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学者姓名：崔洪花
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Abstract ：
Birefringent crystals play an irreplaceable role in optical systems by adjusting the polarization state of light in optical devices. This work successfully synthesized a new thiophosphate phase of B-Pb3 P2 S8 through the high-temperature solid-state spontaneous crystallization method. Different from the cubic a-Pb3 P2 S8 , the B-Pb3 P2 S8 crystallizes in the orthorhombic Pbcn space group. Notably, B-Pb3 P2 S8 shows a large band gap of 2.37 eV in lead-based chalcogenides, wide infrared transparent window (2.5-15 mu m), and excellent thermal stability. Importantly, the experimental birefringence shows the largest value of 0.26@550 nm in chalcogenides, even larger than the commercialized oxide materials. The Barder charge analysis result indicates that the exceptional birefringence effect is mainly from the Pb2 + and S2- in the [PbSn ] polyhedrons. Meanwhile, the parallelly arranged polyhedral layers could improve the structural anisotropic. Therefore, this work supports a new method for designing chalcogenides with exceptional birefringence effect in the infrared region. (c) 2024 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
Keyword ：
Birefringent crystals Birefringent crystals Chalcogenides Chalcogenides Optical properties Optical properties Structural ansotropic Structural ansotropic
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| GB/T 7714 | Guo, Weiping , Zhu, Ying , Cui, Hong-Hua et al. B-Pb 3 P 2 S 8: A new optical crystal with exceptional birefringence effect [J]. | CHINESE CHEMICAL LETTERS , 2025 , 36 (2) . |
| MLA | Guo, Weiping et al. "B-Pb 3 P 2 S 8: A new optical crystal with exceptional birefringence effect" . | CHINESE CHEMICAL LETTERS 36 . 2 (2025) . |
| APA | Guo, Weiping , Zhu, Ying , Cui, Hong-Hua , Li, Lingyun , Yu, Yan , Luo, Zhong-Zhen et al. B-Pb 3 P 2 S 8: A new optical crystal with exceptional birefringence effect . | CHINESE CHEMICAL LETTERS , 2025 , 36 (2) . |
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SnTe is an intriguing alternative to PbTe for midtemperature thermoelectric applications. Despite steady progress, its performance is lagging, in part because of the large energy difference(Delta EL-Sigma) between the light (L-band) and heavy (Sigma-band) valence bands and higher lattice thermal conductivity (kappa(L)). Previous studies have shown that applying pressure can enhance the Seebeck coefficient (S) and power factor (PF) of SnTe. Inspired by this study, we showcase how the high-pressure effect can be emulated under ambient pressure by substituting Sn with atoms possessing smaller atomic radii. Specifically, Sb- and Ge-doping combined with CdTe- or CdS-alloying induce lattice shrinkage, also referred to as "chemical pressure", raising the energy of the Sigma-band. Additionally, these substituted atoms lower the contribution of Sn 5s-Te 5p antibonding states to the L-band, thereby reducing its energy and dispersion. These combined effects decrease Delta EL-Sigma from 0.36 to 0.09 eV, leading to the enhanced S and average PFavg. Notably, the PFavg, ranging from 323 to 873 K, increases from 8.1 mu W cm(-1) K-2 for pristine SnTe to 21.6 mu W cm(-1) K-2 for Sn0.79Ge0.15Sb0.06Te-5% CdTe. Furthermore, the intensified phonon scattering resulting from discordant nature of Ge and Cd atoms, creating point defects soften phonon modes, and the presence of Ge-rich nanoprecipitates lead to a substantial 62% reduction in kappa(L) at 873 K. This strong valence band convergence and enhanced phonon scattering collectively contribute to a high peak ZT of 1.5 (873 K) and high average ZT(avg) = 0.81 over the temperature range of 323-873 K.
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| GB/T 7714 | Ming, Hongwei , Luo, Zhong-Zhen , Chen, Zixuan et al. Chemical Pressure-Driven Band Convergence and Discordant Atoms Intensify Phonon Scattering Leading to High Thermoelectric Performance in SnTe [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 , 146 (41) : 28448-28458 . |
| MLA | Ming, Hongwei et al. "Chemical Pressure-Driven Band Convergence and Discordant Atoms Intensify Phonon Scattering Leading to High Thermoelectric Performance in SnTe" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146 . 41 (2024) : 28448-28458 . |
| APA | Ming, Hongwei , Luo, Zhong-Zhen , Chen, Zixuan , Cui, Hong-Hua , Zheng, Wenwen , Zou, Zhigang et al. Chemical Pressure-Driven Band Convergence and Discordant Atoms Intensify Phonon Scattering Leading to High Thermoelectric Performance in SnTe . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 , 146 (41) , 28448-28458 . |
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The Pb4Sb12-xBi8+xSe34 (x = 0, 1, 2, 3, 4, and 5) crystals belong to pavonite homologues composed of thick NaCl- and thin GeS-type slabs which crystallize in the C2/m space group. Pb4Sb12-xBi8+xSe34 compounds exhibit n-type semiconductor transport behavior and demonstrate excellent thermodynamic stability. These intrinsic compounds have high carrier concentrations of similar to 2.18 x 10(19) to 4.47 x 10(20) cm(-3), leading to high electrical conductivities. The two-band electronic structure results in a high Seebeck coefficient. Taking Pb4Sb9Bi11Se34 as an example, it has a remarkable Seebeck coefficient of -149.1 mu V K-1 and high electrical conductivity of similar to 118 S cm(-1). It is comparable with other pavonite at 723 K. On the other hand, due to mixed occupancies of cation sites and complex crystal structure, the Pb4Sb9Bi11Se34 features ultralow lattice thermal conductivity of similar to 0.25 W m(-1) K-1 at 723 K. The high figure of merit, ZT, of 0.48 for Pb4Sb9Bi11Se34 is obtained at 723 K.
Keyword ：
crystal structure crystal structure pavonite pavonite Pb4Sb12-x Bi8+x Se34 Pb4Sb12-x Bi8+x Se34 thermoelectric thermoelectric ultralow thermalconductivity ultralow thermalconductivity
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| GB/T 7714 | Yang, Ruizhi , Li, Xia , Ming, Hongwei et al. Crystal Structure and Thermoelectric Properties of Pavonite Homologous Pb4Sb12-x Bi8+x Se34 [J]. | ACS APPLIED ENERGY MATERIALS , 2024 , 7 (11) : 4942-4949 . |
| MLA | Yang, Ruizhi et al. "Crystal Structure and Thermoelectric Properties of Pavonite Homologous Pb4Sb12-x Bi8+x Se34" . | ACS APPLIED ENERGY MATERIALS 7 . 11 (2024) : 4942-4949 . |
| APA | Yang, Ruizhi , Li, Xia , Ming, Hongwei , Guo, Weiping , Chen, Zixuan , Cui, Hong-Hua et al. Crystal Structure and Thermoelectric Properties of Pavonite Homologous Pb4Sb12-x Bi8+x Se34 . | ACS APPLIED ENERGY MATERIALS , 2024 , 7 (11) , 4942-4949 . |
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PbS is an attractive thermoelectric material with low cost, high thermostability, and large abundance in the Earth's crust. However, its largest energy difference between the light and heavy valence bands (Delta Ev) Delta E v ) leads to a huge challenge in achieving valence band convergence (VBC), resulting in the lowest power factor (PF) PF ) compared to PbSe and PbTe. This low PF impedes the output power density of thermoelectric devices. In this work, the Ag dopant can reduce Delta E v from 0.34 eV to 0.20 eV, achieving VBC in p-type PbS for the first time, significantly improving the Seebeck coefficient. Additionally, Pb 0.98 Ag 0.02 S exhibits semiconductor-like electrical conductivity caused by the grain boundaries scattering below 473 K. With coarse-graining, the mobility improves substantially from 4.6 cm2 2 V-1 s-1 to 241 cm2 2 V-1 s- 1 at room temperature. Consequently, the PF of Pb 0.98 Ag 0.02 S increases from 0.3 mu W cm-- 1 K-2 to 12.2 mu W cm-- 1 K-2 with the figure of merit ZT value rising from 0.0027 to 0.10 at 300 K. More importantly, Pb 0.98 Ag 0.02 S crystal maintains a high PF from 300 K to 823 K, giving a record-high average PF of 13.0 mu W cm-- 1 K-2 and an increased ZT . This work certifies Ag as an effective p-type dopant for weakening electron transport coupling for PbS-based thermoelectric materials.
Keyword ：
Coarse-graining Coarse-graining Power factor Power factor P-type PbS P-type PbS Thermoelectric Thermoelectric Valence band convergence Valence band convergence
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| GB/T 7714 | Wu, Ming , Cui, Hong-Hua , Chen, Zixuan et al. Realization of valence band convergence for high thermoelectric performance p-type PbS [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 494 . |
| MLA | Wu, Ming et al. "Realization of valence band convergence for high thermoelectric performance p-type PbS" . | CHEMICAL ENGINEERING JOURNAL 494 (2024) . |
| APA | Wu, Ming , Cui, Hong-Hua , Chen, Zixuan , Zhou, Jing , Ming, Hongwei , Luo, Zhong- Zhen et al. Realization of valence band convergence for high thermoelectric performance p-type PbS . | CHEMICAL ENGINEERING JOURNAL , 2024 , 494 . |
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Although orthorhombic GeSe is predicted to have an ultrahigh figure of merit, ZT approximate to 2.5, up to now, the highest experimental value is approximate to 0.2 due to the low carrier concentration (n(H) approximate to 10(18) cm(-3)). Improving symmetry is an effective approach for enhancing the ZT of GeSe-based materials. With Te-alloying, Ge4Se3Te displays the two-dimensional hexagonal structure and high n(H) approximate to 1.23 x 10(21) cm(-3). Interestingly, Ge4Se3Te transformed from the hexagonal into the rhombohedral phase with only approximate to 2% I-V-VI2-alloying (I = Li, Na, K, Cu, Ag; V = Sb, Bi; VI = Se, Te). According to the calculated results of Ge0.82Ag0.09Bi0.09Se0.614Te0.386 single-crystal grown via AgBiTe2-alloying, it exhibits a higher valley degeneracy than the hexagonal Ge4Se3Te. For instance, AgBiTe2-alloying induces a strong band convergence and band inversion effect, resulting in a significantly enhanced Seebeck coefficient and power factor with a similar n(H) from 17 mu V K-1 and 0.63 mu W cm(-1) K-2 for pristine Ge4Se3Te to 124 mu V K-1 and 5.97 mu W cm(-1) K-2 for 12%AgBiTe2-alloyed sample, respectively. Moreover, the sharply reduced phonon velocity, nano-domain wall structure, and strong anharmonicity lead to low lattice thermal conductivity. As a result, a record-high average ZT approximate to 0.95 over 323-773 K with an excellent ZT approximate to 1.30 is achieved at 723 K.
Keyword ：
Ge4Se3Te Ge4Se3Te multi-band convergence multi-band convergence nano-domain wall structure nano-domain wall structure symmetry manipulation symmetry manipulation thermoelectricity thermoelectricity
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| GB/T 7714 | Guo, Mingjie , Cui, Hong-Hua , Guo, Weiping et al. Achieving Superior Thermoelectric Performance in Ge4Se3Te via Symmetry Manipulation with I-V-VI2 Alloying [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (18) . |
| MLA | Guo, Mingjie et al. "Achieving Superior Thermoelectric Performance in Ge4Se3Te via Symmetry Manipulation with I-V-VI2 Alloying" . | ADVANCED FUNCTIONAL MATERIALS 34 . 18 (2024) . |
| APA | Guo, Mingjie , Cui, Hong-Hua , Guo, Weiping , Chen, Zixuan , Ming, Hongwei , Luo, Zhong-Zhen et al. Achieving Superior Thermoelectric Performance in Ge4Se3Te via Symmetry Manipulation with I-V-VI2 Alloying . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (18) . |
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Improving polarizability is an important strategy for designing high-performance mid-infrared (mid-IR) nonlinear optical (NLO) materials. The substitution of equivalent or aliovalent atoms can manipulate the polarizability by adjusting the symmetry of the polyhedron. Herein, the Li+ and Cd2+ are introduced into the Cu3PS4 as the equivalent and aliovalent dopants for the Cu site. As a result, Li+ can significantly improve the bandgap (E-g) of LixCu3-xPS4 from 2.38 to 2.88 eV, leading to a higher laser-induced damage threshold (LIDT) of 4.9 times than AgGaS2 (AGS) with a comparable second harmonic generation (SHG) response of AGS (26-45 mu m). Interestingly, Cd2+ can improve the SHG response and enlarge the E-g simultaneously. As a result, Cd0.4Cu2.2PS4 has a large SHG response of 10 x AGS at 2050 nm (26-45 mu m) and a LIDT of 2.6 x AGS. Theoretical calculations reveal that lattice vacancies induced by Cd2+ significantly boost polarizability compared to LixCu3-xPS4 with no vacancy, leading to a strong NLO response.
Keyword ：
aliovalent substitution aliovalent substitution lattice vacancies lattice vacancies Mid-IR NLO Mid-IR NLO polarizability polarizability SHG response SHG response
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| GB/T 7714 | Guo, Weiping , Fu, Yudi , Cui, Hong-Hua et al. Vacancy-Induced Extraordinary Second Harmonic Generation Response for Diamond-Like Cu3PS4 [J]. | ADVANCED OPTICAL MATERIALS , 2024 , 12 (18) . |
| MLA | Guo, Weiping et al. "Vacancy-Induced Extraordinary Second Harmonic Generation Response for Diamond-Like Cu3PS4" . | ADVANCED OPTICAL MATERIALS 12 . 18 (2024) . |
| APA | Guo, Weiping , Fu, Yudi , Cui, Hong-Hua , Li, Lingyun , Yu, Yan , Luo, Zhong-Zhen et al. Vacancy-Induced Extraordinary Second Harmonic Generation Response for Diamond-Like Cu3PS4 . | ADVANCED OPTICAL MATERIALS , 2024 , 12 (18) . |
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P-type lead chalcogenides have superior thermoelectric performance because they exhibit the energy convergence of several valence bands. However, despite the existence of two conduction bands, there has been no report about conduction band (CB) convergence for n-type counterparts because of the large energy difference between them. New strategies are required to manipulate the CBs if enhancing the electrical transport performance of n-type lead chalcogenides is to be achieved. PbS is a highly attractive member of the lead chalcogenides because of its high earth-abundance and low cost. Here, we report that the introduction of GaSb can successfully dope the PbS matrix with Ga and Sb atoms occupying the Pb site in its rock salt structure. GaSb doping leads to conduction band convergence and enlarged effective density of state mass for n-type PbS. This effect results in superior power factor and decreased lattice thermal conductivity caused by the soft phonon modes and point defect scattering of phonons. Consequently, a record-high average power factor PFavg of similar to 20.4 mu W cm(-1) K-2 and figure of merit ZT(avg) of similar to 0.84 in the temperature range of 400 K to 923 K were obtained, higher than any n- and p-type PbS-based thermoelectric materials.
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| GB/T 7714 | Chen, Zixuan , Cui, Hong-Hua , Hao, Shiqiang et al. GaSb doping facilitates conduction band convergence and improves thermoelectric performance in n-type PbS [J]. | ENERGY & ENVIRONMENTAL SCIENCE , 2023 , 16 (4) : 1676-1684 . |
| MLA | Chen, Zixuan et al. "GaSb doping facilitates conduction band convergence and improves thermoelectric performance in n-type PbS" . | ENERGY & ENVIRONMENTAL SCIENCE 16 . 4 (2023) : 1676-1684 . |
| APA | Chen, Zixuan , Cui, Hong-Hua , Hao, Shiqiang , Liu, Yukun , Liu, Hui , Zhou, Jing et al. GaSb doping facilitates conduction band convergence and improves thermoelectric performance in n-type PbS . | ENERGY & ENVIRONMENTAL SCIENCE , 2023 , 16 (4) , 1676-1684 . |
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This study investigates Ga-doped n-type PbTe thermoelectric materials and the dynamic phase conversion process of the second phases via Cu2Se alloying. Introducing Cu2Se enhances its electrical transport properties while reducing its lattice thermal conductivity (kappa(lat)) via weak electron-phonon coupling. Cu2Te and CuGa(Te/Se)(2) (tetragonal phase) nanocrystals precipitate during the alloying process, resulting in Te vacancies and interstitial Cu in the PbTe matrix. At room temperature, Te vacancies and interstitial Cu atoms serve as n-type dopants, increasing the carrier concentration and electrical conductivity from approximate to 1.18 x 10(19) cm(-3) and approximate to 1870 S cm(-1) to approximate to 2.26 x 10(19) cm(-3) and approximate to 3029 S cm(-1), respectively. With increasing temperature, the sample exhibits a dynamic change in Cu2Te content and the generation of a new phase of CuGa(Te/Se)(2) (cubic phase), strengthening the phonon scattering and obtaining an ultralow kappa(lat). Pb0.975Ga0.025Te-3%CuSe exhibits a maximum figure of merit of approximate to 1.63 at 823 K, making it promising for intermediate-temperature device applications.
Keyword ：
Cu Cu dynamic phase conversion dynamic phase conversion electron-phonon coupling electron-phonon coupling n-type PbTe n-type PbTe Se-2 alloying Se-2 alloying thermoelectrics thermoelectrics
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| GB/T 7714 | Wu, Ming , Cui, Hong-Hua , Cai, Songting et al. Weak Electron-Phonon Coupling and Enhanced Thermoelectric Performance in n-type PbTe-Cu2Se via Dynamic Phase Conversion [J]. | ADVANCED ENERGY MATERIALS , 2022 . |
| MLA | Wu, Ming et al. "Weak Electron-Phonon Coupling and Enhanced Thermoelectric Performance in n-type PbTe-Cu2Se via Dynamic Phase Conversion" . | ADVANCED ENERGY MATERIALS (2022) . |
| APA | Wu, Ming , Cui, Hong-Hua , Cai, Songting , Hao, Shiqiang , Liu, Yukun , Bailey, Trevor P. et al. Weak Electron-Phonon Coupling and Enhanced Thermoelectric Performance in n-type PbTe-Cu2Se via Dynamic Phase Conversion . | ADVANCED ENERGY MATERIALS , 2022 . |
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