The technique of femtosecond four-wave mixing is described, including spectrally-resolved and time-resolved configurations. We illustrate the utility of this technique for the investigation of crucial physical properties in the III-V diluted magnetic semiconductors, afforded by its nonlinearity and high temporal resolution.
The application of femtosecond four-wave mixing to the study of fundamental properties of diluted magnetic semiconductors ((s,p)-d hybridization, spin-flip scattering) is described, using experiments on GaMnAs as a prototype III-Mn-V system. Spectrally-resolved and time-resolved experimental configurations are described, including the use of zero-background autocorrelation techniques for pulse optimization. The etching process used to prepare GaMnAs samples for four-wave mixing experiments is also highlighted. The high temporal resolution of this technique, afforded by the use of short (20 fsec) optical pulses, permits the rapid spin-flip scattering process in this system to be studied directly in the time domain, providing new insight into the strong exchange coupling responsible for carrier-mediated ferromagnetism. We also show that spectral resolution of the four-wave mixing signal allows one to extract clear signatures of (s,p)-d hybridization in this system, unlike linear spectroscopy techniques. This increased sensitivity is due to the nonlinearity of the technique, which suppresses defect-related contributions to the optical response. This method may be used to measure the time scale for coherence decay (tied to the fastest scattering processes) in a wide variety of semiconductor systems of interest for next generation electronics and optoelectronics.
III-V diluted magnetic semiconductors exhibit ferromagnetic coupling mediated by carriers (holes), permitting external manipulation of magnetic characteristics using electrical and optical control of the carrier population. This feature makes these materials attractive for a whole host of magneto-sensitive electronic and optoelectronic devices1-15, including the possible integration of logic and memory.11-15 Realizing such applications requires a good understanding of the fundamental properties of these materials; however, the large density of defects associated with their growth at low temperatures (essential for the substitutional incorporation of magnetic dopants such as Mn) severely complicates the theoretical treatment of exchange coupling and ferromagnetic order16-18. These defects also impede the interpretation of transport and linear optical experiments on these materials19-24.
The utility of the nonlinear optical technique of four-wave mixing spectroscopy for gaining new insight into these materials was recently revealed in experiments on GaMnAs25,26, representing the prototype III-V diluted magnetic semiconductor. The nonlinearity of the technique was shown to provide a much greater sensitivity to fine structure in the optical joint density of states, indicating a strong enhancement of the interband optical response with the incorporation of Mn25. This observation is a signature of (s,p)-d hybridization that had been recently predicted in tight-binding calculations18. This new insight was afforded by the low optical dipole moment associated with transitions involving the mid-gap defect states, which mask these effects of hybridization in linear optical experiments27. The high time-resolution of the four-wave mixing technique has also been used to obtain the first direct measurement of the time-scale of hole-Mn spin flip scattering in this system26, providing new insight into exchange coupling. These experiments also showed that the optical response of this material is a photon echo, indicating that the dephasing time is independent of carrier energy despite defect-induced localization.
Here we present a detailed description of the four-wave mixing technique used in references25,26, illustrating how it may be used to measure the dephasing time (T2), the nonlinear (third-order) spectral response, and the nature of broadening (homogeneous or inhomogeneous) in a material of interest. Spectrally-resolved and temporally-resolved experimental configurations are featured, together with an explanation of the zero-background autocorrelation technique used in conjunction with a prism compressor to minimize the pulse duration at the sample position. This pulse duration determines the overall time-resolution of the technique and must be below 30 fsec to resolve spin-flip scattering in GaMnAs. The etching process used to prepare the GaMnAs samples for experiments in the transmission geometry is also highlighted. This work builds upon the established utility of four-wave mixing techniques for studying scattering processes and many-body effects in traditional semiconductors28-32 by extending it to the investigation of fundamental interactions and electronic structure in diluted magnetic semiconductors. Our results will have implications for the long-term engineering of these novel magnetic materials.
The four-wave mixing technique may be used to measure the time scale for coherence decay on optical transitions in a wide range of material systems. For a variety of applications in advanced electronics and optoelectronics, this dephasing time is of crucial importance. For instance, in quantum computing applications (for which exciton transitions in semiconductors represent the fundamental quantum bit in several proposals36-38), the dephasing time determines the temporal window during which quantum operations and error correction must be carried out. The time scale for coherence decay is dictated by the fastest scattering processes of electrons and holes in the material, and so measurements of the dephasing time also provide insight into the nature and strength of the associated interactions responsible for these fast scattering processes. The type of interactions involved will depend strongly on the semiconductor system under study, and will govern both transport and coherence decay in any device application using this material. The four-wave mixing method therefore provides an important tool to characterize materials of interest for next generation electronic and optoelectronic devices. In such studies, the time-resolution is the most important limitation. This resolution is dictated by the optical pulse duration, which must be shorter than the dephasing time in the material under study. The specific experimental configuration described here is ideally applied to the study of fast decay processes (< a few picoseconds in duration). For measurement of slower temporal dynamics, lock-in detection methods and a slow-scanning delay stage with a larger range of motion are commonly employed.
Here we elucidate the utility of this technique for the investigation of III-V diluted magnetic semiconductors, in which strong hole-Mn exchange coupling leads to carrier-mediated ferromagnetism. Spin-flip scattering between holes and Mn ions is also caused by the hole-Mn exchange interaction. We have shown that four-wave mixing techniques may be used to obtain a direct measurement of the time scale of this process, providing insight into exchange coupling in this important class of materials. We have also shown that the nonlinearity of the four-wave mixing technique provides a highly sensitive probe of the band edge states in these materials, providing clear signatures of the (s,p)-d hybridization process that is the origin of the strong exchange coupling in this system. The increased sensitivity of four-wave mixing relative to linear optical techniques (e.g. absorption, ellipsometry, magnetic circular dichroism) to these band edge states stems from the nonlinearity of this technique, which suppresses defect-related contributions to the optical response.
This work lays the foundation for applications of this technique to study key physical properties of interest, such as the electronic structure and exchange coupling, in a wide range of III-V diluted magnetic semiconductors. This will allow these materials to be engineered for applications in semiconductor spintronics, including a whole host of magneto-sensitive electronic and optoelectronic devices.
The authors have nothing to disclose.
This research is supported by the Natural Sciences and Engineering Research Council of Canada, Lockheed Martin Corporation, and the National Science Foundation (Grant DMR10-05851).
Ti:Sapphire Oscillator | Coherent | Mira-Seed | Part of full laser system |
Manual Translation Stage | Newport | 462 | Quantity: 2 |
Optical/Optomechanical Components | Thorlabs, Others | Various | |
DC Regulated Power Supply | Tenma | 72-6628 | |
Function Generator | GW Instek | GFG-8216A | |
Digital Delay Generator | Stanford Research Systems | DG645 | |
Speaker Amplifier | Sony | XM-222W | |
Silicon Photodetector | Thorlabs | PDA36A | |
Photomultiplier Tube | Hamamatsu | ||
Digital Oscilloscope | Tektronix | TDS2024B | |
Optical Cryostat | Janis | ST-300 | |
Cornerstone 260 Monochromator | Newport | Newport 74110 | |
Sapphire Window | General Ruby and Sapphire | ||
Citric Acid | Sigma-Aldrich | C1909 | |
Optical Adhesive | Norland | Thorlabs NOA61 | |
Hydrogen Peroxide Solution | Sigma-Aldrich | H3410 | |
Deionized Water | Water from a Type I water system |