Size dependence of the third-order susceptibility of copper nanoclusters investigated by four-wave mixing

We report on the observation of the forward degenerate four-wave mixing in four composite samples with Cu nanoclusters embedded in fused silica. The mean diameters of the copper particles in the four samples were 5, 7, 10, and 13 nm. The independent tensor elements of optical Kerr susceptibility were measured with different wave-mixing polarizations by use of 35-ps laser pulses from a mode-locked, frequency-doubled Nd:YAG laser. The measured third-order susceptibilities were on the order of 10−9–10−8 esu; the response time of the nonlinearity is faster than the laser pulse duration. The experimental results are consistent with a d−3 size dependence predicted for quantum-confined conduction band electrons in Cu nanoclusters.

[1]  U. Kreibig The transition cluster-solid state in small gold particles , 1978 .

[2]  Fujimoto,et al.  Femtosecond studies of nonequilibrium electronic processes in metals. , 1987, Physical review letters.

[3]  P. Roussignol,et al.  Surface-mediated enhancement of optical phase conjugation in metal colloids. , 1985, Optics letters.

[4]  R. Doremus Optical Properties of Small Gold Particles , 1964 .

[5]  A. Smirl,et al.  Theory of degenerate four-wave mixing in picosecond excitation-probe experiments , 1983 .

[6]  W. Halperin,et al.  Quantum size effects in metal particles , 1986 .

[7]  Paul R. Ashley,et al.  Degenerate four-wave mixing in colloidal gold as a function of particle size , 1990 .

[8]  R. Zuhr,et al.  Picosecond nonlinear optical response of copper clusters created by ion implantation in fused silica , 1991 .

[9]  François Hache,et al.  Optical nonlinearities of small metal particles: surface-mediated resonance and quantum size effects , 1986 .

[10]  R. W. Christy,et al.  Optical Constants of the Noble Metals , 1972 .

[11]  Robert R. Alfano,et al.  Third-order optical nonlinearity in polycondensed thiophene-based polymers and polysilane polymers , 1989 .

[12]  G. Eesley,et al.  Generation of nonequilibrium electron and lattice temperatures in copper by picosecond laser pulses. , 1986, Physical review. B, Condensed matter.

[13]  François Hache,et al.  The optical kerr effect in small metal particles and metal colloids: The case of gold , 1988 .

[14]  Gary M. Carter,et al.  Excited-state dynamics and temporally resolved nonresonant nonlinear-optical processes in polydiacetylenes , 1987 .

[15]  Taylor,et al.  Ultraviolet photoelectron spectra of mass-selected copper clusters: Evolution of the 3d band. , 1990, Physical review letters.

[16]  Changes in the refractive index of fused silica due to implantation of transition-metal ions , 1991 .