As the average radius of a CdS0.12Se0.8 microcrystallite decreases from 9 to 3 nm, the values of T2 gradually change from 640 to 230 fsec at 18 K, respectively. The size and temperature dependences of T2 for the CdSSeMs show that there is the discrepancy between the theory and the measured T2. The discrepancy showes the presence of the acoustic-phonon-assisted relaxation processes other than the pure-dephasing processes. It is indicated that T2 becomes long by reducing the excessive acoustic-phonon-assisted relaxation processes, and that the longer T2 might enhance σeff. We investigate the enhancement of σeff in CdSeMs by making T2 longer. The τ, σeff, and T2 of CdSeM an average radius of 3 nm are 40 psec, 4.510-15 cm2, and 150 fsec at room temperature. The σeff is ten times as large as that of CdSSeM sample at the same average radius and the enhancement of σeff can be considered to be caused by the longer T2.