Nonlinear Optics and Carrier Dynamics in Nanostructured and Two-Dimensional Materials

Understanding and measuring the interaction of light with sub-wavelength structures and atomically thin materials is of critical importance for the development of next generation photonic devices.  One approach to achieve the desired optical properties in a material is to manipulate its mesoscopic structure or its composition in order to affect the properties of the light-matter interaction.  There has been tremendous recent interest in so called two-dimensional materials, consisting of only a single to a few layers of atoms arranged in a planar sheet.  These materials have demonstrated great promise as a platform for studying unique phenomena arising from the low-dimensionality of the material and for developing new types of devices based on these effects.  A thorough investigation of the optical and electronic properties of these new materials is essential to realizing their potential.  In this work we present studies that explore the nonlinear optical properties and carrier dynamics in nanoporous silicon waveguides, two-dimensional graphite (graphene), and atomically thin black phosphorus. We first present an investigation of the nonlinear response of nanoporous silicon optical waveguides using a novel pump-probe method. A two-frequency heterodyne technique is developed in order to measure the pump-induced transient change in phase and intensity in a single measurement. The experimental data reveal a characteristic material response time and temporally resolved intensity and phase behavior matching a physical model dominated by free-carrier effects that are significantly stronger and faster than those observed in traditional silicon-based waveguides.  These results shed light on the large optical nonlinearity observed in nanoporous silicon and demonstrate a new measurement technique for heterodyne pump-probe spectroscopy. Next we explore the optical properties of low-doped graphene in the terahertz spectral regime, where both intraband and interband effects play a significant role. Probing the graphene at intermediate photon energies enables the investigation of the nonlinear optical properties in the graphene as its electron system is heated by the intense pump pulse. By simultaneously measuring the reflected and transmitted terahertz light, a precise determination of the pump-induced change in absorption can be made. We observe that as the intensity of the terahertz radiation is increased, the optical properties of the graphene change from interband, semiconductor-like absorption, to a more metallic behavior with increased intraband processes. This transition reveals itself in our measurements as an increase in the terahertz transmission through the graphene at low fluence, followed by a decrease in transmission and the onset of a large, photo-induced reflection as fluence is increased.  A hybrid optical-thermodynamic model successfully describes our observations and predicts this transition will persist across mid- and far-infrared frequencies.  This study further demonstrates the important role that reflection plays since the absorption saturation intensity (an important figure of merit for graphene-based saturable absorbers) can be underestimated if only the transmitted light is considered. These findings are expected to contribute to the development of new optoelectronic devices designed to operate in the mid- and far-infrared frequency range.  Lastly we discuss recent work with black phosphorus, a two-dimensional material that has recently attracted interest due to its high mobility and direct, configurable band gap (300 meV to 2eV), depending on the number of atomic layers comprising the sample. In this work we examine the pump-induced change in optical transmission of mechanically exfoliated black phosphorus flakes using a two-color optical pump-probe measurement. The time-resolved data reveal a fast pump-induced transparency accompanied by a slower absorption that we attribute to Pauli blocking and free-carrier absorption, respectively. Polarization studies show that these effects are also highly anisotropic - underscoring the importance of crystal orientation in the design of optical devices based on this material. We conclude our discussion of black phosphorus with a study that employs this material as the active element in a photoconductive detector capable of gigahertz class detection at room temperature for mid-infrared frequencies.

COMPREHENSIVE ELECTRICAL/OPTICAL/THERMAL CHARACTERIZATIONS OF HIGH POWER LIGHT EMITTING DIODES AND LASER DIODES

Thermal characterizations of high power light emitting diodes (LEDs) and laser diodes (LDs) are one of the most critical issues to achieve optimal performance such as center wavelength, spectrum, power efficiency, and reliability. Unique electrical/optical/thermal characterizations are proposed to analyze the complex thermal issues of high power LEDs and LDs. First, an advanced inverse approach, based on the transient junction temperature behavior, is proposed and implemented to quantify the resistance of the die-attach thermal interface (DTI) in high power LEDs. A hybrid analytical/numerical model is utilized to determine an approximate transient junction temperature behavior, which is governed predominantly by the resistance of the DTI. Then, an accurate value of the resistance of the DTI is determined inversely from the experimental data over the predetermined transient time domain using numerical modeling. Secondly, the effect of junction temperature on heat dissipation of high power LEDs is investigated. The theoretical aspect of junction temperature dependency of two major parameters – the forward voltage and the radiant flux – on heat dissipation is reviewed. Actual measurements of the heat dissipation over a wide range of junction temperatures are followed to quantify the effect of the parameters using commercially available LEDs. An empirical model of heat dissipation is proposed for applications in practice. Finally, a hybrid experimental/numerical method is proposed to predict the junction temperature distribution of a high power LD bar. A commercial water-cooled LD bar is used to present the proposed method. A unique experimental setup is developed and implemented to measure the average junction temperatures of the LD bar. After measuring the heat dissipation of the LD bar, the effective heat transfer coefficient of the cooling system is determined inversely. The characterized properties are used to predict the junction temperature distribution over the LD bar under high operating currents. The results are presented in conjunction with the wall-plug efficiency and the center wavelength shift.