Carrier Dynamics In Semiconductors Research Articles

Massively parallel FDTD-FBMC simulations of nonlinear hole dynamics in silicon at cryogenic temperatures driven by intense EM THz pulses

THz spectroscopy with intense electromagnetic (EM) pulses offers unique avenues to study the charge carrier dynamics in semiconductors. Quantitative analysis of the experiment requires a detailed microscopic model that is based on the wave propagation within the sample and on the strongly nonparabolic dispersion relation of the valence bands. With a finite difference time domain (FDTD) solver for the EM wave in conjunction with a full band Monte Carlo (FBMC) model for the holes the generation of higher harmonics by the nonlinear hole response in the p-doped silicon sample can be simulated. Due to impurity freeze-out at the cryogenic temperature the hole density is low and the FDTD solver can be decoupled from the FBMC model by a perturbation approach. This enables the independent processing of a very large number of holes on a computer cluster with nearly 100% computational efficiency resulting in a very low level of stochastic noise, which is necessary to achieve a reasonable signal to noise ratio for the faint higher harmonics. The simulations show that at THz frequencies and cryogenic temperatures strong generation of higher harmonics is only possible, if the band structure is nonparabolic.

Terahertz response of ultrafast spin polarization in semi-insulating GaAs

Due to its high sensitivity and time-resolved ability, terahertz time-domain spectroscopy is a powerful tool for investigating ultrafast carrier dynamics in semiconductors. In addition to charges, spins of ultrafast carriers provide an alternate degree of freedom to design modern electronic devices but are rarely studied by terahertz time-domain spectroscopy. Here, ultrafast spin polarization in semi-insulating GaAs is studied by optical-pump terahertz-probe experiments at room temperature. We used circularly and linearly polarized femtosecond laser pulses to inject nonequilibrium carriers in GaAs and observed that both the transmitted and reflected terahertz signals exhibited different dynamical evolutions under the excitations of linearly and circularly polarized laser pulses, which are ascribed to the generation and relaxation of spin-polarized electrons. The lifetime of the ultrafast spin polarization was obtained from our experiments, highlighting the potentialities of terahertz spectroscopy for the investigation of spin relaxation in semiconductors.

Observation of photo-excited carrier dynamics in semiconductors with time, space, and energy resolutions

Observation of photo-excited carrier dynamics in semiconductors with time, space, and energy resolutions

Ultrafast dynamics of photoinduced terahertz electron-hole plasma waves in semiconductor junctions

The ultrafast transport processes of electrons and holes excited by femtosecond laser pulses are essential for a better understanding of carrier dynamics in semiconductors. Transient optical techniques are commonly used to investigate the carrier excitation and transport in these materials. Recently, ultrafast scanning electron microscopy has been employed to elucidate the ballistic dynamics of such hot carriers near a $p\text{\ensuremath{-}}n$ junction. We provide here a model not only to explain the previously reported superfast expansion of electron-hole clouds but also to predict plasma wave behavior at high laser fluences. In addition to a bipolar junction, we also investigate the well structure of a $p\text{\ensuremath{-}}n\text{\ensuremath{-}}p$ junction sandwiched by insulating layers. By confining hot carriers inside junctions, these carriers begin to oscillate as a result of Coulomb interactions among carriers and with the intrinsic field at the depletion zone, leading to the occurrence of terahertz-scale plasma waves for potential applications as pulsed terahertz light sources.

Time-Domain Observation of Spectral Diffusion in Defective ZnO.

Defects can affect all aspects of materials by altering their electronic structures and mediating the carrier dynamics. However, in the past decades, most research efforts were restricted to nonstoichiometric defects, while the effects of high-density defects on the carrier dynamics of semiconductors remained elusive. In this work, using transient absorption spectroscopy, we have observed for the first time a hybrid carrier relaxation dynamics with the feature of a Poisson-like retard shoulder in a time-domain profile in highly defective ZnO crystals. This novel behavior has been attributed to the spectral diffusion within continuum defect states, which is further confirmed by a proposed diffusion (in energy space) controlled carrier dynamic model. Our results thus reveal an alternative energy decay channel in highly defective crystals and may provide a new route for defect engineering.

Ultrahigh sensitive transient absorption spectrometer.

Transient absorption (TA) spectroscopy is considered as a powerful technique that reflects the ultrafast dynamics of photogenerated carriers in photoelectric and photocatalysis materials. However, limited by its sensitivity, the photogenerated carrier density in TA measurements of solar energy materials is usually much higher than that in the real working condition. Here, we present a combination of kHz macro-pulse and MHz micro-pulse technique for an ultrahigh sensitive TA spectrometer, which improves the sensitivity to the 10-7 level of ΔOD. It enables us to study ultrafast carrier dynamics pumped by very low power, which can avoid the influence of many-body interactions and the nonlinear effect associated with high carrier density. This work provides a novel TA method with ultrahigh sensitivity, which will play an important role in investigating the carrier dynamics of semiconductors in the working condition.

Hydrostatic pressure effect of photocarrier dynamics in GaAs probed by time-resolved terahertz spectroscopy.

Pressure effects on photocarrier dynamics such as interband relaxations and intraband cooling in GaAs have been investigated using in situ time-resolved terahertz spectroscopy with a diamond anvil cell. The interband photocarrier lifetime significantly decreases by nearly two orders of magnitude as the external hydrostatic pressure is increased up to 10 GPa. Considerable pressure tuning for the intervalley scattering processes has also been observed, and the time constants under different pressures are extracted based on the three-state rate model. This work provides new perspectives on tailoring nonequilibrium carrier dynamics in semiconductors using hydrostatic pressure and may serve as the impetus for the development of high-pressure terahertz spectroscopy.

Nonuniform Carrier Heating Induced Nonlinear Electron Transport Properties in Asymmetrically Necked InAs Mesa Structures

IntroductionTerahertz (THz) wave has been very attractive light for scientific and practical applications such as light source for characterizing fundamental physics on ultra-fast carrier dynamics in semiconductors and imaging applications in the submillimeter wavelength regime. Therefore, there have been studied on various kind of emitting and detecting methods on THz waves in this quarter century. So far, we also have proposed simple and low-cost THz wave source with InAs thin films grown on GaAs substrates combining with a time-domain spectroscopy system [1, 2]. In case of THz detectors, there are not so many techniques which enable to detect THz wave at room temperature with high responsivity without biasing. For example, square-law field rectifier detectors, such as Schottky diodes and InGaAs-based bow-tie diodes, respond to THz electric field at room temperature with no external power supply [3]. Nonlinear current-voltage characteristics of the latter technique is based on unique operation principle which is generated by nonuniform carrier heating in asymmetric bow-tie shaped planar structures. Since InAs possesses one of the highest electron mobility at room temperature among semiconductors, this material based thin films will be hopeful candidate for detecting THz waves by fabricating this unique nonlinear device structures on them. In this paper, we devise utilizing InAs THz wave emitter thin films to base material for asymmetrically necked bow-tie mesa structures for the THz detector. As a first step of this idea, nonlinear current-voltage characteristics of these devices are presented. We especially discuss on the curvature of current-voltage characteristic at zero-bias point which is closely related to the sensitivity on square-law detection for THz wave.ExperimentalNominally undoped InAs thin films were epitaxially grown on semi-insulating GaAs (100) substrate by molecular beam epitaxy. For improving the crystal quality of InAs channel layer, 150 nm thick InAs buffer layer was directly grown with gradually changing growth temperature from 300 to 500°C on GaAs substrate. An 1 µm think InAs channel layer was grown on this buffer layer at 450°C. This growth condition is same as that of THz emitter InAs films we have reported [2]. The patterning of asymmetric bow-tie mesa structure was carried out by photo lithography and phosphoric acid based wet chemical etching. After defining mesa structures, in order to investigate the film thickness dependence on nonlinear current properties, some samples were performed recess etching for InAs channel, which were made each thickness to be 265 nm, 435 nm, 625 nm and 835 nm. Finally, non-alloyed ohmic contact metals of Ti/Pt/Au (50/30/170 nm) were deposited by electron-beam evaporation technique and defined by lift-off. The structure of asymmetric bow-tie diode and the measurement configuration are shown in Fig. 1. Current-voltage characteristics were measured by using Keithley 4200A-SCS system at room temperature.Results and Conclusion Typical current-voltage characteristic of the investigated InAs asymmetric bow-tie diode is represented in Fig. 2, which was the result measured with the sample of 265 nm thick InAs channel. It showed clear asymmetric current-voltage characteristic depended on the polarity of applied voltage, which was considered originated from nonlinear carrier transport related to non-uniform carrier heating in asymmetric mesa structure. In order to evaluate the nonlinearity of current-voltage curve at zero-biased point, the zero-biased curvature coefficient γ was calculated, which is given by the formula written in Fig. 3. A fifth order polynomial fit was utilized to current-voltage curves in determining the curvature. As shown in Fig. 3, the zero-bias curvature clearly depended on thickness of InAs thin film. The highest zero-bias curvature of 0.12 V-1 was obtained in the thinnest sample. In addition, this value was about 2.2 times larger than that of the GaAs/AlGaAs heterostructure-based asymmetric bow-tie diode which had the same shape and size (not shown here). These results indicate that the InAs thin film for THz radiation has possibility to be applied to square-law detection device for THz wave. The details of nonlinearity which depends on mesa shape and size and comparison between InAs based structures and that of GaAs/AlGaAs will be discussed at the conference.

Radiation field analysis of a photoconductive antenna using an improved carrier dynamics

Photoconductive antennae are one of the most common sources of terahertz radiation. Although extensive experimental and simulation work has been done to analyze the radiated fields, very limited theoretical analysis has been done to build elegant and compact models. This work presents the derivation of the radiated fields from a photoconductive antenna incorporating the effect of the semiconductor substrate. Additionally, an improved model of the semiconductor carrier dynamics has been proposed to analyze the radiation characteristics of the photoconductive antenna. The proposed carrier dynamics includes a novel analysis of the transient behavior of the substrate temperature and its effect on the parameters of the substrate material. It also incorporates the effect of the lifetime, polarization and velocities of the carriers as well as the effects of the radiated near zone fields and antenna geometry. The derived formulae and the proposed carrier dynamics model have been validated by comparing the results with the available experimental results in the literature. It has been found that the analytically calculated results closely follow the experimental results reported in the literature.

Modeling Plasmon-Induced Hot-Carrier Transfer

In this issue of Chem , Zhang et al. use first-principle simulations (i.e., no empirically adjustable parameters) to elucidate the detailed mechanisms of plasmon-induced hot-carrier transfer at a heterojunction interface between a plasmonic gold nanomaterial and a semiconductor. Together with earlier work by Long and Prezhdo, this study shows how the donor-acceptor interaction at the interface determines the mechanism by which plasmonic excitations lead to hot-electron transfer at interfaces.

Magnetic Field-Assisted Radiation Enhancement From a Large Aperture Photoconductive Antenna

The generation of terahertz radiation using photoconductive antennas is becoming very popular. Several experimental and simulation studies have been performed to study the characteristics of the photoconductive antenna (PCA). Although various methods have been proposed to increase the radiated power from it, the radiated power remains very low. In this paper, we present an analytical study of improving the radiated power from a large aperture PCA using an external magnetic field source. The transit time behavior of the carriers is computed using the basic semiconductor carrier dynamics model, including the transient mobilities with the dependencies on the electric field and carrier’s concentration. Analytical studies show that substantial enhancement in the radiated field can be achieved when such external magnetic field is applied. Furthermore, the polarity of the radiated field depends on the orientation of the applied magnetic field. The results obtained from analytical calculations exhibit similar behavior as reported in some experimental results.

20th International Conference on Electron Dynamics in Semiconductors, Optoelectronics and Nanostructures (EDISON 20)

The 20th International Conference on Electron Dynamics in Semiconductors, Optoelectronics and Nanostructures (EDISON 20) was held at the Hyatt Regency Hotel and Conference Center in downtown Buffalo, New York, USA from July 17–21, 2017. The meeting serves as the premier forum for researchers working on the study of nonequilibrium phenomena in semiconductors, from all parts of the globe, and was organized locally by faculty at the University at Buffalo and the University of Rochester.EDISON is an international conference series with biennial meetings that cover recent progress in the field of electron dynamics in solid-state materials and devices. Initially established with the title Hot Carriers in Semiconductors (HCIS), the first meeting took place in Modena, Italy in 1973. The name was changed to International Conference on Nonequilibrium Carrier Dynamics in Semiconductors at the 1997 Berlin meeting, and again at the 2009 meeting in Montpellier to the current form. Since then, EDISON conferences have been held in Santa Barbara, USA (2011); Matsue, Japan (2013); Salamanca, Spain (2015); and Buffalo, USA (2017).The EDISON 20 program included 12 invited talks, 50 oral contributions, 116 accepted abstracts, and one special seminar. In total, 152 participants from 22 countries gathered to share and exchange ideas and recent results. Approximately 45% of the participants were from North America, 30% from Europe, and 25% from the Asia Pacific region. Fully 30% of the participants were students, and there was a very good balance between experimental and theoretical approaches. Topics with the most contributions were: Electronic and optical properties of graphene and other 2D materials; Nonequilibrium carrier transport; and Terahertz phenomena in semiconductor materials and devices.I thank all the members of the Program Committee and the International Advisory Committee for their valuable input, as well as Professor Jonathan Bird and Alex Desha for their many hours devoted to organizing a successful EDISON conference. Also critical to the success of the conference is financial support, so I thank the School of Engineering and Applied Sciences, the Vice President for Research and Economic Development, the Department of Physics, and the Department of Electrical Engineering at the University at Buffalo, as well as the U.S. Department of Energy, Kurt J. Lesker Company, and the Hajim School of Engineering & Applied Sciences at the University of Rochester for their sponsorship of EDISON 20. Finally, I thank all the scientists who contributed to the preparation and peer-review of these proceedings.Erik Einarsson, EditorEDISON 20 Publications ChairUniversity at Buffalo

Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium

Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 1020 cm−3. Separate electron and hole relaxation times are observed as a function of hot carrier energies. A first-order electron and hole decay of ∼1 ps suggests a Shockley–Read–Hall recombination mechanism. The simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.

Erratum: Carrier dynamics in semiconductors studied with time-resolved terahertz spectroscopy [Rev. Mod. Phys. 83 , 543 (2011)

Received 23 February 2017DOI:https://doi.org/10.1103/RevModPhys.89.029901© 2017 American Physical Society

Charge separation effects in time-resolved photoluminescence of Cu(In,Ga)Se2 thin film solar cells

Time-resolved photoluminescence (TRPL) is a powerful tool for investigating the charge carrier dynamics in semiconductors. Many mechanisms may contribute to the PL decay characteristics, such as radiative band-to-band recombination, non-radiative Shockley-Read-Hall recombination, capture and re-emission of minority carriers via trap states, as well as separation of the generated electron-hole pairs by gradients in their electrochemical potentials combined with different conductivities. In Cu(In,Ga)Se2 thin film solar cells charge separation has been shown to dominate the TRPL signal at low injection levels in complete devices whereas the PL decay in CdS-covered absorbers seemed unaffected by charge separation and has been reported to equal that of the bare absorber layer. In this study we investigate the PL decay of complete cells, CdS-covered absorbers and bare absorbers as a function of injection level. We show that the PL decay of not only the complete cell but also the CdS-covered absorber is dominated by charge separation at sufficiently low injection levels. In this injection regime the TRPL signal of the CdS-covered absorber significantly differs from that of the bare absorber, but also at higher injection levels different decay time constants are observed. By means of time-resolved device simulations we analyse the mechanisms of charge separation and their impact on the transient PL decay.

Carrier dynamics in femtosecond-laser-excited bismuth telluride

The carrier dynamics of $\mathrm{B}{\mathrm{i}}_{2}\mathrm{T}{\mathrm{e}}_{3}$ is studied using the femtosecond pump-probe technique. Three distinct processes, including free carrier absorption, band filling, and electron-hole recombination, are found to contribute to the reflectivity changes. The two-temperature model is used to describe the intraband energy relaxation process of carriers, and the Drude contribution well explains the intensity dependence of the peak values of the nonoscillatory component in the reflectivity signal. The combined effects of free carrier absorption and band filling result in a reflection minimum at about 2 ps after laser excitation. The nonzero background signal increases linearly with the pump fluence, which is attributed to the electron-hole recombination. Finally, our results provide an illustration of investigating the carrier dynamics in semiconductors from the ultrafast reflectivity spectra.

Research on MeV pulsed radiation detection based on refractive index modulaiton

High time resolution detecting systems for MeV pulsed radiation are essential for inertial confinement fusion diagnostics. Traditional detection of system time resolution is restricted by cable bandwidth. Based on recording excess carrier dynamics in semiconductors, a new detecting mechanism, called RadOptic, was developed by Lawrence Livermore National Laboratory (LLNL). The variation of intensity of pulsed radiation with time was converted into the variation of intensity of infrared laser probe by using this mechanism. The sensing material was InGaAsP quantum wells with severalmicrometer thickness. Picosecond time resolution for several keV pulsed radiation has been demonstrated. The reported system is not suitable for MeV pulses due to its low efficiency to MeV photons. Multiple cascaded structure for MeV photon to electron transformation was proposed by LLNL. Applying bulk material with several-hundredmicrometer thickness is an alternative. Based on transient free carrier absorption, a system recording bulk materials' instantaneous refractive index change is established. The system consists of a probe laser, an interferometer module, a signal transmission module and a signal recording module. The probe is a tunable infrared continuous wave laser whose wavelength is ~1453 nm, guided by single mode fiber to the interferometer. The interferometer consists of a single mode fiber head coupled directly with the polished face of a bulk semiconductor. The interference pattern forms by multiple beams reflected from the front face and the back face of the bulk. Part of interference light is coupled to the single mode fiber and forms the output signal. Pulsed radiation will deposit energy and generate excess carriers in the bulk material. The refractive index of the bulk material changes therewith according to the Drude model. The interference pattern and the light coupled to the single mode fiber also change therewith. The signal is transmitted by a long single mode fiber. The signal recording module consists of photoelectric detectors and a digital oscilloscope. The signal generation process and the time resolution of the system are analyzed. Intrinsic GaAs refractive index change is exploited under electron pulses and X ray pulses. The analysis of signal generation process shows that when the excess carriers recombine much faster/much slower than the pulse width, the output signal/output signal differential can be viewed as a measure of intensity variation with time of the incident pulse. For this prototype system, the time resolution is restricted by the digital oscilloscope to 1 GHz. Bulk intrinsic GaAs demonstrates 30 ns refractive index response time, which is longer than the incident pulse width. The differential signal can be viewed as a measure of incident pulse intensity when GaAs is exposed to 1 ns~0.2 MeV electrons pulses. The differential signal width is shorter than the pulse width when GaAs is exposed to 5 ns~0.2 MeV electrons pulses. Auger recombination process may occur in the pulse duration under this situation. The differential signal width is longer than the pulse width when GaAs is exposed to 1 ns~0.2 MeV X ray pulses. The poor signal to noise ratio affects the signal. The excess carrier generation process may be longer than theoretically estimated one under X ray pulse incident situation. The generation process and recombination process of excess carriers in GaAs show very different characteristics compared with optical excitation. The relationship between the system output signal and the incident pulsed radiation depends on the type of the incident radiation. With carefully considering the effects from incident pulse type and transient carriers density, the system can be used to detect ~MeV pulsed radiation. With an upgraded recording module, the system would demonstrate much higher time resolution.

Excitation correlation photoluminescence in the presence of Shockley-Read-Hall recombination

Excitation correlation photoluminescence (ECPL) measurements are often analyzed in the approximation of a cross correlation of charge carrier populations generated by the two delayed pulses. In semiconductors, this approach is valid for a linear non-radiative recombination path, but not for a non-linear recombination rate as in the general Shockley-Read-Hall recombination scenario. Here, the evolution of the ECPL signal was studied for deep trap recombination following Shockley-Read-Hall statistics. Analytic solutions can be obtained for a fast minority trapping regime and steady state recombination. For the steady state case, our results show that the quadratic radiative term plays only a minor role, and that the shape of the measured signal is mostly determined by the non-linearity of the recombination itself. We find that measurements with unbalanced intense pump and probe pulses can directly provide information about the dominant non-radiative recombination mechanism. The signal traces follow the charge carrier concentrations, despite the complex origins of the signal, thus showing that ECPL can be applied to study charge carrier dynamics in semiconductors without requiring elaborate calculations. The model is compared with measurements on a reference sample with alternating layers of InGaAs/InAlAs that were additionally cross-checked with time resolved optical pump terahertz probe measurements and found to be in excellent agreement.

Transient reflectivity as a probe of ultrafast carrier dynamics in semiconductors: A revised model for low-temperature grown GaAs

We revisit pump-probe transient reflectivity (PPTR) as a probe of ultrafast carrier dynamics in photoconductive materials, using low-temperature grown GaAs (LT-GaAs) as an exemplar. The carrier dynamics in a series of annealed LT-GaAs wafers were measured by PPTR. The wafer growth and anneal conditions were tailored to produce a material system with a sub-picosecond carrier lifetime. The PPTR signals from these wafers are bipolar with time constants on the order of 100 fs and 1 ps, consistent with previous literature reports on LT-GaAs. We examined the utility of numerical simulations of the pump-probe transients described in [V. Ortiz et al., J. Appl. Phys. 102, 043515 (2007)] to model our experimental results. We discovered a discrepancy between the model's predictions and experiment with respect to the scaling of the PPTR response with injected carrier density, and show that this discrepancy is rooted in how the model accounts for the index of refraction change due to band filling (BF) and band gap renormalization (BGR). We demonstrate that any model that includes a non-negligible BGR effect is inconsistent with our experimental observations of LT-GaAs. We present a revised model to simulate PPTR signals that account for BF and incorporate optical absorption from mid-gap states. This model can reproduce the experimental results on LT-GaAs and enables comparative assessments of alternate trapping and recombination hypotheses. For LT-GaAs, we compared point defects and nanoparticles as sites for Shockley-Read-Hall recombination, with the result that nanoparticle trapping and recombination centers most accurately reproduce the PPTR probe of carrier dynamics in LT-GaAs.

Femtosecond time-resolved photoemission electron microscopy for spatiotemporal imaging of photogenerated carrier dynamics in semiconductors.

We constructed an instrument for time-resolved photoemission electron microscopy (TR-PEEM) utilizing femtosecond (fs) laser pulses to visualize the dynamics of photogenerated electrons in semiconductors on ultrasmall and ultrafast scales. The spatial distribution of the excited electrons and their relaxation and/or recombination processes were imaged by the proposed TR-PEEM method with a spatial resolution about 100 nm and an ultrafast temporal resolution defined by the cross-correlation of the fs laser pulses (240 fs). A direct observation of the dynamical behavior of electrons on higher resistivity samples, such as semiconductors, by TR-PEEM has still been facing difficulties because of space and/or sample charging effects originating from the high photon flux of the ultrashort pulsed laser utilized for the photoemission process. Here, a regenerative amplified fs laser with a widely tunable repetition rate has been utilized, and with careful optimization of laser parameters, such as fluence and repetition rate, and consideration for carrier lifetimes, the electron dynamics in semiconductors were visualized. For demonstrating our newly developed TR-PEEM method, the photogenerated carrier lifetimes around a nanoscale defect on a GaAs surface were observed. The obtained lifetimes were on a sub-picosecond time scale, which is much shorter than the lifetimes of carriers observed in the non-defective surrounding regions. Our findings are consistent with the fact that structural defects induce mid-gap states in the forbidden band, and that the electrons captured in these states promptly relax into the ground state.