CN115046958A - Terahertz super-surface enhanced fingerprint detection method based on incident angle scanning - Google Patents
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Abstract
The invention discloses a terahertz super-surface enhanced fingerprint detection method based on incident angle scanning. The invention comprises a substrate and four medium cylinders positioned above the substrate, and optimizes the structural parameters of the sensor, so that the characteristic absorption frequency of the selected analyte to be detected is positioned in the working frequency range of the sensor; placing an analyte to be detected on the surface of a sensor, obtaining a series of transmission peak spectrums by continuously changing the incident angle of terahertz waves, and forming a wide-range transmission envelope band by frequency shift of the lowest peak point of the transmission peak spectrums; and judging whether the target analyte exists or not by comparing the transmittance difference of the envelope bands of the transmission peaks before and after the analyte to be detected is loaded. The invention can realize qualitative identification by directly obtaining fingerprint peaks of the analytes, has high sensitivity and can realize the measurement of the target analytes with the thickness of 0.1 micrometer.
Description
Technical Field
The invention relates to a method for enhancing detection of trace analytes by taking a terahertz super-surface structure based on incident angle scanning as a detection device, belonging to the technical field of terahertz detection application.
Background
As most of spectral information such as absorption, dispersion, characteristic absorption frequency and the like represented by intramolecular or intermolecular rotation and collective vibration transition of biomolecules are in the terahertz waveband, the identification of the type of a target analyte can be realized through the absorption fingerprint spectrum of the target analyte to terahertz waves, which is the most popular research in the field of terahertz detection application at present. In addition, the terahertz spectrum has been rapidly developed and applied in recent years due to its characteristics of high penetration, low photon energy, fingerprint characteristics, nondestructive testing, etc., and is a new testing technology and applied to a plurality of fields such as physics, chemistry, biomedicine, environmental monitoring, etc. However, since the nanoscale size of most analyte molecules is much smaller than the micron-sized size of terahertz wavelengths, the interaction between the molecules and terahertz waves is very weak, and it is almost difficult to observe the fingerprint spectrum of the analyte molecules. In conventional Terahertz detection methods using transmission, the analyte is usually detected in the form of a solid tablet, the thickness of the sample particles typically reaches several millimeters, which means that a large sample of analyte is required (l.ho, m.pepper, et al, "Terahertz spectroscopy: Signatures and fingers," nat. photonics 2(9),541 (2008)). Obviously, such a conventional terahertz detection method is not suitable for detecting a trace amount of analyte. The mismatch between the terahertz wavelength and the molecular size greatly hinders the development and application of terahertz in trace analyte detection, and researchers make many efforts to solve the problem. Lee (D.K. Lee, J.H. Kang, et al, "high hly inductive and selective surface detection by terahertz nano-antennas," Sci.Rep.5(1),15459(2015) ") et al, using a nano-antenna structure operating in the frequency range of terahertz (0.5-2.5THz), can effectively increase the molecular absorption cross-section, achieve detection of various types of carbohydrate molecules in the molecular concentration range of hundreds micromolar to tens micromolar, and provide a prospect for detecting molecules in the terahertz band. X.Shi (X.Shi, Z.ZHao, et al, "high throughput sensing and selective gas sensing using the defect mode of a compact terrestrial photonic crystal cavity," Sens.actuators B chem.274, 188-193 (2018)), and others successfully detected the analyte at the nanometer level based on the cavity defect mode of the one-dimensional photonic crystal cavity, but the requirements for the precision of the detection device are high, and the operation process is complicated and difficult. Based on the multi-pole plasmon resonance research, the corrugated metal disc can show huge local field enhancement in the terahertz range, which indicates that the corrugated metal disc structure has potential application prospect in the aspect of sensing.
Disclosure of Invention
The invention provides a terahertz super-surface enhanced fingerprint detection method based on incident angle scanning, aiming at the problem that the existing terahertz detection technology is difficult to detect trace analyte samples, and the method can effectively improve the sensitivity of terahertz fingerprint detection and realize the identification and detection of target analytes with the thickness of 0.1 micrometer.
In order to achieve the above object, the technical scheme adopted by the invention is as follows:
a terahertz super-surface enhanced fingerprint detection method based on incident angle scanning comprises the following steps:
step a: designing an all-dielectric super-surface sensor for detection;
step b: recording the spectrum of a transmission peak of the super-surface sensor when the terahertz waves vertically enter, continuously changing the terahertz wave incident angle (the scanning range of the terahertz wave incident angle is 0-18 degrees, the step length is 0.25 degrees), and testing and recording 72 terahertz transmission spectra of the super-surface sensor after scanning;
step c: loading an analyte to be detected on the surface of the designed all-dielectric super-surface sensor, continuously scanning a terahertz wave incident angle (the scanning range of the terahertz wave incident angle is 0-18 degrees, and the step length is 0.25 degrees), and testing and recording 72 terahertz transmission spectrums of the analyte to be detected after scanning on the super-surface sensor;
step d: after the terahertz wave incident angle is continuously scanned, the lowest peak point of 72 terahertz transmission spectra forms a wide-range envelope band through frequency shift, and whether the target substance exists is judged by comparing the transmittance of the envelope band curve before and after the analyte to be detected is loaded.
The method comprises the following steps: after the super-surface sensor which is not loaded with the analyte to be detected is scanned by continuous terahertz wave incidence angles, the transmission peak spectrum generates blue shift, the lowest peak point of the blue-shifted transmission spectrum forms a wide-range envelope band through fitting, and the envelope band is a straight line with the transmittance approximate to zero. After the analyte to be detected is loaded, through continuous terahertz wave incident angle scanning, the lowest peak point of the transmission spectrum forms an envelope band through blue shift, the transmittance of the envelope band is increased at the characteristic absorption frequency of the analyte to be detected, so that the target analyte can be identified, the thickness of the loaded target analyte can be calculated by calculating the increase degree of the transmittance of the envelope band at the resonance frequency, and quantitative analysis is realized. The method based on the terahertz wave incident angle scanning can realize qualitative identification by directly obtaining the fingerprint spectrum of the analyte to be detected, compared with the traditional terahertz detection method, the method not only keeps the specificity of the terahertz spectrum fingerprint detection, but also can improve the detection sensitivity and realize the identification and detection of the analyte with the thickness of 0.1 micron, and the method is hopeful to be applied to the aspects of food safety detection, biochemical sensing and the like.
The transmission spectrum modulation depth of the all-dielectric super-surface sensor adopted by the method is approximately 100%, the super-surface sensor is subjected to transmission type detection by combining an angle scanning strategy, the characteristic fingerprint identification of an analyte with the thickness of 0.1 micrometer can be realized, and the method has the characteristics of high sensitivity, characteristic fingerprint detection, obvious enhancement of absorption signals and the like.
Preferably, the all-dielectric super-surface sensor in the step a comprises two parts, namely (1) and (2), wherein the first part (1) is a substrate layer, the substrate layer has a certain absorption effect on terahertz waves, and the substrate layer is silicon dioxide; the second part (2) is four dielectric cylinders above the substrate, where the dielectric cylinders are high-resistance silicon.
Preferably, in the step b, a transmission spectrum of the super surface sensor before the analyte to be measured is loaded when the incident angle of the terahertz wave is 0 ° (vertical incidence) is detected and recorded, a transmission spectrum when the incident angle is gradually converted from vertical to oblique incidence is detected and recorded, and the transmittance intensity of an envelope curve formed by the transmission spectrum is observed.
Preferably, in the step c, a transmission spectrum of the super-surface structure after the analyte to be detected is loaded when the incident angle is gradually converted from vertical to oblique incidence is detected and recorded, and the transmittance intensity of an envelope curve formed by the transmission spectrum is observed.
Preferably, in the step d, when the transmittance of the transmission envelope curve formed by the transmission spectrum at the characteristic absorption frequency of the analyte to be detected is obviously increased, the target analyte exists; when the envelope curve transmittance does not increase significantly, it indicates that the analyte to be detected is not the target analyte.
Preferably, after determining the presence of the target analyte in step d, the thickness of the target analyte loaded on the super-surface sensor can be calculated by calculating the degree of enhancement of the transmission rate of the envelope curve at the characteristic absorption frequency of the analyte. The method not only can realize the type identification of the analyte to be detected in the working frequency range of the sensor, but also can realize the quantitative analysis of the target analyte. By fitting the relationship between the analyte thickness and the transmission rate of the envelope curve at the resonance peak, the prediction of the thickness of the target analyte through the transmission rate can be theoretically realized.
The beneficial effects of the invention are: compared with the existing fingerprint detection method, the method is based on the combination of the all-dielectric super-surface sensor and the terahertz wave incident angle scanning strategy, not only can retain the fingerprint identification characteristic of terahertz spectrum detection, but also has high detection sensitivity, can realize the characteristic fingerprint detection and identification of the analyte with the thickness of 0.1 micrometer, and is expected to be used in the aspects of food safety, biochemical sensing and the like.
Drawings
FIG. 1 is a schematic diagram of terahertz enhanced fingerprint detection of an all-dielectric super-surface sensor according to the present invention;
FIG. 2(a) is the transmission spectrum of the super-surface sensor itself at normal incidence of terahertz waves; FIG. 2(b) is the electric field distribution of the transmission spectrum of the super-surface sensor at the plane of xoy and xoz when terahertz waves are vertically incident.
FIG. 3(a) is a graph showing the dielectric constant spectrum of the analyte α -lactose to be tested; FIG. 3(b) is a transmission spectrum of the super-surface sensor itself at a terahertz wave incident angle scanning range of 0 to 18 °; FIG. 3(c) is a transmission spectrum of loading alpha-lactose with a thickness of 0.1 micrometer on the surface of the super-surface sensor when the terahertz wave incident angle scanning range is 0-18 degrees;
FIG. 4(a) is a graph of the transmission envelope when the super surface sensor surface is loaded with different thickness of alpha-lactose;
FIG. 4(b) is a graph of a linear fit of transmittance at the resonance peak in the transmission envelope curve to the thickness of alpha-lactose when the super-surface structure is loaded with alpha-lactose of different thickness;
FIG. 5 is a graph of transmission envelopes of a super surface sensor coated with different analytes, respectively.
Detailed Description
The technical solution of the present invention is further described below by using specific embodiments and with reference to the accompanying drawings. It should be noted that the implementation of the present invention is not limited to the following embodiments, and any changes and/or modifications made to the present invention shall fall within the protection scope of the present invention.
The invention relates to a terahertz super-surface enhanced fingerprint detection method based on incident angle scanning, which comprises the following specific steps of:
step a, designing an all-dielectric super-surface sensor for detection;
step b, recording a transmission peak spectrum of the super-surface sensor when terahertz waves are vertically incident, continuously changing a terahertz wave incident angle (the scanning range of the terahertz wave incident angle is 0-18 degrees, the step length is 0.25 degrees), and testing and recording 72 terahertz transmission spectra of the super-surface sensor after scanning;
loading an analyte to be detected on the surface of the designed all-dielectric super-surface sensor, continuously changing a terahertz wave incident angle (the scanning range of the terahertz wave incident angle is 0-18 degrees, the step length is 0.25 degrees), and testing and recording 72 terahertz transmission spectrums of the analyte to be detected after scanning on the super-surface sensor;
and d, fitting the lowest peak value point of each transmission peak after scanning to form a wide transmission envelope curve, and judging whether the target substance exists or not by comparing the transmittance of the envelope band before and after the analyte to be detected is loaded.
The terahertz fingerprint detection schematic diagram of the super-surface sensor is shown in fig. 1: terahertz waves are incident on the super-surface structure at a variable angle, the substrate of the sensor is silicon dioxide, the dielectric constant is 3.75, the four dielectric columns above the substrate are silicon, the dielectric constant is 11.7, and the electric field polarization direction of incident electromagnetic waves is the Y direction during calculation. Parameters of the sensor are adjusted through CST software simulation, and the optimal parameters are as follows: the period P is 394 micrometers, the thickness d of the substrate layer is 98 micrometers, the thicknesses t of the four dielectric columns are 24 micrometers, the distance L between the centers of two adjacent dielectric columns is 144 micrometers, and the radii r of the four dielectric columns are 67 micrometers.
The transmission spectrum of the super-surface sensor under the vertical incidence is obtained through simulation of a frequency domain solver in CST, and the curve is shown in FIG. 2(a), so that the modulation depth of the super-surface sensor reaches 100%. The electric field distribution at the transmission peak was simultaneously calculated, as shown in FIG. 2 (b). From the electric field distribution on the xoy plane, it can be seen that the electric field energy is mainly limited in the central regions of the four cylinders, which indicates that the sensor has strong field confinement capability, and meanwhile, from the electric field distribution on the xoz plane, the electric field energy is mostly concentrated in the waveguide layer, and the propagation direction of the waveguide is the X direction.
In order to verify the feasibility of the terahertz super-surface enhanced fingerprint detection method based on incident angle scanning, alpha-lactose is selected as a target analyte, and in simulation, the relative dielectric constant of the alpha-lactose is characterized by a Lorentzian resonators (Lorentzian resonators) model:
wherein epsilon ∞ Background relative permittivity, ω, of non-resonance p And gamma p Angular frequency and damping rate, respectively, of the intrinsic absorption resonance p Is the oscillation intensity factor. For simple calculations, we only consider the characteristic absorption of a-lactose at 0.529THz, when ε is ∞ ＝3.145，γ p ＝1.59*10 11 rad/s,Δε p The dielectric constant profile of α -lactose is shown in fig. 3(a), and can be obtained from the real part profileThe average dielectric constant is seen to be 3.49, and it can be seen from the imaginary graph that there is a bump at the characteristic frequency of alpha-lactose.
The transmission spectrum of terahertz waves (at which the sensor surface is not loaded with the analyte) at an incident angle ranging from 0 ° to 18 ° (step size of 0.25 °) was numerically calculated, and the result is shown in fig. 3 (b). It can be seen that the transmission spectrum undergoes a blue shift as the angle of incidence increases and the lowest peak point of the resonance peak forms a broad envelope curve with a transmission of approximately 0. When the structure surface was directly loaded with 0.1 micron thick α -lactose, it can be seen that the intensity of the transmission envelope curve at the α -lactose characteristic frequency of 0.529THz was significantly increased, approximately 10% due to the absorption of α -lactose, with the results shown in fig. 3 (c). It can be seen from fig. 4(a) that the envelope curve transmittance at the characteristic frequency also shows a tendency of significantly increasing with the increase in the thickness of α -lactose. From fig. 4(b), it can be seen that the thickness of the loaded α -lactose is in a linear function relationship with the transmittance at the characteristic absorption peak, and the transmittance increases significantly with the increase of the thickness of the α -lactose, which indicates that we can predict the thickness of the loaded α -lactose to a certain extent by the transmittance at the resonance peak of the envelope curve, so as to realize quantitative analysis.
To verify that the method has a certain qualitative recognition capability, we consider alpha-lactose as the target analyte and D-glucose as the non-target analyte. The transmission spectrum was calculated by covering the ultra-surface sensor surface with a 0.4 μm thick α -lactose sugar, and as shown by the dotted line in fig. 5, the transmission of the envelope curve at a characteristic absorption frequency of 0.529THz of α -lactose was significantly enhanced, with an enhancement of about 20%. Taking the transmission envelope curve of the super surface sensor without the substance as a reference, as shown by the solid line in fig. 5, the transmittance of the envelope curve is 0. The transmission spectrum was calculated by covering the super-surface with D-glucose having a thickness of 0.4 μm, as shown by the dashed line in fig. 5, at which the transmittance of the envelope curve was almost 0, because the characteristic absorption frequency of D-glucose was in the vicinity of 1.4THz, and its absorption of terahertz waves was also present only in the vicinity of 1.4 THz. Therefore, the two different saccharides can be distinguished according to whether the resonance intensity at the resonance part of the transmission envelope curve is changed after scanning, so that the target analyte and the non-target analyte are distinguished and detected, and the qualitative identification effect is achieved. The present invention can distinguish the kind of target analyte by directly obtaining fingerprint spectrum of the analyte, and can predict the thickness of the analyte by using the enhancement degree of the transmittance to realize quantitative analysis.
The terahertz fingerprint detection method has the characteristics of high sensitivity, characteristic fingerprint and specificity selection, can realize qualitative identification and quantitative analysis, and has a great application prospect in the field of terahertz fingerprint detection.
The foregoing description of the specific embodiments is merely exemplary for the purposes of explanation and understanding, and is not intended to limit the invention in any way.
Claims (7)
1. A terahertz super-surface enhanced fingerprint detection method based on incident angle scanning is characterized by comprising the following steps:
step a, selecting a target analyte, and designing a super-surface sensor to enable the characteristic absorption frequency of the target analyte to be in the working frequency range of the super-surface sensor;
step b, recording the transmission peak spectrum of the super-surface sensor when the terahertz waves vertically enter, continuously changing the terahertz wave incident angle (the scanning range of the terahertz wave incident angle is 0-18 degrees, and the step length is 0.25 degrees), and testing and recording 72 terahertz transmission spectra of the super-surface sensor after scanning;
loading an analyte to be detected on the surface of the designed super-surface sensor, continuously changing a terahertz wave incident angle (the scanning range of the terahertz incident angle is 0-18 degrees, and the step length is 0.25 degrees), and testing and recording 72 terahertz transmission spectrums of the analyte to be detected after scanning on the super-surface sensor;
d, continuously scanning the incident angle of the terahertz wave, forming a wide transmission envelope band by the lowest peak point of 72 transmission peaks through frequency shift, and judging whether the target substance exists or not by comparing the transmittance difference of the transmission envelope band before and after loading the analyte to be detected; specifically, when the transmission rate of the envelope band at the characteristic absorption frequency of the analyte to be detected is obviously increased, the existence of the target analyte is indicated; when the envelope transmittance curve is not enhanced, the analyte to be detected is not the target analyte; after the target analyte exists, the thickness of the loaded target analyte can be calculated by calculating the enhancement degree of the transmission rate of the envelope band at the characteristic absorption frequency of the analyte;
the super-surface sensor is a unit structure array composed of a substrate layer (1) and a medium column layer (2) positioned above the substrate layer, wherein the medium column layer (2) is composed of four medium cylinders, and the electric field polarization direction of incident electromagnetic waves is the Y direction during calculation.
2. The terahertz super-surface enhanced fingerprint detection method based on incident angle scanning as claimed in claim 1, wherein: the substrate material of the super-surface sensor is silicon dioxide with a dielectric constant of 3.75, and the four dielectric cylinder materials above the substrate are high-resistance silicon with a dielectric constant of 11.7.
3. The terahertz super-surface enhanced fingerprint detection method based on incident angle scanning as claimed in claim 1, wherein: the period P of the designed super-surface sensor is 394 micrometers, the thickness d of the substrate layer is 98 micrometers, the thicknesses t of the four medium columns are 24 micrometers, the distance L between the centers of two adjacent medium columns is 144 micrometers, and the radiuses r of the four medium columns are 67 micrometers.
4. The terahertz super-surface enhanced fingerprint detection method based on incident angle scanning as claimed in claim 1, wherein: the four dielectric columns above the substrate are distributed in axial symmetry and central symmetry.
5. The terahertz super-surface enhanced fingerprint detection method based on incident angle scanning as claimed in claim 1, wherein in step a, the terahertz wave is incident on the super-surface sensor at a continuously varying angle, the incident angle is an included angle between the incident direction of the terahertz wave and the z-axis (the terahertz wave is incident along the xoz plane of the super-surface sensor), and the direction variation of the incident angle during continuous angle scanning is gradually converted from vertical incidence to oblique incidence.
6. The terahertz super-surface enhanced fingerprint detection method based on incident angle scanning as claimed in claim 1, wherein: when the polarization direction of an electric field of incident terahertz waves is the Y direction, regular frequency shift can be realized by the transmission peak scanned by continuous incident angles to form a transmission envelope band.
7. The terahertz super-surface enhanced fingerprint detection method based on incident angle scanning as claimed in claim 1, wherein in step d, when continuously scanning the incident angle of the terahertz wave, a series of transmission resonance peaks undergo frequency shift to form a wide transmission envelope band, and whether the target substance exists can be determined by whether the transmission rate of the transmission envelope band increases; when the transmittance of the transmission envelope band is increased, indicating that the target substance appears; otherwise, no target analyte is present; after determining the presence of the target analyte, the thickness of the loaded target analyte can be calculated by calculating the degree of enhancement of the transmission of the envelope at the characteristic absorption frequency of the analyte.
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