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Front. Optoelectron.    2014, Vol. 7 Issue (2) : 156-198    https://doi.org/10.1007/s12200-014-0396-4
REVIEW ARTICLE
Terahertz radiation-enhanced-emission-of-fluorescence
Jingle LIU1,*(),Xi-Cheng ZHANG2,*()
1. Bloomberg Tradebook LLC, 120 Park Ave, New York, NY 10017, USA
2. The Institute of Optics, University of Rochester, Rochester, NY 14627-0186, USA
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Abstract

Terahertz (THz) wave science and technology have been found countless applications in biomedical imaging, security screening, and non-destructive testing as they approach maturity. However, due to the challenge of high ambient moisture absorption, the development of remote open-air broadband THz spectroscopy technology is lagging behind the compelling need that exists in homeland security, astronomy and environmental monitoring. Furthermore, the underlying physical mechanisms behind the interaction between the THz wave and laser-induced plasma which responds strongly to electromagnetic waves have not been fully understood.

This review aims to explain the light-plasma interaction at THz frequencies within a semiclassical framework along with experimental study of the femtosecond-laser-induced nitrogen plasma fluorescence under the illumination of single-cycle THz pulses. The results indicate that THz-radiation-enhanced-emission-of-fluorescence (THz-REEF) is dominated by electron kinetics in the THz field and the electron-impact excitation of gas molecules/ions. The information of the time-dependent THz field can be recovered from the measured time-resolved THz-REEF from single-color laser induced plasma with the help of the bias as local oscillator. The calculations and experimental verification lead to complete understanding of the science behind these effects and push forward to extend their capabilities in related applications such as remote THz sensing, plasma diagnostics and ultrafast photoluminescence modulation.

Systematic studies in selected gases including neon, argon, krypton, xenon, methane (CH4), ethane (C2H6), propane (C3H8), and n-butane (C4H10) gases were performed to obtain an improved understanding of the THz-REEF. The dependences of the enhanced fluorescence on the THz field, laser excitation intensity, gas pressure, and intrinsic atomic properties were experimentally characterized. Both narrow line emission and broad continuum emission of the gas plasma were enhanced by the THz field. Their fluorescence enhancement ratios and time-resolved enhanced fluorescence were largely dependent on the scattering cross section and ionization potential of atoms.

For the first time, we demonstrated a novel ‘all-optical’ technique of broadband THz wave remote sensing by coherently manipulating the fluorescence emission from asymmetrically ionized gas plasma that interacted with THz waves. By studying the ultrafast electron dynamics under the single cycle THz radiation, we found that the fluorescence emission from laser-induced air plasma was highly dependent on the THz electric field and the symmetry of the electron drift velocity distribution created by two-color laser fields. The time-resolved THz-REEF can be tailored by switching the relative two-color phase and laser polarizations. Owing to the high atmospheric transparency and omni-directional emission pattern of fluorescence, this technique can be used to measure THz pulses at standoff distances with minimal water vapor absorption and unlimited directionality for optical signal collection. The coherent THz wave detection at a distance of 10 m had been demonstrated. The combination of this method and previously demonstrated remote THz generation would eventually make remote THz spectroscopy available.

We also introduced a unique plasma diagnostic method utilizing the THz-wave-enhanced fluorescence emission from the excited atoms or molecules. The electron relaxation time and plasma density were deduced through applying the electron impact excitation/ionization and electron-ion recombination processes to the measured time-delay-dependent enhanced fluorescence. The electron collision dynamics of nitrogen plasma excited at different gas pressures and laser pulse energies were systematically investigated. This plasma diagnostic method offers picosecond temporal resolution and is capable of omni-directional optical signal collection.

The ultrafast quenching dynamics of laser-pulse-induced photoluminescence in semiconductors under the radiation of single-cycle THz pulses was studied. It was found that the quenching in both cadmium telluride (CdTe) and gallium arsenide (GaAs) was linearly proportional to the intensity of incident THz waves and reaches up to 17% and 4% respectively at the peak intensity of 13 MW/cm2. The THz-wave-induced heating of the carriers and lattice and the subsequent decreased efficiency of photocarrier generation and recombination were most likely to be responsible for the quenching. This is potentially useful for the applications of a non-invasive ultrafast light modulator for photoluminescence devices with picoseconds switching time in the fields of the light-emitting devices and optical communication.
Keywords terahertz (THz)      fluorescence      optical sensing      gas plasma     
Corresponding Author(s): Jingle LIU   
Issue Date: 25 June 2014
 Cite this article:   
Jingle LIU,Xi-Cheng ZHANG. Terahertz radiation-enhanced-emission-of-fluorescence[J]. Front. Optoelectron., 2014, 7(2): 156-198.
 URL:  
https://academic.hep.com.cn/foe/EN/10.1007/s12200-014-0396-4
https://academic.hep.com.cn/foe/EN/Y2014/V7/I2/156
Fig.1  Electromagnetic spectrum. THz frequency falls between microwave and visible bands
Fig.2  (a) Optical image of a 600 mm × 600 mm panel of foam insulation on a metal substrate. There exist some defects hidden underneath the surface; (b) THz image of the same panel. Black circles are the embedded defects [6]
Fig.3  (a) Internal structure of a human tooth mapped out by THz imaging; (b) THz image of a human hand; (c) optical image of a person carrying a concealed weapon; (d) THz image of the same person (http://thznetwork.net/)
Fig.4  Schematics of the experimental setup of broadband THz generation and detection using gases. HV, high voltage; BBO, beta barium borate. Filter, 400 nm interference filter. Detector, photo-multiplier tube (Courtesy of Jianming Dai)
Fig.5  (a) Typical time-domain waveform of a THz pulse using air generation and air detection. A 35 fs ultrashort laser pulse is used for Thz generation and detection; (b) corresponding THz spectrum in the frequency domain. ABCD, air-biased-coherent-detection (Courtesy of I-Chen Ho)
Fig.6  (a) Schematic of the experimental setup for remote THz wave generation from laser-induced plasma in the ambient air. PC, phase compensator; M1, convex spherical mirror used to expand the optical beams; M2, concave spherical mirror used to remotely focus optical beams; (b) THz waveforms generated in ambient air at distances of 6.5, 10 and 17 m respectively. 1 mm thick ZnTe crystal was used as sensor (Courtesy of Jianming Dai)
Fig.7  Illustration of the frequent electron-molecules collisions within THz pulse duration. Small circles are electrons and big circles are molecules. Arrow represents the direction of electron motion
Fig.8  Illustration of the frequency of the electron-molecules collisions within the THz pulse duration (a) at extreme low pressure and (b) at extreme high pressure
Fig.9  Schematic of THz-REEF experiment. Red beam is 800 nm laser. Blue beam is the THz generated from the LiNbO3 prism. Purple beam is the fluorescence emission from the laser-induced plasma. Inset, the enlarged image of the LiNbO3 prism
Fig.10  (a) Schematics of the interaction between the THz wave and laser-induced plasma; (b) measured fluorescence spectra versus THz field as td=-1?ps; (c) measured quadratic THz field dependence of 357 nm fluorescence emission line as td=-1?ps. Inset: The isotropic emission pattern of THz-REEF
Fig.11  (a) Time-resolved THz-REEF ΔIFL(td) and THz field E→THz(td); (b) time-resolved ΔIFL(td), E→THz(td), dΔIFL(td)/dtd and E→THZ2(td) on the rising edge in the expanded scale of (a). All curves are normalized and offset for clarity
Fig.12  THz pulse enhanced fluorescence in nitrogen at a pressure range of 1300 to 10 torr. (a) Measured time-resolved ΔIFL(td) (offset for clarity); (b) expanded scale of the measured time-resolved ΔIFL(td) on the rising edge; (c) calculated time-resolved ΔIFL(td) on the rising edge
Fig.13  Vector potential A→(td) of THz pulse measured by THz REEF and the dA→(td)/dtd compared with the THz waveform measured by EO detection
Fig.14  Experimental setup of THz-REEF in gases. BS, beam splitter; PM, parabolic mirror; PMT, photo multiplier tube
Fig.15  (a) Ne fluorescence spectra between 580 and 760 nm at different laser pulse energies (without THz field). The Ne fluorescence spectra at the laser pulse energies of (b) 100, and (c) 120 μJ in the THz field
Fig.16  Laser pulse energy dependence of (a) absolute emission intensity and (b) enhancement ratio of Ne 702 nm line in the THz field
Fig.17  (a) Ar fluorescence spectra between 680 and 780 nm at different laser pulse energies (without THz field). The Ar fluorescence spectra at laser pulse energies of (b) 80, (c) 100, and (d) 140 μJ in the THz field
Fig.18  Pulse energy dependence of (a) absolute emission intensity and (b) relative enhancement of Ar 763 nm line in the THz field
Fig.19  (a) Kr fluorescence spectra between 820 and 900 nm at different laser pulse energies (without THz field). The Kr fluorescence spectra at laser pulse energies of (b) 60, (c) 70 and (d) 90 μJ in the THz field
Fig.20  Pulse energy dependence of the (a) 759 nm line and (b) continuum emission in Kr plasma in the THz field; (c) pulse energy dependence of the enhancement ratio in the THz field. The shadow area is the enhancement saturation region
Fig.21  (a) Xe fluorescence spectra between 810 and 850 nm at different laser pulse energies (without THz field). The fluorescence spectra at laser pulse energies of (b) 40, (c) 50, and (d) 80 μJ in the THz field
Fig.22  Pulse energy dependence of the (a) 823 nm line and (b) continuum emission in Xe plasma in the THz field; (c) laser pulse energy dependence of the enhancement ratio in the THz field. The shadow area is enhancement saturation region
Fig.23  Time-dependent enhancement of the fluorescence emission in Ar, Kr, and Xe gases when the excitation pulse energy is 70 μJ and pressure is 30 torr
Fig.24  Fluorescence spectra of alkane gases in the THz field
Fig.25  Schematics of the THz wave remote sensing. The 2ω pulse is generated by passing the fundamental beam through a type I β-BBO crystal. Both of the fundamental and second harmonic optical pulses are linearly polarized along a vertical direction. The relative phase change between the ω and 2ω pulses is tuned by the lateral translation of fused silica wedges in the optical beam path after the α-BBO. The two optical pulses are focused by a parabolic mirror with effective focal length of 150 mm into air to generate plasma. The time delay td is defined as the delay between optical pulse peak and THz pulse peak. The distance of the remote sensing is varied by moving the fluorescence detection system
Fig.26  Photo image of the in-line phase compensator consisting of a β-BBO crystal, a few α-BBO crystals, a pair of the fused silica wedges, and a dual wave plate.
Fig.27  (a) High-lying states can be ionized by a series of collisions with energetic electrons; (b) interaction between the THz pulse and the asymmetric photoelectron velocity distributions generated by two-color fields ionization; (c) measured phase dependence of fluorescence emission IFL and plasma-photocurrent-induced THz emission ITHzpla are compared with the calculated phase dependence of ion yield N2+ and ITHzpla; (d) zoom-in of c (shifted and normalized for clarity). Electron velocity direction is reversed as Δ?ω,2ω is changed by π
Fig.28  (a) 3D plot of THz-REEF at different relative optical phase between ω and 2ω pulses when ω, 2ω and THz beams are all vertically polarized; (b) 3D plot REEF at different relative optical phase when ω, 2ω beams are horizontally polarized and THz beam is vertically polarized; (c) 3D plot of differential REEF between ΔIFL(td,Δ?ω,2ω) with any velocity distribution and ΔIFL(td,0) with symmetric velocity distribution, under the same polarization condition as that in (a)
Fig.29  Measured time-resolved REEF at relative optical phase change Δ?ω,2ω=±lπ/2
Fig.30  (a) Measured time-resolved THz-REEF at phase Δ?ω,2ω=0,±π/2 respectively; (b) comparison between the THz waveform measured by electro-optic (EO) sampling and THz waveform obtained from the difference of the two REEF curves with opposite velocity distribution; (c) simulated THz-REEF derived from Eq. (12) at Δ?ω,2ω=0,±π/2, respectively
Fig.31  (a) Measured THz waveforms using REEF in dry nitrogen and ambient air environment, respectively; (b) corresponding THz spectra in logarithmic scale. The spectral resolution is 0.02 THz. Inset: Zoom-in on water vapor absorption features in shadow area
Fig.32  THz absorption spectrum of 4A-DNT measured by REEF compared with that measured by electric-optic sampling
Fig.33  Broadband THz wave remote sensing. The measured THz waveforms by EO sampling and REEF at different distances from plasma were shown respectively. Waveforms are normalized and shifted for clarity. Inset: THz spectrum measured at a distance of 10 m
Fig.34  Measured field dependence of the REEF signal (solid dots) and quadratic fit (dashed line) (a) in linear scale and (b) in log scale
Fig.35  Schematics of plasma characterization using THz-wave-enhanced fluorescence. IF, interference filter; PMT, photo-multiplier tube; Enh. Fl., enhanced fluorescence
Fig.36  Pressure dependences of the enhanced fluorescence (Enh. Fl.) in (a) pure nitrogen gas and (b) mixture of nitrogen and helium gas. The laser pulse energy is 80 μJ. (c) Comparison between measured (solid squares) and calculated (dash line) relaxation time. The error bar is due to the uncertainty from the fitting for 5 individual scans measured at the same pressure
Fig.37  (a) Measured (symbol) and fitted (line) ΔIFL(td) at 100, 300 and 500 torr, respectively. All the curves are normalized for clarity; (b) plasma densities extracted from ΔIFL(td) curves are compared with normalized background fluorescence signal (without THz field) at different pressures. Norm. Enh. Fl., normalized enhanced fluorescence
Fig.38  (a) Measured nitrogen fluorescence (Fl.) with different excitation laser pulse energies at 65 torr. The shade area is enlarged for clarity; (b) measured electron relaxation time. Inset, the measured background fluorescence signal (sold red circle) and calculated ion density being normalized to fluorescence signal (blue dash line)
Fig.39  (a) Schematic of the THz-wave-induced photoluminescence quenching experiment; (b) measured photoluminescence emission spectra of CdTe and GaAs at the peak THz intensity of 0 (solid lines) and 13 MW/cm2 (dashed lines)
Fig.40  Measured time-resolved photoluminescence (PL) quenching in CdTe at 837 nm (top) and in GaAs at 850 nm (middle) in comparison with the time-domain waveform of a THz pulse (bottom)
Fig.41  Solid black squares and red dots show the measured THz intensity dependence of photoluminescence in CdTe and GaAs, respectively. Solid lines are the linear fit. The error bars were obtained from the multiple measurements at the same point. Norm. PL, normalized photoluminescence
Fig.42  Measured photoluminescence signal (normalized) as a function of time delay between THz pulse and optical excitation pulse, and fitting results in (a) CdTe and (b) GaAs, respectively. PL Quen., photoluminescence quenching
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