Time-resolved terahertz

Parkinson P, Joyce HJ, Gao Q, Tan HH, Zhang X, Zon J, Jagadish C, Heiz LM, Johnston MB (2009) Carrier lifetime and mobility enhancement in nearly defect-free core-shell nanowires measured using time-resolved terahertz spectroscopy. Nano Lett 9 3349... 

Terahertz spectroscopy uses continuous wave (CW) and short pulsed laser excitation in the spectrum region between infrared and microwave frequencies. Pulsed laser excitation using pulse widths in the range of 10-100 femtoseconds has enabled the use of time-resolved terahertz spectroscopy, which is capable of capturing dynamic information at subpicosecond time scales. 

Time-resolved terahertz imaging is capable of providing information about the dynamics of chemical reactions in materials science, chemistry, and biology. 

The three methods taken together allow time-resolved spectroscopic characterization of propagating modes with far greater ease and completeness than has been possible in the past. They facilitate a number of important possibilities including spatiotemporal control over propagating modes, excitation and characterization of nonlinear lattice responses, tunable terahertz-frequency spectroscopy, and terahertz frequency and bandwidth signal processing. 

Additional experiments observing MEG have been reported for CdSe (Schaller et al., 2005b), PbTe (Murphy et al., 2006) and InAs (Pijpers et al, 2007). In addition to transient absorption studies, these optical experiments use time-resolved photoluminescence, terahertz spectroscopy, and quasi-CW spectroscopy. 

Transient terahertz spectroscopy Time-resolved terahertz (THz) spectroscopy (TRTS) has been used to measure the transient photoconductivity of injected electrons in dye-sensitised titanium oxide with subpicosecond time resolution (Beard et al, 2002 Turner et al, 2002). Terahertz probes cover the far-infrared (10-600 cm or 0.3-20 THz) region of the spectrum and measure frequency-dependent photoconductivity. The sample is excited by an ultrafast optical pulse to initiate electron injection and subsequently probed with a THz pulse. In many THz detection schemes, the time-dependent electric field 6 f) of the THz probe pulse is measured by free-space electro-optic sampling (Beard et al, 2002). Both the amplitude and the phase of the electric field can be determined, from which the complex conductivity of the injected electrons can be obtained. Fitting the complex conductivity allows the determination of carrier concentration and mobility. The time evolution of these quantities can be determined by varying the delay time between the optical pump and THz probe pulses. The advantage of this technique is that it provides detailed information on the dynamics of the injected electrons in the semiconductor and complements the time-resolved fluorescence and transient absorption techniques, which often focus on the dynamics of the adsorbates. A similar technique, time-resolved microwave conductivity, has been used to study injection kinetics in dye-sensitised nanocrystalline thin films (Fessenden and Kamat, 1995). However, its time resolution is limited to longer than 1 ns. 

In this book, most chapters deal with FT-IR spectrometry and its applications to various methods of infrared spectroscopic measurements. Only terahertz spectrometry in Chapter 19 and a large part of time-resolved infrared spectrometry in Chapter 20 are laser-based measurements. This shows how widely FT spectrometry is used at present in the measurements of vibrational spectfa. 

In practice, an electromagnetic pulse with an infinitely short width does not exist, but ultrashort laser pulses are now used for various spectroscopic measurements. Terahertz spectrometry described in Chapter 19 is based on femtosecond laser pulses. In Chapter 20, time-resolved infrared spectroscopic methods using picosecond to femtosecond laser pulses are described. Such ultrashort laser pulses have large spectral widths in the frequency domain. Let us discuss the relation between the pulse width in the time domain and its spectral width expressed in either frequency or wavenumber. 

Carrier Dynamics in Photovoltaic Structures and Materials Studied by Time-Resolved Terahertz Spectroscopy... 

Terahertz Generation, Detection and Time-Resolved Terahertz Spectroscopy Setup... 

Whereas CM in bulk materials is usually determined in photocurrent device measurements, that is, by collecting the carriers, CM in QDs is studied by (optical) spectroscopic measurements, in which the orbital occupation of the QDs is probed on ultrafast (picosecond) timescales. Hence, the commonly used experimental procedures to determine CM in QDs (ultrafast spectroscopy) and in bulk (device measurements) are rather different. While time-resolved optical and IR spectroscopies are ideally suited to probe carrier populations in colloidal QDs, " light of terahertz (THz) frequencies interacts strongly with free carriers in the bulk material and allows the direct characterization of carrier density and mobility. From THz-time domain spectroscopy (TDS) experiments, one can quantitatively assess the number of photogenerated carriers in bulk semiconductors picoseconds after the light is absorbed. Additionally, as a result of the contact-free nature of the THz probe, it is possible to determine the CM factor in isolated samples of bulk semiconductors without the need to apply contacts, which is necessary in the device measurements. For these reasons, THz-TDS experiments have been employed to quantify CM in bulk PbSe and PbS on ultrafast timescales " in order to make a bulk-QD comparison in the context of the CM controversy. The CM factor in bulk PbS and PbSe was determined for excitation with various photon energies from the UV to the IR. 

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