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Author Contact: gblinick@wesleyan.edu
Local Identifier: 321
PID: ir:2816"},{"label":"Author-supplied Keywords","value":["Recombination","Charge carrier lifetime","Photovoltaics","TRTS","Pump-probe measurements","Time resolved measurements","Optics","Physics"]},{"label":"Degree","value":["Master of Arts"]},{"label":"Description","value":"

Improving the efficiency of photovoltaic devices requires the use of semiconductors with long charge carrier lifetimes. Traditional lifetime measurement techniques, like photoluminescence (PL) and time resolved THz spectroscopy (TRTS) have been effective at characterizing the lifetimes of some photovoltaic materials. However collectively, they have a number of shortcomings as PL techniques can only be used on direct band gap semiconductors while TRTS techniques have small measurement timescales. The motivation for this thesis is to develop a new measurement technique, asynchronous time resolved terahertz spectroscopy, that enables the calculation of charge carrier lifetimes in photovoltaic materials over long time scales. ATRTS is a non-contact optical pump-probe technique characterized by the decoupling of the optical excitation pump and THz probe laser sources, which facilitates the measurement of time dependent photoconductivity decay in a material over lengthened timescales. The development of the ATRTS technique required extensive optimization to achieve sufficiently high signal to noise ratio and signal sensitivity to perform experiments. We measured undoped, n-type silicon and germanium samples and report recombination lifetimes of 9.9 ± 0.7 μs and 21 ± 3 μs for Si and Ge respectively, which are consistent with values expected from literature. We also performed ATRTS on a 5% Cs doped MAFAPb(IBr)3 hybrid perovskite sample, but limitations in signal sensitivity inhibited the calculation of a lifetime for the sample. Presently, the ATRTS technique is sensitive to signal modulations greater than 6% and the time resolution is limited to measure samples with lifetimes longer than 3 microseconds. Our measurements revealed the presence of an electronic artifact when the optical pump and THz probe pulses were simultaneously incident on the sample, or at the time zero, t0, location. We discuss the impact of the electronic artifact and signal convolution on our technique and end with methods to improve the signal sensitivity and time resolution of ATRTS for future iterations of the technique.

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