Two phases of Ga2S3: promising infrared second-order nonlinear optical materials with very high laser induced damage thresholds

Zhang, Ming‐Jian; Jiang, Xiao‐Ming; Zhou, Liujiang; Guo, Guo‐Cong

doi:10.1039/c3tc30808a

Cited by 256 publications

(242 citation statements)

References 36 publications

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“…For the monoclinic Ga 2 S 3 , the highest valence band is consisted of mainly S 3 p and some Ga 4 p orbitals29. Unlike the other s orbital has highly spherical symmetry, the p states in the valence band of Ga 2 S 3 are strongly oriented dump-bell shape (axial dependent) distribution, which may enhance the anisotropic character present in the optical property of the diindium trisulfide.…”

Section: Discussionmentioning

confidence: 99%

Optically decomposed near-band-edge structure and excitonic transitions in Ga2S3

Chen

2014

Sci Rep

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The band-edge structure and band gap are key parameters for a functional chalcogenide semiconductor to its applications in optoelectronics, nanoelectronics, and photonics devices. Here, we firstly demonstrate the complete study of experimental band-edge structure and excitonic transitions of monoclinic digallium trisulfide (Ga2S3) using photoluminescence (PL), thermoreflectance (TR), and optical absorption measurements at low and room temperatures. According to the experimental results of optical measurements, three band-edge transitions of EA = 3.052 eV, EB = 3.240 eV, and EC = 3.328 eV are respectively determined and they are proven to construct the main band-edge structure of Ga2S3. Distinctly optical-anisotropic behaviors by orientation- and polarization-dependent TR measurements are, respectively, relevant to distinguish the origins of the EA, EB, and EC transitions. The results indicated that the three band-edge transitions are coming from different origins. Low-temperature PL results show defect emissions, bound-exciton and free-exciton luminescences in the radiation spectra of Ga2S3. The below-band-edge transitions are respectively characterized. On the basis of experimental analyses, the optical property of near-band-edge structure and excitonic transitions in the monoclinic Ga2S3 crystal is revealed.

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Section: Discussionmentioning

confidence: 99%

Optically decomposed near-band-edge structure and excitonic transitions in Ga2S3

Chen

2014

Sci Rep

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“…A crystallographic non‐centrosymmetric (NCS) structure is the prerequisite condition of an NLO material. Over the past decades, numerous strategies have been introduced to design new NCS materials, and many MFIR NLO compounds with strong powder SHG responses have been discovered and prepared . Among them, construction of diamond‐like frameworks (DLFs) has been considered as one of the most effective methods to obtain new MFIR NLO materials with excellent properties; typical examples include BaGa 4 Q 7 (Q=S, Se), Ba 3 AGa 5 Se 10 Cl 2 (A=K‐Cs), PbGa 4 S 7 , Li 2 CdGeS 4 , and BaGa 2 MQ 6 (M=Si, Ge, Sn; Q=S, Se) …”

Section: Introductionmentioning

confidence: 99%

Non‐centrosymmetric Selenides AZn₄In₅Se₁₂ (A=Rb, Cs): Synthesis, Characterization and Nonlinear Optical Properties

Lin

Zheng

et al. 2016

Chemistry An Asian Journal

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Two new non-centrosymmetric polar quaternary selenides, namely, RbZn In Se and CsZn In Se , have been synthesized and structurally characterized. They exhibit a 3D diamond-like framework (DLF) consisting of corner-shared MSe (M=Zn/In) tetrahedra, in which the A ions are located. Both compounds are thermally stable up to 1300 K and exhibit large transmittance in the infrared region (0.65-25 μm) with measured optical band gaps of 2.06 eV for RbZn In Se and 2.11 eV for CsZn In Se . Inspiringly, they exhibit a good balance between strong second harmonic generation (SHG) efficiency (3.9 and 3.5×AgGaS ) and high laser-induced damage thresholds (13.0×AgGaS ). Theoretical calculations based on density functional theory (DFT) methods confirm that such strong SHG responses originate from the 3D DLF structure.

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“…Remarkably, in comparison with bandgaps and χ (2) of those typical phasing‐matchable ternary IR NLO selenides (Table S2, Supporting Information), title compounds also possess promising performances. Meanwhile, the powder LIDTs of 1 and 2 and the reference AGS measured by the single pulse powder LIDT method are shown in Figure b and Table S3 in the Supporting Information. The estimated LIDTs for 1 and 2 are 7.5 and 5.6 MW·cm −2 , which are 5.0 and 3.7 times larger than those of AGS (1.5 MW·cm −2 ), respectively, thereby indicating that compounds 1 and 2 may be good candidates for high power IR‐NLO applications.…”

Section: Resultsmentioning

confidence: 99%

Strong SHG Response via High Orientation of Tetrahedral Functional Motifs in Polyselenide A₂Ge₄Se₁₀ (A = Rb, Cs)

Liu

Zeng

et al. 2018

Advanced Optical Materials

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and strong nonlinearity. However, these materials suffer from intrinsic drawbacks, such as low laser damage threshold and two-photon absorptions, which seriously limit their high-power applications. Therefore, new promising IR-NLO materials need to be discovered.Motivated by Chen's anionic group theory, [6] which states that NLO efficiency mainly originates from anionic groups, many NLO-active structure building units (NLO functional motifs) [7] have been developed over the past few decades, such as those with d 0 transition-metal centers (e.g., Ti 4+ , Zr 4+ , Nb 5+ , Ta 5+ , Mo 6+ , etc.) [8] or maingroup cations with stereoactive lone pairs (e.g., Pb 2+ , Sb 3+ , Te 4+ , I 5+ , etc.), [9] and distorted tetrahedral MQ 4 (M = Zn, Ga, Ge, In, Sn, etc.; Q = S, Se). [10] The flexible assembly of these units produces some IR-NLO materials, such as 3These discoveries highlight the guiding role of NLO functional motifs in the development of new IR-NLO materials.SHG may originate from static and induced dipole moments. Some well-known IR-NLO functional motifs, including the distorted tetrahedral MQ 4 that usually exists in many IR-NLO metal chalcogenides, [10] possess a static dipole moment. However, their overall contributions to the total SHG responses of some compounds are negligible because the tetrahedral units are not properly aligned, thereby canceling out to a large extent the static contributions along different directions and leaving only the laser-induced contributions. For instance, in AgGaS 2 , AgGaSe 2 , and ZnGeP 2 , the static SHG contributions from GaS 4 , GaSe 4, and GeP 4 tetrahedra are exactly zero because of their nonpolar symmetry. Therefore, to maximize the static NLO contributions to the SHG response, structures with NLO-active units which are aligned in an almost parallel manner must be designed.The induced contribution of an NLO material to the SHG response is dominated by charge transfers which are close to the Fermi level. The terminal chalcogen atoms and those atoms which form QQ bonds in metal chalcogenides usually have a much larger contribution than the bridged chalcogen atoms which are connected to two neighboring metal Nonlinear optical (NLO) materials with strong second harmonic generation (SHG) responses are technologically and scientifically important for tunable lasers. This work puts forward a new strategy for designing promising infrared nonlinear optical (IR-NLO) materials with strong SHG responses by strengthening both the static and induced contributions via the high orientation of NLO functional motifs. Two new polyselenides Rb 2 Ge 4 Se 10 and Cs 2 Ge 4 Se 10 are studied to verify the strategy, they have 2D infinite 2 ∞ ∞ [Ge 4 Se 10 ] 2− layers comprising highly oriented distorted GeSe 4 tetrahedra. Their large SHG signals (8.0 and 8.5 times that of commercial AgGaS 2 ) can be ascribed to both the static contribution enhancement from the high orientation of the local dipole moment of GeSe 4 tetrahedra and the induced contribution enhancement from terminal and SeSe bon...

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Two phases of Ga2S3: promising infrared second-order nonlinear optical materials with very high laser induced damage thresholds

Cited by 256 publications

References 36 publications

Optically decomposed near-band-edge structure and excitonic transitions in Ga2S3

Optically decomposed near-band-edge structure and excitonic transitions in Ga2S3

Non‐centrosymmetric Selenides AZn₄In₅Se₁₂ (A=Rb, Cs): Synthesis, Characterization and Nonlinear Optical Properties

Strong SHG Response via High Orientation of Tetrahedral Functional Motifs in Polyselenide A₂Ge₄Se₁₀ (A = Rb, Cs)

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Two phases of Ga2S3: promising infrared second-order nonlinear optical materials with very high laser induced damage thresholds

Cited by 256 publications

References 36 publications

Optically decomposed near-band-edge structure and excitonic transitions in Ga2S3

Optically decomposed near-band-edge structure and excitonic transitions in Ga2S3

Non‐centrosymmetric Selenides AZn4In5Se12 (A=Rb, Cs): Synthesis, Characterization and Nonlinear Optical Properties

Strong SHG Response via High Orientation of Tetrahedral Functional Motifs in Polyselenide A2Ge4Se10 (A = Rb, Cs)

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Non‐centrosymmetric Selenides AZn₄In₅Se₁₂ (A=Rb, Cs): Synthesis, Characterization and Nonlinear Optical Properties

Strong SHG Response via High Orientation of Tetrahedral Functional Motifs in Polyselenide A₂Ge₄Se₁₀ (A = Rb, Cs)