Institute of Chemistry and the Center for Nanoscience & Nanotechnology, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
ACS Nano. 2011 Jun 28;5(6):4712-9. doi: 10.1021/nn200645h. Epub 2011 Jun 7.
The optical response of hybrid metal-semiconductor nanoparticles exhibits different behaviors due to the proximity between the disparate materials. For some hybrid systems, such as CdS-Au matchstick-shaped hybrids, the particles essentially retain the optical properties of their original components, with minor changes. Other systems, such as CdSe-Au dumbbell-shaped nanoparticles, exhibit significant change in the optical properties due to strong coupling between the two materials. Here, we study the absorption of these hybrids by comparing experimental results with simulations using the discrete dipole approximation method (DDA) employing dielectric functions of the bare components as inputs. For CdS-Au nanoparticles, the DDA simulation provides insights on the gold tip shape and its interface with the semiconductor, information that is difficult to acquire by experimental means alone. Furthermore, the qualitative agreement between DDA simulations and experimental data for CdS-Au implies that most effects influencing the absorption of this hybrid system are well described by local dielectric functions obtained separately for bare gold and CdS nanoparticles. For dumbbell shaped CdSe-Au, we find a shortcoming of the electrodynamic model, as it does not predict the "washing out" of the optical features of the semiconductor and the metal observed experimentally. The difference between experiment and theory is ascribed to strong interaction of the metal and semiconductor excitations, which spectrally overlap in the CdSe case. The present study exemplifies the employment of theoretical approaches used to describe the optical properties of semiconductors and metal nanoparticles, to achieve better understanding of the behavior of metal-semiconductor hybrid nanoparticles.
由于不同材料之间的接近,混合金属-半导体纳米粒子的光学响应表现出不同的行为。对于一些混合系统,如 CdS-Au 棒状混合体,粒子基本上保留了其原始组件的光学性质,只有微小的变化。其他系统,如 CdSe-Au 哑铃状纳米粒子,由于两种材料之间的强耦合,其光学性质发生显著变化。在这里,我们通过将实验结果与使用离散偶极近似方法(DDA)进行的模拟进行比较来研究这些混合体的吸收,该方法使用裸组件的介电函数作为输入。对于 CdS-Au 纳米粒子,DDA 模拟提供了有关金尖端形状及其与半导体界面的信息,这些信息很难仅通过实验手段获得。此外,DDA 模拟与 CdS-Au 实验数据之间的定性一致性表明,影响该混合系统吸收的大多数效应都可以通过分别针对裸金和 CdS 纳米粒子获得的局部介电函数很好地描述。对于哑铃状 CdSe-Au,我们发现电动力学模型存在一个缺点,因为它不能预测实验中观察到的半导体和金属的“冲洗”光学特征。实验与理论之间的差异归因于金属和半导体激发的强烈相互作用,在 CdSe 情况下,它们在光谱上重叠。本研究示例说明了用于描述半导体和金属纳米粒子光学性质的理论方法的应用,以更好地理解金属-半导体混合纳米粒子的行为。