scholarly journals Single Shot Time-Resolved Terahertz Spectroscopy for Optoelectronic Materials

2021 ◽  
Author(s):  
◽  
Aleksa Djorović

<p>Optoelectronic materials and devices, such as LEDs and solar cells, are ubiquitous in the modern, technologically driven world. Understanding the fundamental physical process in optoelectronic materials is essential for the design and development of new devices which are more efficient, cheaper, printable, as well as environmentally friendly. Two particularly important material properties for device performance are charge mobility and photoconductivity, as they increase charge separation and extraction efficiencies, and thus give specific insight into device efficiency. The best suited technique for measuring mobility and conductivity on ultrafast timescales is Terahertz spectroscopy. Terahertz spectroscopy is a non-invasive, contact-free probe of the mobility of charges in optoelectronic materials. Terahertz time-domain spectroscopy allows for the direct determination of the entire complex-valued conductivity. As a result, important optical properties such as the complex refractive index and dielectric function of a material can be measured directly. The short duration of THz pulses, on the order of 1 ps, also allows for time-resolved studies of the transient photoconductivity in optically-excited materials with sub-picosecond time resolution, i.e. Time-Resolved Teraherz Spectroscopy (TRTS). Traditionally, only the peak of the THz pulse signal is measured with TRTS, due to the time constraints of a two-delay experiment. This does not allow for frequency-resolved THz spectra. As a result, it discards a lot of the information Terahertz-TDS spectroscopy contains, as well as its advantages over other spectroscopic techniques. Frequency-resolved TRTS would allow for the calculation of transient conductivity at each pump-probe delay time and can differentiate between signals of excitons and free charge carriers. This would allow for robust interpretations of charge mobility in novel materials. However, frequency-resolved TRTS is not practically feasible in a dual-delay configuration. We develop in this thesis a novel single-shot method based on angle-to-time mapping of a rotating probe. This method is applied to build a single-shot Terahertz-TDS spectrometer. A transmissive grating applies pulse front tilt which allows for the measurement of the entire THz transient (over a 5.7 ps window) in a single laser shot on a CMOS multichannel detector, thus alleviating the need for delay stage sampling of the THz transient, and leading to a reduction of experimental time by several orders of magnitude. An optical pump excitation is incorporated to allow a time-resolved measurement (TRTS) of the entire terahertz time-domain spectrum, and thus frequency-resolved TRTS. We show qualitative agreement between the THz time domain spectra obtained with the single shot technique and the standard free-space electro-optic (EO) sampling with balanced photodiodes, with an order of magnitude increased signal sensitivity. A proof-of-concept single shot TRTS study of a Si semiconductor sample is also given, showing we are able to resolve the TRTS signal of the entire THz pulse in a single shot, in time. This technique allows us to obtain significantly more information than traditional TRTS methods without any compromise in experiment time. However we find that the implemented single shot technique seems to suffer at higher frequencies (above 2 THz), which must be addressed to confirm the viability of a full spectrum single shot TRTS experiment. Further improvements, such as tighter focusing of the THz radiation, must be made to both the single-shot spectrometer as well as to the optical pump, for a quantitative single shot measurement. However, the proof-of-concept results in this thesis prove frequency-resolved TRTS is viable by using the developed single-shot detection method. As such it directly allows a novel spectroscopic tool which can lead to new insights into charge mobilities in optoelectronic materials, and may encourage wider application of TRTS.</p>

2021 ◽  
Author(s):  
◽  
Aleksa Djorović

<p>Optoelectronic materials and devices, such as LEDs and solar cells, are ubiquitous in the modern, technologically driven world. Understanding the fundamental physical process in optoelectronic materials is essential for the design and development of new devices which are more efficient, cheaper, printable, as well as environmentally friendly. Two particularly important material properties for device performance are charge mobility and photoconductivity, as they increase charge separation and extraction efficiencies, and thus give specific insight into device efficiency. The best suited technique for measuring mobility and conductivity on ultrafast timescales is Terahertz spectroscopy. Terahertz spectroscopy is a non-invasive, contact-free probe of the mobility of charges in optoelectronic materials. Terahertz time-domain spectroscopy allows for the direct determination of the entire complex-valued conductivity. As a result, important optical properties such as the complex refractive index and dielectric function of a material can be measured directly. The short duration of THz pulses, on the order of 1 ps, also allows for time-resolved studies of the transient photoconductivity in optically-excited materials with sub-picosecond time resolution, i.e. Time-Resolved Teraherz Spectroscopy (TRTS). Traditionally, only the peak of the THz pulse signal is measured with TRTS, due to the time constraints of a two-delay experiment. This does not allow for frequency-resolved THz spectra. As a result, it discards a lot of the information Terahertz-TDS spectroscopy contains, as well as its advantages over other spectroscopic techniques. Frequency-resolved TRTS would allow for the calculation of transient conductivity at each pump-probe delay time and can differentiate between signals of excitons and free charge carriers. This would allow for robust interpretations of charge mobility in novel materials. However, frequency-resolved TRTS is not practically feasible in a dual-delay configuration. We develop in this thesis a novel single-shot method based on angle-to-time mapping of a rotating probe. This method is applied to build a single-shot Terahertz-TDS spectrometer. A transmissive grating applies pulse front tilt which allows for the measurement of the entire THz transient (over a 5.7 ps window) in a single laser shot on a CMOS multichannel detector, thus alleviating the need for delay stage sampling of the THz transient, and leading to a reduction of experimental time by several orders of magnitude. An optical pump excitation is incorporated to allow a time-resolved measurement (TRTS) of the entire terahertz time-domain spectrum, and thus frequency-resolved TRTS. We show qualitative agreement between the THz time domain spectra obtained with the single shot technique and the standard free-space electro-optic (EO) sampling with balanced photodiodes, with an order of magnitude increased signal sensitivity. A proof-of-concept single shot TRTS study of a Si semiconductor sample is also given, showing we are able to resolve the TRTS signal of the entire THz pulse in a single shot, in time. This technique allows us to obtain significantly more information than traditional TRTS methods without any compromise in experiment time. However we find that the implemented single shot technique seems to suffer at higher frequencies (above 2 THz), which must be addressed to confirm the viability of a full spectrum single shot TRTS experiment. Further improvements, such as tighter focusing of the THz radiation, must be made to both the single-shot spectrometer as well as to the optical pump, for a quantitative single shot measurement. However, the proof-of-concept results in this thesis prove frequency-resolved TRTS is viable by using the developed single-shot detection method. As such it directly allows a novel spectroscopic tool which can lead to new insights into charge mobilities in optoelectronic materials, and may encourage wider application of TRTS.</p>


2016 ◽  
Vol 87 (9) ◽  
pp. 095101 ◽  
Author(s):  
Zhao-Hui Zhai ◽  
Sen-Cheng Zhong ◽  
Jun Li ◽  
Li-Guo Zhu ◽  
Kun Meng ◽  
...  

2010 ◽  
Vol 5 (4) ◽  
pp. 123-129
Author(s):  
Mu Kaijun ◽  
Zhang Cunlin

We examined the feasibility of Terahertz time-domain spectroscopy (THz-TDS) using a 4-mm-thick quartz crystal to extract the angle of rotation of THz radiation polarization induced by a two-color laser in air plasma. We also used the THz-TDS technique to identify explosives and melamine in mixtures. In addition, we presented a new opto-mechanical scanner for security applications using the method of passive THz imaging


Holzforschung ◽  
2014 ◽  
Vol 68 (1) ◽  
pp. 61-68 ◽  
Author(s):  
Tetsuya Inagaki ◽  
Ian D. Hartley ◽  
Satoru Tsuchikawa ◽  
Matthew Reid

Abstract Wood is relatively transparent to terahertz (THz) radiation with wavelengths in the submillimeter range. This radiation has a high potential for sensing and imaging wood with a good spatial resolution. THz is especially sensitive to moisture content, fiber alignment, and density – all of which are critical in the manufacturing of wood products. In this work, a systematic study was undertaken on 46 very different wood species by means of THz time-domain spectroscopy with density determination in focus. The dielectric response of wood was modeled based on the Maxwell-Garnett effective medium theory. The dielectric function of the cell wall material was found to be extremely consistent over this large number of species with very different properties. This renders possible to determine wood density by THz time-domain spectroscopy. A strong correlation between the measured and predicted densities has been observed for all the samples investigated.


2020 ◽  
Vol 1 (1) ◽  
pp. 1-4
Author(s):  
Chiara Ciccarelli ◽  
Hannah Joyce ◽  
Jason Robinson ◽  
Farhan Nur Kholid ◽  
Dominik Hamara ◽  
...  

Time-Domain terahertz spectroscopy (THz TDS) has attracted attention from many scientific disciplines as it enables accessing the gap between electronic and optical techniques. One application is to probe spintronic dynamics in sub-picosecond time scale. Here, we discuss principles and technical aspects of a typical THz TDS setup. We also show an example of terahertz time-domain data obtained from a Co/Pt thin film calibrant, which is a well-studied spintronic structure emitting strong THz radiation. See video at https://youtu.be/X7vrvQcmy8c.


2013 ◽  
Vol 320 ◽  
pp. 133-137
Author(s):  
Xiao Jian Fu ◽  
Ji Zhou

Terahertz radiation refers to the electromagnetic wave whose frequency is usually defined between 0.1 and 10 THz (1 THz=1012 Hz). With the development of the emission and detection technologies of THz radiation, terahertz time-domain spectroscopy (THz-TDS) has been widely used in medical diagnosis, security inspection and materials characterization. In this paper, we introduced briefly the progress of terahertz measurement technologies, and then reviewed the applications of THz spectra in functional materials researches. As two important functional optical materials, TiO2 nanoparticles and yttrium aluminum garnet (YAG) crystal have been investigated with THz-TDS. We introduced the electron injection process in TiO2 studied by time resolved THz spectroscopy which is reported in the literature, and then presented our own work, the THz optical constants of undoped and Tm3+ doped YAG crystals.


2003 ◽  
Vol 770 ◽  
Author(s):  
Nathanael Smith ◽  
Max J. Lederer ◽  
Marek Samoc ◽  
Barry Luther-Davies ◽  
Robert G. Elliman

AbstractOptical pump-probe measurements were performed on planar slab waveguides containing silicon nanocrystals in an attempt to measure optical gain from photo-excited silicon nanocrystals. Two experiments were performed, one with a continuous-wave probe beam and a pulsed pump beam, giving a time resolution of approximately 25 ns, and the other with a pulsed pump and probe beam, giving a time resolution of approximately 10 ps. In both cases the intensity of the probe beam was found to be attenuated by the pump beam, with the attenuation increasing monotonically with increasing pump power. Time-resolved measurements using the first experimental arrangement showed that the probe signal recovered its initial intensity on a time scale of 45-70 μs, a value comparable to the exciton lifetime in Si nanocrystals. These data are shown to be consistent with an induced absorption process such as confined carrier absorption. No evidence for optical gain was observed.


2019 ◽  
Vol 629 ◽  
pp. A112 ◽  
Author(s):  
B. M. Giuliano ◽  
A. A. Gavdush ◽  
B. Müller ◽  
K. I. Zaytsev ◽  
T. Grassi ◽  
...  

Context. Reliable, directly measured optical properties of astrophysical ice analogues in the infrared and terahertz (THz) range are missing from the literature. These parameters are of great importance to model the dust continuum radiative transfer in dense and cold regions, where thick ice mantles are present, and are necessary for the interpretation of future observations planned in the far-infrared region. Aims. Coherent THz radiation allows for direct measurement of the complex dielectric function (refractive index) of astrophysically relevant ice species in the THz range. Methods. We recorded the time-domain waveforms and the frequency-domain spectra of reference samples of CO ice, deposited at a temperature of 28.5 K and annealed to 33 K at different thicknesses. We developed a new algorithm to reconstruct the real and imaginary parts of the refractive index from the time-domain THz data. Results. The complex refractive index in the wavelength range 1 mm–150 μm (0.3–2.0 THz) was determined for the studied ice samples, and this index was compared with available data found in the literature. Conclusions. The developed algorithm of reconstructing the real and imaginary parts of the refractive index from the time-domain THz data enables us, for the first time, to determine the optical properties of astrophysical ice analogues without using the Kramers–Kronig relations. The obtained data provide a benchmark to interpret the observational data from current ground-based facilities as well as future space telescope missions, and we used these data to estimate the opacities of the dust grains in presence of CO ice mantles.


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