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Frontiers of Optoelectronics

Front. Optoelectron.    2014, Vol. 7 Issue (2) : 220-242     DOI: 10.1007/s12200-014-0398-2
Application of broadband terahertz spectroscopy in semiconductor nonlinear dynamics
I-Chen HO1,*(),Xi-Cheng ZHANG2,3,*()
1. Rensselaer Polytechnic Institute, Troy, NY 12180-3590, USA
2. The Institute of Optics, University of Rochester, Rochester, NY 14627-0186, USA
3. Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074, China
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Semiconductor nonlinearity in the range of terahertz (THz) frequency has been attracting considerable attention due to the recent development of high-power semiconductor-based nanodevices. However, the underlying physics concerning carrier dynamics in the presence of high-field THz transients is still obscure. This paper introduces an ultrafast, time-resolved THz pump/THz probe approach to study semiconductor properties in a nonlinear regime. The carrier dynamics regarding two mechanisms, intervalley scattering and impact ionization, was observed for doped InAs on a sub-picosecond time scale. In addition, polaron modulation driven by intense THz pulses was experimentally and theoretically investigated. The observed polaron dynamics verifies the interaction between energetic electrons and a phonon field. In contrast to previous work which reported optical phonon responses, acoustic phonon modulations were addressed in this study. A further understanding of the intense field interacting with solid materials will accelerate the development of semiconductor devices.

This paper can be divided into 4 sections. Section 1 starts with the design and performance of a table-top THz spectrometer, which has the advantages of ultra-broad bandwidth (one order higher bandwidth compared to a conventional ZnTe sensor) and high electric field strength (>100 kV/cm). Unlike the conventional THz time-domain spectroscopy, the spectrometer integrated a novel THz air-biased-coherent-detection (THz-ABCD) technique and utilized gases as THz emitters and sensors. In comparison with commonly used electro-optic (EO) crystals or photoconductive (PC) dipole antennas, the gases have the benefits of no phonon absorption as existing in EO crystals and no carrier life time limitation as observed in PC dipole antennas. In Section 2, the newly development THz-ABCD spectrometer with a strong THz field strength capability provides a platform for various research topics especially on the nonlinear carrier dynamics of semiconductors. Two mechanisms, electron intervalley scattering and impact ionization of InAs crystals, were observed under the excitation of intense THz field on a sub-picosecond time scale. These two competing mechanisms were demonstrated by changing the impurity doping type of the semiconductors and varying the strength of the THz field.

Another investigation of nonlinear carrier dynamics in Section 3 was the observation of coherent polaron oscillation in n-doped semiconductors excited by intense THz pulses. Through modulations of surface reflection with a THz pump/THz probe technique, this work experimentally verifies the interaction between energetic electrons and a phonon field, which has been theoretically predicted by previous publications, and shows that this interaction applies for the acoustic phonon modes. Usually, two transverse acoustic (2TA) phonon responses are inactive in infrared measurement, while they are detectable in second-order Raman spectroscopy. The study of polaron dynamics, with nonlinear THz spectroscopy (in the far-infrared range), provides a unique method to diagnose the overtones of 2TA phonon responses of semiconductors, and therefore incorporates the abilities of both infrared and Raman spectroscopy. Finally, some conclusions were presented in Section 4. In a word, this work presents a new milestone in wave-matter interaction and seeks to benefit the industrial applications in high power, small scale devices.

Keywords terahertz (THz)      nonlinear      spectroscopy      broadband      semiconductor     
Corresponding Authors: I-Chen HO   
Issue Date: 25 June 2014
 Cite this article:   
I-Chen HO,Xi-Cheng ZHANG. Application of broadband terahertz spectroscopy in semiconductor nonlinear dynamics[J]. Front. Optoelectron., 2014, 7(2): 220-242.
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Fig.1  Schematic illustration of broadband THz wave generation and detection. BS, beam splitter; BBO, beta barium borate; HV, high voltage bias; PMT, photomultiplier tube
Fig.2  (a) Measured time-domain waveforms with a conventional ZnTe sensor (black curve) and with a THz-ABCD sensor (red curve). The air plasma is utilized as an emitter in both measurements; (b) corresponding spectra obtained through discrete Fourier transform of the THz waveforms. The frequency range from 0.5 to 35 THz in THz-ABCD shows one order of bandwidth improvement in comparison with a conventional ZnTe sensor
Fig.3  (a) Measured reflection spectra of a CaCO3 crystal and the reference (solid lines) as well as measured phase responses (dashed lines); (b) measured transmission spectra of the same crystal; (c) refractive indices (n and k) of o axis from 0.8 to 8 THz according to (a); (d) refractive indices (n and k) of e axis from 0.8 to 8 THz according to (a)
Fig.4  Experimental setup. The THz beam is generated by mixing the fundamental and SH beams (after a type-I beta BBO crystal) at the air plasma point in front of parabolic mirror P1. A high resistivity silicon wafer acts as a beam splitter which blocks the residual 800 and 400 nm beams, but passes and reflects the THz beam. The sample position is located at the focal point of parabolic mirror P2. The THz beam is detected by measuring the coherent time-resolved SH signal induced by mixing the probe field, the THz field, and the alternating current (AC) bias electrical field at the focal point of P3
Fig.5  (a) Measured time domain waveform and (b) Fourier transform spectrum of (a) with an 85 fs amplified laser; (c) measured time domain waveform and (d) Fourier transform spectrum of (c) with a 32 fs amplified laser with an R-THz-ABCD spectrometer
Fig.6  Time-domain waveform of water vapor absorption measured with an R-THz-ABCD spectrometer. The relative humidity is ~15%
Fig.7  Comparison of water vapor absorption spectra between R-THz-ABCD and FTIR measurement. The magnification shows the spectral range from 2 to 2.5 THz. The relative humidity is ~15%
Fig.8  (a) and (b) Measured reflective waveforms of a α-BBO crystal at an angle of 0° and 90°, respectively; (c) and (d) Fourier transform spectra of (a) and (b). The black dashed lines in (c) and (d) indicate the spectra dips due to the phonon resonances for 0° and the blue dashed lines for 90°
Fig.9  (a) Reflectance of an n-type InAs sample. The plasma resonance is around 3 THz and the phonon resonance is around 7.2 THz; (b) reflectance of a p-type InAs sample. The phonon resonance is around 7.2 THz
Fig.10  (a) Beam steepening unit consists of two convex lenses; (b) Fourier transform spectrum (red curve) and noise floor (black curve) measured with adding the beam steepening unit; (c) reflectance of a GaAs sample with the phonon resonance around 8.8 THz; (d) reflectance of a GaP sample with the phonon resonance around 11 THz
R-THz-ABCD (85 fs laser)Traditional THz-TDSFTIR (Bruker IFS 66v/S)
Sourcedry nitrogenZnTemercury lamp
Detectordry nitrogenZnTeDTGS
DR of power (<3THz)>106>108~300
bandwidth (10% or greater of peak amplitude)0.5-10 THz0.1-3 THzfar to mid-infrared
resolution~0.1 cm-1~0.1 cm-1~0.1 cm-1
peak power6 × 104 W2 × 103 W (amplified laser)1 × 10-7 W
data acquisition timeseconds or minutesminutesminutes
uniquenesstime resolved & broad bandwidthtime resolved & high SNRbroad bandwidth
Tab.1  Comparison of R-THz-ABCD, traditional THz-TDS, and FTIR
Fig.11  SNR of the R-THz-ABCD (red curve) in a nine-time scan average and SNR of the FTIR (black curve) in a nine-time scan average
Fig.12  Illustration of impact ionization process. The electron in conduction band gains energy from a THz pulse (a) and generates an electron-hole pair (b); (c) effective mass of holes is much larger than electrons, so only the impact ionization from electrons is considered
Fig.13  Intervalley scattering of electrons between two valleys
Fig.14  Band structures of GaAs, InSb, and InAs at 300 K
Fig.15  Schematic illustration of a reflective pump/probe setup. The THz pump/probe pulses are generated by air plasmas, and the THz probe pulses are detected by EO sampling. BS, beam splitter; QWP, quarter-wave plate. The full-width of half maximum of the THz beam diameter at sample is 0.75 mm, measured with a knife-edge method
Fig.16  Normalized reflection of the THz probe peak field as a function of delay τ. The reflection increases after τ>0 due to a cascaded carrier generation. (a) p-doped InAs crystals with doping concentrations of 1017 cm-3 (solid line) and 1018 cm-3 (solid line with dots); (b) n-doped InSb crystal with a doping concentration of 1016 cm-3
Fig.17  (a) n-doped InAs crystal with a doping concentration of 1017 cm-3 at different THz pump field excitation, 110 kV/cm (solid line) and 90 kV/cm (solid line with dots); (b) n-doped GaAs crystal with a doping concentration of 1017 cm-3. The reflection decreases with τ>0 due to carrier intervalley scattering
Fig.18  Reflection measurement with THz-ABCD. The reflections are of different THz field strengths in n-doped InAs
Fig.19  Experimental estimation of electron fractional occupancy between Г and L valleys at different THz field strengths according to the plasma resonances in Fig. 18. The circular and square dots are experimental data of the Г and L valleys, respectively. The dotted lines are fitting curves
Fig.20  (a) Schematic illustration of the measurement setup. The THz pump/probe pulses are generated in air plasmas and detected by EO sampling or by ABCD (the black-dashed inset). The polarities of the pump/probe pulses are controlled independently. PMT, photomultiplier tube; BS, beam splitter; HV, high voltage; (b) and (c) electron motions driven by different polarities between THz pump/probe pulses, parallel and antiparallel, respectively (by rotating the BBO crystal in the pump beam to change the polarity)
Fig.21  Experimental results of coherent polaron oscillations with EO detection. (a) and (b) InSb of 1014 cm-3 and InAs of 1017 cm-3, respectively. The red solid line and blue solid line with dots show opposite phases as the pump/probe pulses in parallel or antiparallel polarities, respectively; (c) InSb of 1014 and 1016 cm-3 at antiparallel case; (d) InAs of 1017 and 1016 cm-3 at antiparallel case; (e) and (f) show the spectra of the oscillatory features of InAs of 1017 and 1016 cm-3 in (d), respectively. The black arrows indicate the coherent vibration modes due to electron-phonon coupling
Fig.22  (a) and (b) Waveforms retrieved by subtraction of the parallel and antiparallel cases in Figs. 21(a) and 21(b), respectively; (c) and (d) Fourier transforms of the retrieved waveforms in Figs. 22(a) and 22(b). The fitting curves are shown in blue dashed curves to estimate the coherent polaron damping time. Three point adjacent-averaging is applied
Fig.23  Second-order acoustic Raman spectra of InSb, InAs, and InP compared with the overtones of two-phonon density of states calculated with the OVS model. Cited from Ref. [59]
Fig.24  n-doped GaAs at 100 kV/cm THz pump field and 15 kV/cm THz probe field
Fig.25  Reflection measurement with THz-ABCD. (a) Reflections are of different THz field strengths in InSb of 1014 cm-3; (b) and (c) refractive index (real part) and absorption coefficient according to (a)
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