skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Measurement of Carrier Dynamics in Photovoltaic CZTSe by Time-Resolved Terahertz Spectroscopy
We demonstrate the use of time-resolved terahertz spectroscopy coupled with numerical modeling of the transport equations to elucidate photoexcited carrier dynamics in a photovoltaic absorber. By measuring a high-quality Cu2ZnSnSe4 single crystal that exhibited device efficiency of 8.6%, we show that critical parameters including mobility, surface recombination velocity, and Shockley-Read-Hall lifetime can be obtained. Mobility values of 80 cm2/Vs were validated with Hall effect measurements. Surface recombination velocity could be reduced by at least two orders of magnitude, to 10^4 cm/s, with appropriate chemical and mechanical polishing. Carrier lifetimes exceeding 10 ns indicate promise for devices with high photovoltage. Terahertz spectroscopy provides complementary insight to conventional time-resolved photoluminescence and is particularly valuable for materials that are not strongly emissive.  more » « less
Award ID(s):
1507988
PAR ID:
10062218
Author(s) / Creator(s):
; ; ; ;
Date Published:
Journal Name:
Conference record of the IEEE Photovoltaic Specialists Conference
Volume:
2017
ISSN:
0160-8371
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. IEEE (Ed.)
    In this project, Hall bar devices with black phosphorus (BP) as the semiconductor layer were fabricated to measure the Hall mobility and carrier density of exfoliated BP flakes obtained from bulk crystals acquired from various commercial sources. Black phosphorus is proposed as an alternative material for terahertz photoconductive antennas (PCAs) from the standard GaAs or InGaAs PCAs that are currently available commercially. Black phosphorus is an anisotropic material with a reported Hall mobility over three times greater than GaAs, but our preliminary testing of BP PCAs has shown dramatic differences of electrical properties between black phosphorus sourced from three different vendors. To determine the best quality black phosphorus source, Hall bar devices containing 40 nm BP flakes were used to measure the carrier mobility of the semiconductor. A Hall bar device is created by layering a 40nm BP flake underneath a hexagonal boron-nitride (hBN) flake, all on top of gold contacts in a Hall bar arrangement fabricated on a high-resistivity silicon substrate. The hBN acts as a passivation layer for the BP so that it may be safely removed from the glove box without damage. The Hall mobility of the material from different sources ranges from around 100 cm2/Vs to 1600 cm2/Vs, with only one source showing promising, high mobility results. This study allows BP with optimized electrical properties to be incorporated into THz PCAs for characterization via THz time domain spectroscopy. 
    more » « less
  2. Abstract The ultrafast dynamics of photoexcited charge carriers are studied in micron‐scale crystals composed of the inorganic perovskite CsPbBr3with time‐resolved terahertz spectroscopy. Exciting with photon energy close to the band edge, it is found that a fast (<10 ps) decay emerges in the terahertz photoconductivity with increasing pump fluence and decreasing temperature, dominating the dynamics at 4 K. The fluence‐dependent dynamics can be globally fit by a nonlinear recombination model, which reveals that the influence of different nonlinear recombination mechanisms in the studied pump fluence range depends on temperature. Whereas the Auger scattering rate decreases with decreasing temperature from 77 to 4 K, the radiative recombination rate increases by three orders of magnitude. Spectroscopically, the terahertz photoconductivity resembles a Drude response at all delays, yet an additional Lorentz component due to an above‐bandwidth resonance is needed to fully reproduce the data. 
    more » « less
  3. Abstract This work focuses on the low frequency Drude response of bulk-insulating topological insulator (TI) Bi 2 Se 3 films. The frequency and field dependence of the mobility and carrier density are measured simultaneously via time-domain terahertz spectroscopy. These films are grown on buffer layers, capped by Se, and have been exposed in air for months. Under a magnetic field up to 7 Tesla, we observe prominent cyclotron resonances (CRs). We attribute the sharp CR to two different topological surface states from both surfaces of the films. The CR sharpens at high fields due to an electron-impurity scattering. By using magneto-terahertz spectroscopy, we confirm that these films are bulk-insulating, which paves the way to use intrinsic TIs without bulk carriers for applications including topological spintronics and quantum computing. 
    more » « less
  4. The ternary phase, Yb14CdSb11, has been synthesized by flux and polycrystalline methods. The crystal structure is determined via single-crystal X-ray diffraction, revealing that it crystallizes in the Ca14AlSb11 structure type (I41/acd space group with unit cell parameters of a = 16.5962(2) & Aring; and c = 22.1346(5) & Aring;, 90 K, Z = 8, R1 = 2.65%, and wR2 = 4.58%). The polycrystalline form of the compound is synthesized from a stoichiometric reaction of Yb4Sb3, CdSb, Yb, and Sb. The elemental composition is confirmed using scanning electron microscopy and energy-dispersive spectroscopy, and phase purity is verified by powder X-ray diffraction. Thermoelectric measurements, including resistivity, Seebeck coefficient, thermal conductivity, Hall carrier concentration, and Hall mobility, are conducted from 300 to 1273 K. Yb14CdSb11 exhibits a peak zT = 0.90 at 1200 K. Carrier concentration and Hall mobility range from 6.99 x 1020-1.01 x 1021 cm-3 and 4.45-9.35 x 10-1 cm2 V-1 s-1, respectively. This carrier concentration is lower than that reported for the Zn or Mn analogs leading to a lower thermoelectric figure of merit at high temperatures. However, with appropriate doping, this phase should also be a promising p-type candidate for high-temperature energy conversion applications. 
    more » « less
  5. Abstract Germanium sulfide (GeS) is a 2D semiconductor with potential for high-speed optoelectronics and photovoltaics due to its near-infrared band gap and high mobility of optically excited charge carriers. Here, we use time-resolved THz spectroscopy to investigate the differences in ultrafast carrier dynamics in GeS following near-band gap photoexcitation (1.55 eV), which penetrates deep into the multilayer GeS, and excitation with above-band gap photon energy (3.1 eV), which is absorbed within a sub-20 nm surface layer. We find that the photoexcited carriers in the bulk have significantly longer lifetimes and higher mobility, as they are less impacted by trap states that affect carrier behavior in the surface layer. These insights are important for designing GeS-based photodetectors, solar energy conversion devices, and sensors that leverage the sensitivity of surface-layer photoexcited carriers to trap states. 
    more » « less