Details

Autor(en) / Beteiligte

• Ran, Mao‐Yin
• Zhou, Sheng‐Hua
• Wei, Wen‐Bo
• Li, Bing‐Xuan
• Wu, Xin‐Tao
• Lin, Hua
• Zhu, Qi‐Long

Titel

Breaking Through the Trade‐Off Between Wide Band Gap and Large SHG Coefficient in Mercury‐Based Chalcogenides for IR Nonlinear Optical Application

Ist Teil von

• Small (Weinheim an der Bergstrasse, Germany), 2024-02, Vol.20 (6), p.e2304563-n/a

Ort / Verlag

Germany: Wiley Subscription Services, Inc

Erscheinungsjahr

2024

Quelle

Wiley Online Library E-Journals

Beschreibungen/Notizen

• It is substantially challenging for non‐centrosymmetric (NCS) Hg‐based chalcogenides for infrared nonlinear optical (IR‐NLO) applications to realize wide band gap (Eg > 3.0 eV) and sufficient phase‐matching (PM) second‐harmonic‐generation intensity (deff > 1.0 × benchmark AgGaS2) simultaneously due to the inherent incompatibility. To address this issue, this work presents a diagonal synergetic substitution strategy for creating two new NCS quaternary Hg‐based chalcogenides, AEHgGeS4 (AE = Sr and Ba), based on the centrosymmetric (CS) AEIn2S4. The derived AEHgGeS4 displays excellent NLO properties such as a wide Eg (≈3.04–3.07 eV), large PM deff (≈2.2–3.0 × AgGaS2), ultra‐high laser‐induced damage threshold (≈14.8–15 × AgGaS2), and suitable Δn (≈0.19–0.24@2050 nm), making them highly promising candidates for IR‐NLO applications. Importantly, such excellent second‐order NLO properties are primarily attributed to the synergistic combination of tetrahedral [HgS4] and [GeS4] functional primitives, as supported by detailed theoretical calculations. This study reports the first two NCS Hg‐based materials with well‐balanced comprehensive properties (i.e., Eg > 3.0 eV and deff > 1.0 × benchmark AgGaS2) and puts forward a new design avenue for the construction of more efficient IR‐NLO candidates. Two novel non‐centrosymmetric chalcogenides, AEHgGeS4 (AE = Sr and Ba) are developed through the diagonal synergetic substitution strategy, which represents the first two examples breaking through incompatibility between large energy gap (Eg > 3.0 eV) and strong SHG response (deff > 1.0 × benchmark AgGaS2) in Hg‐based chalcogenides, owing to the synergistic effect of highly polarized [HgS4] and [GeS4] tetrahedra.