多面體變異在三元鹵化物及黃銅礦結構化合物對二階非線性光學性質影響之理論與實驗研究

唐立權

doi:10.6842/NCTU.2009.01041

3.236.156.34，Hello！

Close
Search Quick Search Advanced Search Publication Search	Personal Service Member Login Searching History Use Bonus Card SYMSKAN
Browse Browse by University of Graduate Thesis Browse by Pinyin of Graduate Thesis Browse by Conference Proceedings Topic Browse by Conference Proceedings Publisher Browse by Pinyin of Conference Proceedings Browse by eBook Category Browse by eBook Topic Browse by eBook Publisher
Customer Services Authorize Airiti Recommend a Journal

Search Symbol (Half-width)	Description of Search Symbols
Space	"AND" indicates the intertwining of key terms used in a search
Double Quotation Marks ("") ( " " )	Double quotation marks indicate the beginning and end of a phrase, and the search will only include terms that appear in the same order of those within the quotations. Example: "image process" ： " image process "
?	Indicates a variable letter. Entering two ? will indicate two variable letters, and so on. Example: "Appl?", search results will yield apple, apply… e , appl y … ( (often used to English word searches) )
*	Indicates an unlimited number of variable letters to follow, from 1~n. Example: Enter "appl*", search results will yield apple, apples, apply, applied, application…(often used in English word searches) e , appl es , appl y , appl ied , appl ication … ( (often used to English word searches) )
AND、OR、NOT	Boolean logic combinations of key words is a skill used to expand or refine search parameters. (1) AND (1) AND: Refines search parameters (2) OR (2) OR: Expands search parameters (3) NOT: Excludes irrelevant parameters

DOI stands for Digital Object Identifier （ D igital O bject I dentifier ） ,
and is the unique identifier for objects on the internet. It can be used to create persistent link and to cite articles.

Using DOI as a persistent link

To create a persistent link, add「http://dx.doi.org/」「 http://dx.doi.org/ 」 before a DOI.
For instance, if the DOI of an article is 10.5297/ser.1201.002 , you can link persistently to the article by entering the following link in your browser: http://dx.doi.org/ 10.5297/ser.1201.002 。
The DOI link will always direct you to the most updated article page no matter how the publisher changes the document's position, avoiding errors when engaging in important research.

Cite a document with DOI

When citing references, you should also cite the DOI if the article has one. If your citation guideline does not include DOIs, you may cite the DOI link.

DOIs allow accurate citations, improve academic contents connections, and allow users to gain better experience across different platforms. Currently, there are more than 70 million DOIs registered for academic contents. If you want to understand more about DOI, please visit airiti DOI Registration （ doi.airiti.com ）。

Data Source

Cellege of Electrical Engineering > Department of Electro-Optical Engineering
Engineering > Electrical Engineering

Bibliography Management Tool

Related Links

Report an Issue

Purchase Single Articles

Download PDF

多面體變異在三元鹵化物及黃銅礦結構化合物對二階非線性光學性質影響之理論與實驗研究

Theoretical and experimental studies of second-order nonlinear optical properties for various polyhedron distortions in ternary halides and some chalcopyrite compounds

唐立權 , Ph.D　　Advisor：張振雄;黃中垚　　

英文 DOI： 10.6842/NCTU.2009.01041

第一原理計算；二階非線性係數；三元鹵化物；三元氮化物；多面體變異；紅外線； the first principles calculation ； 2nd-order nonlinear optical susceptibility ； the ternary halides ； the ternary nitrides ； polyhedron variations ； infrared

Abstract │ Reference (141) │ Times Cited (115) │ Altmetrics

Abstract 〈TOP〉

Parallel Abstract 〈TOP〉

Microstructures, electronic structures, linear- and nonlinear-optical properties of the crystals
with two main polyhedron categories are examined in this study by using both the first principles
calculation and the experimental methods. The studied crystals include the rhombohedral
ternary halides (ABX$_3$ (A=Cs, Rb, B=Ge, X=Cl, Br, I)),
the wide-bandgap ternary nitrides($A^{II}B^{IV}N_2$ ($A^{II}=Be, Mg$, $B^{IV}=C, Si, Ge$)),
and chalcopyrite AgGaS$_2$, AgGaSe$_2$, and AgGa(S$_x$Se$_{1-x}$)$_2$.
\
First, one of the most important parts, systematic studies based on first-principles calculations of second-order optical susceptibilities as well as the
dielectric function for CsGeX$_3$ (X=Cl, Br, and I; CGX) are presented.
The relation between structural properties and the optoelectronic responses are examined.
The structural factors, $Delta alpha$, $d_{Ge}$, $d_X$  are proposed to describe the degree of
distortion from an ideal perovskite structure. $Delta alpha$ and $d_{Ge}$ increase when the halide anions are changed
from Cl to I; while halide anion displacement, $d_X$, decreases.
The structural distortion effect
on these rhombohedral CGX crystals is analyzed via the first-principles calculations.
The dielectric function and the second harmonic
generation (SHG) response coefficient also increase with increasing $Delta alpha$ and $d_{Ge}$.
The direct bandgaps, $E_G$, of CsGeX$_3$ all occur at the $R$-point, $Delta E_R$.
The experimental bandgaps of CGX crystals become smaller, i.e. $E^{CGC}_G$(3.67eV)$>E^{CGB}_G$(2.32eV)$>E^{CGI}_G$(1.53eV),
as the $Delta alpha$ and $d_{Ge}$ increase, i.e. $d^{CGC}_{Ge}<d^{CGB}_{Ge}<d^{CGI}_{Ge}$.
Partial density of states (PDOS) analysis revealed that the valence
band maximun (VBM) and conduction band minimum (CBM) are mainly contributed from the p-orbitals of Germanium.
The calculated magnitudes of $chi^{(2)}_{ijk}$ are close to some reported experimental values near the band gap.
\
Second, the nonlinear optical (NLO) property of hydrated rubidium germanium chloride (HRGC),
RbGeCl$_3cdot x$(H$_2$O), is identified. Infrared absorption data support
structural evidence that HRGC contain co-ordinated water
molecules with strong hydrogen bond. The infrared spectrum indicated HRGC
is transparent in most of the infrared region with only little influnce from water.
Calculations based on density functional theory shows that the band gap of the RbGeCl$_3$ (RGC) crystal is at least 3.84eV,
which is larger than that of the infrared (IR) NLO crystal CsGeCl$_3$. Single crystals of HRGC,
sized up to 3 $	imes$ 2 $	imes$ 1 cm$^3$, were
grown in aqueous solution by a slow dehydrate technique.
The synthetic, structural, and optical properties of an off-centrosymmetric IR
nonlinear optical (NLO) RbGeCl$_3cdot x$(H$_2$O) crystal were investigated experimentally.
Powder second harmonic generation (PSHG) measurement indicates that the crystal structure of
HRGC becomes off-centrosymmetric.
Precise X-ray diffraction measurements showed that [100] family diffraction peaks split slightly.
Unlike the RGC crystal structure whose space group is P2$_1ar m$,
the HRGC crystal loses the inversion symmetry. Comparisons with known NLO material
KH$_2$PO$_4$ (KDP), indicate that HRGC's NLO susceptibility, $chi^{(2)}$, is about one third
of that for KDP.
The absorption edge of HRGC occured at 310nm ($approx$4.0 eV), which indicates NLO
HRGC crystal can have larger laser damage threshold.
According to the $FTIR$ measurement, HRGC has a transparent region from 0.31 to
30 $mu$m, thus it can
be applied to wider optical spectrum from ultraviolet, visible, to mid-IR.
\
Third, both tetragonal and orthorhombic ternary nitrides $A^{II}B^{IV}N_2$ ($A^{II}$=Be, Mg; $B^{IV}$=C, Si, Ge) are studied by using the first principles calculation, and are compared to the available experimental results. This study reveals the electronic properties, linear and second-order nonlinear optical ($NLO$) properties of the ternary nitrides compounds with chalcopyrite structure performed using the Linear Augmented Slater-Type Orbitals (LASTO) method. The linear and second-order optical susceptibilities as functions of frequency are presented. Specifically, we study the relation between the structural properties and the optical responses. Our electronic band structure and projected density of states (PDOS) analysis reveal that these chalcopyrite $A^{II}B^{IV}N_2$ compounds are direct (with band extrema
 located at the $Gamma$-point) and their band gaps are wide
[from 2.68eV ($BeGeN_2$) to 4.24eV($MgCN_2$)].  Our PDOS analysis also shows that the effective masses of highest valence band are heavy in $MgSiN_2$ and $MgGeN_2$, which are different from other $A^{II}B^{IV}N_2$ compounds. Our calcultions show this new category of wide-bandgap ternary nitrides have potential applications in optoelectronics.
\
Finally, the lattice parameters, electronic structures, optical and bulk
properties of tetragonal nonlinear optical crystals, AgGa(S$_x$Se$_{1-x}$)$_2$ (x=0.0, 0.25, 0.5,
0.75, and 1.0), have been analyzed theoretically with first-principle
calculation and measured experimentally in each composition. Our
calculation results indicate that in these compounds, their electronic
band gaps, optical properties, and bulk moduli are linearly dependent,
which are compatible with the experimental measurements. We also find
the proportionally mixed electronic contributions from sulfur and
selenium at band edges via the partial density of state (PDOS) analysis
of . The linear-dependent relationship of their electronic properties
can be considered as the cell-volume-effect. Furthermore, the cell
parameters, bond length between metal ion and 	extit{S}
or 	extit{Se}, band gap values, and nonlinear optical (NLO)
susceptibilities are also found linearly dependent on the compositions
and the related cell volumes.\

Reference ( 141 ) 〈TOP〉

[1] V~G Dmitriev, G~G Gurzadyan, and D~N Nikogosyan. "Handbook of Nonlinear Optical Crystals," third ed., Springer-Verlag,
連結：
Berlin, 1999.
連結：
[4] Y~R Shen. The Principles of Nonlinear Optics, John Wiley and Sons, 2002.
連結：
[5] R.~H. Kingston., Parametric amplification and oscillation at optical frequencies, Proc. IR, 50:472, 1962.
連結：
[6] J.~A. Giordmaine and R.~C. Miller, Tunable coherent parametric oscillation in linbo3 at optical
連結：

Times Cited (115) 〈TOP〉

Altmetrics

〈TOP〉

E-mail ：

When an article is available to download, a notice will be sent to your mailbox address.

E-mail ：