Second-Harmonic-Generation Switching via Pressure-Suppressed Dynamical Disorder

被引：2

作者：

Jiang, Dequan ^{[1
]}

Jiang, Xingxing ^{[2
]}

Zhang, Xue ^{[3
]}

Li, Chen ^{[4
]}

Liu, Ke ^{[4
]}

Ma, Yingying ^{[4
]}

Cheng, Hao-Ming ^{[4
]}

Pei, Tianyao ^{[4
]}

Wen, Ting ^{[4
]}

Lin, Zheshuai ^{[2
]}

Li, Fangfei ^{[3
]}

Wang, Yonggang ^{[1
,4
]}

机构：

[1] Peking Univ, Sch Mat Sci & Engn, Beijing 100871, Peoples R China

[2] Chinese Acad Sci, Tech Inst Phys & Chem, Funct Crystals Lab, Beijing 100190, Peoples R China

[3] Jilin Univ, State Key Lab Superhard Mat, Changchun 130012, Peoples R China

[4] Ctr High Pressure Sci & Technol Adv Res HPSTAR, Beijing 100193, Peoples R China

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2024年 / 146卷 / 33期

基金：

中国博士后科学基金; 中国国家自然科学基金;

关键词：

PHASE-CHANGE MATERIALS; NONLINEAR-OPTICAL PROPERTIES; BRILLOUIN-SCATTERING; RAMAN-SPECTRUM; THIN-FILMS; NH4CL; GENERATION; TRANSITIONS; NH4BR; ION;

D O I：

10.1021/jacs.4c07504

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Second-harmonic-generation (SHG) switching is an emerging phenomenon with potential applications in bistable storage and optical switches while also serving as a sensitive probe for inversion-symmetry. Temperature-induced disorder-order phase transition has been proven to be a rational design strategy for achieving SHG bi-state switching; however, pressure-sensitive SHG switching via a disorder-order structural transition mechanism is rarely reported and lacks sensitivity and cyclicity as practical switching materials. Herein, we demonstrate the pressure-induced "dynamical disorder-order" phase transition as an effective strategy for triggering SHG and SHG switching in NH4Cl. The "dynamical disorder-order" phase transition of NH4Cl occurring at as low as 1 GPa is confirmed by comprehensive in situ high-pressure XRD, molecular vibrational spectra, and Brillouin scattering spectra. The pressure-induced SHG is responsive to a wide excitation wavelength region (800-1500 nm), and the "off-on" switching is reversible for up to 50 cycles, setting a record for pressure-driven switching materials. It is worth noting that when pressure is further increased to 14 GPa, NH4Cl exhibits another SHG "on-off" switching, which makes it the first triplet SHG "off-on-off" switching material. Molecular dynamics simulations reveal the key role of N-H<middle dot><middle dot><middle dot>Cl hydrogen bonding in the pressure-induced "dynamic disorder-order" mechanism. Finally, we verified that chemical pressure and physical pressure can jointly regulate the SHG switching behavior of NH4X (X = Cl, Br). The pressure-driven "dynamic disorder-order" transition mechanism sheds light on the rational design of multistable SHG switching materials for photoswitches and information storage.

引用

页码：23508 / 23516

页数：9