CN101799420A - Metal micro-nano structure for improving Raman scattering of molecule - Google Patents
Metal micro-nano structure for improving Raman scattering of molecule Download PDFInfo
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Abstract
The invention relates to a metal micro-nano structure for improving Raman scattering of molecule, which comprises the following steps: (1) estimating limitation of internal memory capacity of a computer; (2) determining parameters such as mesh partition, peripheral medium environment conditions and exciting light condition, and primarily determining initial parameters of the metal micro-nano structure; (3) calculating scattering property Qsca of the metal micro-nano structure; (4) calculating plasma resonant frequency gamma LSPR for simulating the metal micro-nano structure and comparing the plasma resonant frequency gamma LSPR with the system exciting light frequency gamma ex, if the plasma resonant frequency is basically equal to the system exciting light frequency, the next step is entered, and if the plasma resonant frequency is not equal to the system exciting light frequency, the parameters of the peripheral medium environment condition of the metal micro-nano structure is changed; (5) calculating Raman reinforcing factor of the metal micro-nano structure; (6) preparing the micro-nano structure through the parameters of the metal micro-nano structure obtained in the step (4); (7) and realizing the metalation of the micro-nano structure. The metal micro-nano structure can maximally strengthen the Raman scattering of the molecule to be tested, can realize the low-concentration detection, and is simple and practical.
Description
Technical field
The invention belongs to the micro-nano technical field, relate to a kind of metal micro-nanostructure, particularly a kind of metal micro-nanostructure that strengthens Raman scattering of molecule.
Background technology
Raman scattering (RS) is a kind of scattering phenomenon of light, is photon and testing molecule interaction when monochromatic incident light, and inelastic collision takes place, and between photon and the molecule energy exchange takes place, and photon changes the scattering that direction of motion and frequency took place.Raman spectrum is by India physicist 1930 Nobel laureate C.V.Raman invention, and Raman spectrum (RS) is called as the dactylogram of molecule, can be used for structure analysis, has clear and definite directive property.But, be a kind of absorption spectrum, so weak strength because itself and infrared spectrum are similar.
Research to the Raman scattering enhancement effect at present only rests on the primary stage, and the mechanism of generation effect is also indeterminate.Show Raman scattering intensity ∝ 1/ λ after deliberation
4Adopt equal laser power, the raman spectral signal intensity of 266nm laser excitation is 2 of 532nm laser excitation raman spectrum strength (Stokes and anti-Stokes)
4=16 times.Therefore can adopt ultraviolet light to improve Raman signal, but this method may excite more fluorescence.In addition, when adopting tuning excitation wavelength to the molecule absorption peak, can obtain hundred times and even to ten thousand times resonance enhancement, one side is the elevator system detection limit significantly, can realize selective excitation (2-4 the order of magnitude that the molecule (s) of interest launching efficiency is surpassed other molecules in the experimental system) on the other hand.But enhancement effect is limited.Simultaneously, ultraviolet resonance raman system is for the Raman spectrum collection system, the luminous flux optimization of spectrometer and the optimization of spectrum CCD or ICCD all have very high requirement, the laser instrument of ultraviolet band, the spectrum CCD of optical system, the microscope that ICCD and even ultraviolet are optimized is all expensive, has limited the widespread use of this method.
Summary of the invention
The problem to be solved in the present invention is: overcome that prior art Raman scattering enhancer is low, the shortcoming of apparatus expensive, a kind of metal micro-nanostructure of high enhancer is provided, make the testing molecule Raman scattering obtain the maximum method that strengthens.
The technical solution adopted for the present invention to solve the technical problems is: a kind of metal micro-nanostructure that strengthens Raman scattering of molecule, and the method for making step is as follows:
(1), selects the Electromagnetic Calculation method for use, estimation calculator memory capacity limit according to molecular detection;
(2) according to the calculator memory capacity limit that obtains in the step (1), determine grid dividing, surrounding medium environment refractive index, excitation wavelength, tentatively determine the parameter of metal micro-nanostructure then, the parameter of described metal micro-nanostructure comprises material, characteristic dimension, cycle, arranges;
(3) utilize condition in the step (2), calculate the Extinction Characteristic Qext of metal micro-nanostructure and the absorption characteristic Qabs of metal micro-nanostructure,, obtain the scattering properties Qsca of metal micro-nanostructure by the difference of Extinction Characteristic Qext and absorption characteristic Qabs;
(4) utilize the scattering properties Qsca of the metal micro-nanostructure that obtains in the step (3), calculate the plasma resonance frequency lambda of simulation metal micro-nanostructure
LSPR, and with structure plasma resonance frequency lambda
LSPRCompare with the exciting light frequency lambda ex of system, change next step (5) over to,, then return step (2), remodify the parameter and the surrounding medium environmental baseline of metal micro-nanostructure if both are unequal if both are equal;
(5) calculate the average electric field enhancer E (w) of metal micro-nanostructure and the electric field enhancer E that testing molecule is located at characteristic peak w ' (w '), and then obtain metal micro-nanostructure Raman enhancer F (w)=E (w) E (w ');
(6) the metal micro-nanostructure parameter of utilizing step (4) to draw adopts the method for nanosphere self assembly or interference lithography or impression or two-photon laser direct-writing to prepare micro-nano structure;
(7) method of the micro-nano structure that obtains in the step (6) being passed through magnetron sputtering or evaporation or electroless plating realizes the micro-nano structure metallization, finally obtains metal micro-nanostructure.
Molecule in the described step (1) is gas molecule or solid molecule or fluid molecule.
Electromagnetism in the described step (1) calculates analogy method by discrete dipole approximate (DDA) or Finite Difference-Time Domain branch (FDTD) or finite element method or method of transition matrices or strict coupled modes analysis means, and the situation that the nano-structure array electromagnetic field distributes is analyzed and calculated to the physical characteristics of metal nano particles array.
Surrounding medium environmental baseline in the described step (1) is ambient environmental conditions material or optical field distribution or Distribution of Magnetic Field.
The advantage that the present invention is compared with prior art had is: it is low that the present invention overcomes prior art Raman scattering enhancer, the shortcoming of apparatus expensive, a kind of metal micro-nanostructure of high enhancer is provided, it strengthens principle based on the Raman electromagentic resonance: if molecule is in when taking place in the local surfaces plasma resonance enhancing electromagnetic field, its Raman scattering signal will be amplified greatly, make the testing molecule Raman scattering obtain the maximum method that strengthens, and it is simple and practical, solved the key technical problem of realizing low-concentration detection, this method is surveyed the development Raman spectrum and is had great significance, and can be widely used in the gas trace and surveys, or high sensitivity solid, fields such as solution detection.
Description of drawings
Fig. 1 is the little realization flow figure of metal that the present invention strengthens Raman scattering of molecule;
Fig. 2 is that the present invention utilizes metal Nano structure to realize the schematic diagram that Raman scattering strengthens, wherein Fig. 2 a is the Raman scattering situation of testing molecule when not adding metal Nano structure, after Fig. 2 b is the additional metal nanostructured, the Raman scattering of testing molecule strengthens, among the figure: 1, testing molecule, 2, micro-nano metal construction, 3, the Raman scattering of testing molecule, 4, the Raman scattering after strengthening.
Embodiment
As shown in Figure 1, the present invention realizes by following steps:
(1), selects the Electromagnetic Calculation method for use, estimation calculator memory capacity limit according to molecular detection;
(2) according to the restriction of the memory size that obtains in the step (1), determine grid dividing, surrounding medium environment refractive index, excitation wavelength, the material of the metal micro-nanostructure of input in the processing conditions allowed band, characteristic dimension, cycle, the initial parameter of arranging;
The specific implementation of this step is:
A. according to the restriction of the memory size that obtains in the step (1), determine that computing grid divides, as different grid dividing such as 512 * 512 or 1024 * 1024 or 2048 * 2048;
B. import the surrounding medium environmental baseline, as refractive index size, magnetic field size, distribution of light intensity etc.;
C. import the material, characteristic dimension, cycle of the metal micro-nanostructure in the processing conditions allowed band, the initial parameter of arranging;
(3) utilize Extinction Characteristic Qext, absorption characteristic Qabs and the scattering properties Qsca that calculates analogy method emulation metal micro-nanostructure;
The specific implementation of this step is:
A. calculate the Extinction Characteristic Qext of metal micro-nanostructure, Q
Ext=C
Ext/ π a
2 Eff, wherein, C
ExtBe extinction coefficient, a
2 EffA parameter for the characterizing metal micro-nano structure;
B. calculate the absorption characteristic Qabs of metal micro-nanostructure, Q
Abs=C
Abs/ π a
2 Eff, wherein, C
AbsBe absorption coefficient, a
2 EffA parameter for the characterizing metal micro-nano structure;
C. by the difference of Extinction Characteristic Qext and absorption characteristic Qabs, obtain the scattering properties Qsca of metal micro-nanostructure, Qsca=Qext-Qabs;
(4) calculate the plasma resonance frequency lambda of simulating metal micro-nanostructure
LSPR, and with the exciting light frequency lambda ex of system relatively, if both equate then change next step over to, if both are unequal, then return step (2), revise material or the characteristic dimension or the cycle of metal micro-nanostructure or arrange or the surrounding medium environmental baseline;
Being embodied as of this step:
A. calculate the plasma resonance frequency lambda of simulation metal micro-nanostructure
LSPR(known in this field, it is the strongest to resonate, delustring point of maximum intensity wavelength)
B. with the plasma resonance frequency lambda that obtains among a
LSPRCompare with the exciting light frequency lambda ex of system, if both equate then change next step over to;
If relatively λ among the b c.
LSPRUnequal with λ ex, then return step (2), revise material or the characteristic dimension or the cycle of metal micro-nanostructure or arrange or the surrounding medium environmental baseline;
(5) calculate the average electric field enhancer E (w) of micro-nano structure, E (w)=| E|
2, testing molecule levy the electric field enhancer E that peak w ' locates (w ', E (w ')=| E|
2, and then obtain metal micro-nanostructure Raman enhancer F (w)=E (w) E (w ');
(6) the metal micro-nanostructure parameter of utilizing step (4) to draw utilizes the method for nanosphere self assembly or interference lithography or impression to prepare micro-nano structure;
(7) utilize the method for magnetron sputtering or evaporation or electroless plating to realize the micro-nano structure metallization.
Fig. 2 is that the present invention utilizes metal Nano structure to realize the schematic diagram that Raman scattering strengthens, and wherein a is the Raman scattering situation of testing molecule when not adding metal Nano structure, and after the more weak b of scattering was the additional metal nanostructured, the Raman scattering of testing molecule strengthened.
The present invention is described in more detail below by embodiment
Present embodiment is the metal micro-nanostructure that strengthens glucose solution.
Implementation procedure is: (1) is little according to molecular detection glucose molecule structure, selects for use discrete dipole approximate (DDA) to be the Electromagnetic Calculation method, and the workstation calculated capacity is about 8G;
(2) input division grid is that 1024 * 1024 matrixes, surrounding medium environmental baseline are air, and refractive index is 1, and exciting light is selected 442nm laser for use; Select metallic gold for use, characteristic dimension is 50nm, and the cycle is 300nm, and the triangular array that regular hexagon is arranged, thickness are 20nm;
(3) utilize Extinction Characteristic Qext, absorption characteristic Qabs and the scattering properties Qsca that calculates analogy method emulation metal micro-nanostructure; Absorption characteristic Q
Abs=C
Abs/ π a
2 Eff, C wherein
AbsBe scattering cross-section, a
2 EffFor characterizing the parameter of micro-nano structure size, Extinction Characteristic Q
Ext=C
Ext/ π
Eff, C wherein
ExtBe the delustring cross section.
(4) calculate the plasma resonance frequency lambda of metal micro-nanostructure
LSPRBe 550nm, compare with the exciting light frequency lambda ex of system (442nm) that both differ bigger, the thickness of revising metal micro-nanostructure is 10nm, and the cycle is 330nm, calculates emulation again, the plasma resonance frequency lambda of metal micro-nanostructure
LSPRSuitable substantially with the exciting light frequency lambda ex of system;
(5) the average electric field enhancer E (w) according to micro-nano structure is 10
3, glucose molecule is 10 at characteristic peak (w '=the electric field enhancer E that 1146nm) locates (w ')
4, calculating glucose molecule is 10 at characteristic peak (w '=Raman enhancer F (w)=E (w) E of 1146nm) locating (w ')
7
(6) output metal micro-nanostructure parameter, metallic gold, characteristic dimension are 50nm, and the triangular array that regular hexagon is arranged, thickness are 10nm, and the cycle is 330nm, utilizes the method for nanosphere self assembly to prepare micro-nano structure;
(7) utilize the method for magnetron sputtering to realize the micro-nano structure metallization, finish the making of the metal micro-nanostructure that strengthens glucose solution.
If adopt that nano metal colloidal sol produces at random, incoherent output, only can reach 1 * 10
4About Raman scattering strengthen.This method has improved the Raman scattering of glucose solution, utilizes this method can realize low-concentration detection.
Present embodiment is the metal micro-nanostructure that strengthens the solid molecule.(1) suitable substantially according to molecular detection structure and wavelength, select FDTD Electromagnetic Calculation method for use, calculated capacity is about 2G; (2) input division grid is 512 * 512 matrixes, and exciting light 365nm laser is selected argent for use, and characteristic dimension is 150nm, and the cycle is 350nm, and the rhombus array that quadrilateral is arranged, thickness are 120m; (3) utilize Extinction Characteristic Qext, absorption characteristic Qabs and the scattering properties Qsca that calculates analogy method emulation metal micro-nanostructure; (4) calculating the plasma resonance frequency of simulating metal micro-nanostructure is 360nm, and compares with the exciting light frequency 365nm of system, and both are equal substantially, directly change next step over to; (5) the average electric field enhancer E (w) that calculates micro-nano structure is 10
2, testing molecule is 10 levying the electric field enhancer E that locates at peak (w ') (w ')
2, and then to obtain metal micro-nanostructure Raman enhancer F (w)=E (w) E (w ') be 10
4(6) output metal micro-nanostructure parameter utilizes the method for nano impression to prepare micro-nano structure; (7) utilize the method for chemical silvering to realize the micro-nano structure metallization, realize the making of the metal micro-nanostructure of enhancing solid molecule.
Roughened metal surface produces at random, incoherent output if adopt, and only can reach 1 * 10
3About Raman scattering strengthen.This method has improved the Raman scattering of solid molecule.
A kind of metal micro-nanostructure that strengthens the TNT gas molecule of present embodiment design.(1) according to survey the TNT molecular structure little, select for use discrete dipole approximate (DDA) to be the Electromagnetic Calculation method, calculated capacity is about 4G; (2) the input computing grid is divided 980 * 980 matrixes, surrounding medium for adding magnetic field vacuum, exciting light 780nm, selects argent for use, and characteristic dimension is 30nm.Cycle is 250nm, and the triangular array that quadrilateral is arranged, thickness are 50nm; (3) utilize Extinction Characteristic Qext, absorption characteristic Qabs and the scattering properties Qsca that calculates analogy method emulation metal micro-nanostructure; (4) calculate the plasma resonance frequency lambda of simulating metal micro-nanostructure
LSPR, and compare with the exciting light frequency lambda ex of system, both are equal substantially, change next step over to; (5) the average electric field enhancer E (w) according to micro-nano structure is 10
4, the TNT molecule is 10 at characteristic peak (w '=the electric field enhancer E that 780nm) locates (w ')
6Calculating glucose molecule is 10 at characteristic peak (w '=Raman enhancer F (w)=E (w) E of 780nm) locating (w ')
10(6) output metal micro-nanostructure parameter utilizes the method for interference lithography to prepare micro-nano structure; (7) utilize the method for evaporation to realize the micro-nano structure metallization, realize the making of the metal micro-nanostructure of enhancing TNT gas molecule.
It is low that the present invention overcomes prior art Raman scattering enhancer, the shortcoming of apparatus expensive, a kind of metal micro-nanostructure of high enhancer is provided, it strengthens principle based on the Raman electromagentic resonance: if molecule is in when taking place in the local surfaces plasma resonance enhancing electromagnetic field, its Raman scattering signal will be amplified greatly, make the testing molecule Raman scattering obtain the maximum method that strengthens, and it is simple and practical, solved the key technical problem that Raman spectrum is surveyed, this method is surveyed the development Raman spectrum and is had great significance, and can be widely used in the gas trace and surveys, or high sensitivity solid, fields such as solution detection.
The non-elaborated part of the present invention belongs to general knowledge known in this field.
The above only is a preferred implementation of the present invention; should be pointed out that for those skilled in the art, under the prerequisite that does not break away from the principle of the invention; can also make some improvements and modifications, these improvements and modifications also should be considered as protection scope of the present invention.
Claims (4)
1. metal micro-nanostructure that strengthens Raman scattering of molecule, it is characterized in that: the method for making step of described metal micro-nanostructure is as follows:
(1), selects the Electromagnetic Calculation method for use, estimation calculator memory capacity limit according to molecular detection;
(2) according to the calculator memory capacity limit that obtains in the step (1), determine grid dividing, surrounding medium environment refractive index, excitation wavelength, tentatively determine the parameter of metal micro-nanostructure then, the parameter of described metal micro-nanostructure comprises material, shape, characteristic dimension, cycle, arranges;
(3) utilize condition in the step (2), calculate the Extinction Characteristic Qext of metal micro-nanostructure and the absorption characteristic Qabs of metal micro-nanostructure, and obtain the scattering properties Qsca of metal micro-nanostructure by the difference of Extinction Characteristic Qext and absorption characteristic Qabs;
(4) utilize the scattering properties Qsca of the metal micro-nanostructure that obtains in the step (3), calculate the plasma resonance frequency lambda of simulation metal micro-nanostructure
LSPR, and with structure plasma resonance frequency lambda
LSPRCompare with the exciting light frequency lambda ex of system, change next step (5) over to,, then return step (2), remodify the parameter and the surrounding medium environmental baseline of metal micro-nanostructure if both are unequal if both are equal;
(5) calculate the average electric field enhancer E (w) of metal micro-nanostructure and the electric field enhancer E that testing molecule is located at characteristic peak w ' (w '), and then obtain metal micro-nanostructure Raman enhancer F (w)=E (w) E (w ');
(6) the metal micro-nanostructure parameter of utilizing step (4) to draw adopts the method for nanosphere self assembly or interference lithography or impression or two-photon laser direct-writing to prepare micro-nano structure;
(7) method of the micro-nano structure that obtains in the step (6) being passed through magnetron sputtering or evaporation or electroless plating realizes the micro-nano structure metallization, finally obtains metal micro-nanostructure.
2. a kind of metal micro-nanostructure that strengthens Raman scattering of molecule according to claim 1 is characterized in that: the molecule in the described step (1) is gas molecule or solid molecule or fluid molecule.
3. a kind of metal micro-nanostructure that strengthens Raman scattering of molecule according to claim 1, it is characterized in that: the electromagnetism in the described step (1) calculates analogy method and is similar to or Finite Difference-Time Domain branch or finite element method or method of transition matrices or coupled modes analysis means by discrete dipole, and the situation that the nano-structure array electromagnetic field distributes is analyzed and calculated to the physical characteristics of metal nano particles array.
4. a kind of metal micro-nanostructure that strengthens Raman scattering of molecule according to claim 1 is characterized in that: the surrounding medium environmental baseline in the described step (1) is ambient environmental conditions material or optical field distribution or Distribution of Magnetic Field.
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| CN103204460A (en) * | 2013-03-21 | 2013-07-17 | 北京工业大学 | Production method of metal micro-nano structure based on laser interference induced cross-linking reaction |
| CN103853878A (en) * | 2013-12-19 | 2014-06-11 | 兰州空间技术物理研究所 | Method for simulating potential of dielectric material on surface of spacecraft on geosynchronous orbit |
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| CN103204460A (en) * | 2013-03-21 | 2013-07-17 | 北京工业大学 | Production method of metal micro-nano structure based on laser interference induced cross-linking reaction |
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| CN103853878B (en) * | 2013-12-19 | 2017-02-01 | 兰州空间技术物理研究所 | Method for simulating potential of dielectric material on surface of spacecraft on geosynchronous orbit |
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| CN108956577B (en) * | 2017-04-17 | 2020-12-18 | 中国科学院物理研究所 | Detection method based on one-dimensional nano material |
| CN108441843A (en) * | 2018-03-13 | 2018-08-24 | 北京科技大学 | Preparation method is plated in the laser direct-writing preform photocatalysis of material surface metal pattern |
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| CN111218653B (en) * | 2020-01-14 | 2022-03-11 | 江苏师范大学 | Surface-enhanced Raman scattering substrate of spatially folded silver nanorods and preparation method thereof |
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