Tom S. Seifert, Hannes Hempel, Oliver Gueckstock, Robert Schneider, Quentin Remy, Angela N. Fioretti, Thomas Unold, Steffen Michaelis de Vasconcellos, Rudolf Bratschitsch, Rainer Eichberger, Kathrin Dörr, Andriy Zakutayev, Tobias Kampfrath
Terahertz (THz) radiation is a powerful probe of low-energy excitations in all phases of matter. However, it remains a challenge to find materials that efficiently generate THz radiation in a broad range of frequencies following optical excitation. Here, we investigate a pyroelectric material, ZnSnN2, and find that its above-band-gap excitation results in the efficient formation of an ultrafast photocurrent generating THz radiation. The resulting THz electric field spans a frequency range from below 1 THz to above 30 THz. The results suggest that the photocurrent is primarily driven by an ultrafast pyroelectric effect where the photo-excited carriers screen the spontaneous electric polarization of ZnSnN2. Strong structural disorder reduces the photocarrier lifetime significantly and, thus, enables broadband operation. ZnSnN2 shows a similar THz-emitter performance as the best spintronic THz emitters regarding bandwidth and amplitude. The study unveils the large potential of pyroelectric materials as efficient and broadband THz emitters with built-in bias fields.
{"title":"Efficient Broadband Terahertz Generation by Above-Band-Gap Excitation of the Pyroelectric ZnSnN2","authors":"Tom S. Seifert, Hannes Hempel, Oliver Gueckstock, Robert Schneider, Quentin Remy, Angela N. Fioretti, Thomas Unold, Steffen Michaelis de Vasconcellos, Rudolf Bratschitsch, Rainer Eichberger, Kathrin Dörr, Andriy Zakutayev, Tobias Kampfrath","doi":"10.1002/adom.202501905","DOIUrl":"https://doi.org/10.1002/adom.202501905","url":null,"abstract":"<p>Terahertz (THz) radiation is a powerful probe of low-energy excitations in all phases of matter. However, it remains a challenge to find materials that efficiently generate THz radiation in a broad range of frequencies following optical excitation. Here, we investigate a pyroelectric material, ZnSnN<sub>2</sub>, and find that its above-band-gap excitation results in the efficient formation of an ultrafast photocurrent generating THz radiation. The resulting THz electric field spans a frequency range from below 1 THz to above 30 THz. The results suggest that the photocurrent is primarily driven by an ultrafast pyroelectric effect where the photo-excited carriers screen the spontaneous electric polarization of ZnSnN<sub>2</sub>. Strong structural disorder reduces the photocarrier lifetime significantly and, thus, enables broadband operation. ZnSnN<sub>2</sub> shows a similar THz-emitter performance as the best spintronic THz emitters regarding bandwidth and amplitude. The study unveils the large potential of pyroelectric materials as efficient and broadband THz emitters with built-in bias fields.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"14 1","pages":""},"PeriodicalIF":7.2,"publicationDate":"2025-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://advanced.onlinelibrary.wiley.com/doi/epdf/10.1002/adom.202501905","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145958129","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lead halide perovskites are promising next-generation optoelectronic materials due to their solution processability, tunable bandgap and excellent photoelectric properties. However, achieving deep-blue emission in all-inorganic CsPbX3 nanocrystals remains challenging due to phase separation, halide volatilization and insufficient stability, limiting industrial application. Herein, a collaborative strategy of “chlorine source regulation—defect passivation—fiber integration” is proposed. By incorporating β-cyclodextrin chloride (βCD-Cl) into CsPbBr3, we synthesized large-scale deep-blue CsPbBr3-xClx@βCD-Cl microcrystals via a mechanosynthesis route. Flexible blue-light fiber films are fabricated via electrospinning, showing a photoluminescence quantum yield (PLQY) of 55.79% and excellent environmental stability, with only a 16 nm red shift observed after 171 days in water. Additionally, the fiber films enable near-infrared (750 nm)-to-blue photon upconversion (450-490 nm), achieving unprecedented bilirubin degradation efficiency (40% within 20 min). They can serve as core components for next-generation phototherapeutic blankets, combining spectral selectivity (blocking harmful radiation < 420 nm) with therapeutic light transmission, eliminating neonatal retinal phototoxicity risks without requiring protective eyewear. The full solution-processed white-light fiber film is prepared, with CIE coordinates (x = 0.32, y = 0.34) near the ideal white light point. Overall, this study clarifies the molecular structure—performance relationships, overcomes stability bottlenecks, and supports photodynamic therapy and bio-photonic devices.
{"title":"Synergistic Chlorine Source Regulation and Defect-Passivation Strategy for Stable Blue-Emitting Perovskite Films Toward Non-Invasive Jaundice Therapy","authors":"Meifang Yang, Yicheng Yuan, Fangnan Shen, Wen-Guang Li, Yuansheng Jiang, Aili Wang, Lvzhou Li, Gengling Liu, Yu-Xin Chen, Qin Xu, Huan Pang, Tian Tian","doi":"10.1002/adom.202502560","DOIUrl":"https://doi.org/10.1002/adom.202502560","url":null,"abstract":"<p>Lead halide perovskites are promising next-generation optoelectronic materials due to their solution processability, tunable bandgap and excellent photoelectric properties. However, achieving deep-blue emission in all-inorganic CsPbX<sub>3</sub> nanocrystals remains challenging due to phase separation, halide volatilization and insufficient stability, limiting industrial application. Herein, a collaborative strategy of “chlorine source regulation—defect passivation—fiber integration” is proposed. By incorporating β-cyclodextrin chloride (βCD-Cl) into CsPbBr<sub>3</sub>, we synthesized large-scale deep-blue CsPbBr<sub>3-x</sub>Cl<sub>x</sub>@βCD-Cl microcrystals via a mechanosynthesis route. Flexible blue-light fiber films are fabricated via electrospinning, showing a photoluminescence quantum yield (PLQY) of 55.79% and excellent environmental stability, with only a 16 nm red shift observed after 171 days in water. Additionally, the fiber films enable near-infrared (750 nm)-to-blue photon upconversion (450-490 nm), achieving unprecedented bilirubin degradation efficiency (40% within 20 min). They can serve as core components for next-generation phototherapeutic blankets, combining spectral selectivity (blocking harmful radiation < 420 nm) with therapeutic light transmission, eliminating neonatal retinal phototoxicity risks without requiring protective eyewear. The full solution-processed white-light fiber film is prepared, with CIE coordinates (x = 0.32, y = 0.34) near the ideal white light point. Overall, this study clarifies the molecular structure—performance relationships, overcomes stability bottlenecks, and supports photodynamic therapy and bio-photonic devices.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"14 2","pages":""},"PeriodicalIF":7.2,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145970095","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Snorre Braathen Kjeldby, Dina Marie Nielsen, Simon Phillip Cooil, Ymir Kalmann Frodason, Eirini Zacharacki, In-Hwan Lee, Andrej Kuznetsov, Lasse Vines, Kristin Bergum, Vegard Standern Olsen
The earth-abundant II-IV-nitrides ZnSnN2 and ZnGeN2 are direct bandgap semiconductors with a wurtzite-derived crystal structure. Their alloys, ZnSnxGe1 − xN2, have bandgaps tunable across the full visible spectrum, making them interesting for many optoelectronic applications. Here, electrical, structural, and optical properties of near-stoichiometric ZnSnxGe1 − xN2 alloys, i.e., where [Zn]/([Zn]+[Ge]+[Sn]) ≈ 0.5, are reported, for samples synthesized by reactive magnetron sputtering. These results reveal unprecedentedly high electrical mobilities in Ge-rich alloys, with values of 136 and 400 cm2/Vs at room-temperature and ≈100 K, respectively. The bandgaps are determined from optical absorption measurements combined with hybrid density functional calculations and reveal a significant Burstein–Moss shift in the Sn rich alloys. Finally, band alignments are determined in the sputter-grown thin films by combining optical transmission measurements, hybrid density functional calculations, and UV photoelectron spectroscopy measurements, where the bandgap variation is predominantly caused by a shift of the conduction band edge. This work elucidates in unprecedented detail the tuning of optical and electrical properties in ZnSnxGe1 − xN2 by variation of the chemical composition, where bandgap values of alloys with x ∈ [0.5−0.7] are suitable for top cell absorbers in two-terminal tandem solar cells assuming a Si bottom cell.
{"title":"Tuning Properties of II-IV-Nitrides for Optoelectronic Applications","authors":"Snorre Braathen Kjeldby, Dina Marie Nielsen, Simon Phillip Cooil, Ymir Kalmann Frodason, Eirini Zacharacki, In-Hwan Lee, Andrej Kuznetsov, Lasse Vines, Kristin Bergum, Vegard Standern Olsen","doi":"10.1002/adom.202502634","DOIUrl":"https://doi.org/10.1002/adom.202502634","url":null,"abstract":"<p>The earth-abundant II-IV-nitrides ZnSnN<sub>2</sub> and ZnGeN<sub>2</sub> are direct bandgap semiconductors with a wurtzite-derived crystal structure. Their alloys, ZnSn<sub><i>x</i></sub>Ge<sub>1 − <i>x</i></sub>N<sub>2</sub>, have bandgaps tunable across the full visible spectrum, making them interesting for many optoelectronic applications. Here, electrical, structural, and optical properties of near-stoichiometric ZnSn<sub><i>x</i></sub>Ge<sub>1 − <i>x</i></sub>N<sub>2</sub> alloys, i.e., where [Zn]/([Zn]+[Ge]+[Sn]) ≈ 0.5, are reported, for samples synthesized by reactive magnetron sputtering. These results reveal unprecedentedly high electrical mobilities in Ge-rich alloys, with values of 136 and 400 cm<sup>2</sup>/Vs at room-temperature and ≈100 K, respectively. The bandgaps are determined from optical absorption measurements combined with hybrid density functional calculations and reveal a significant Burstein–Moss shift in the Sn rich alloys. Finally, band alignments are determined in the sputter-grown thin films by combining optical transmission measurements, hybrid density functional calculations, and UV photoelectron spectroscopy measurements, where the bandgap variation is predominantly caused by a shift of the conduction band edge. This work elucidates in unprecedented detail the tuning of optical and electrical properties in ZnSn<sub><i>x</i></sub>Ge<sub>1 − <i>x</i></sub>N<sub>2</sub> by variation of the chemical composition, where bandgap values of alloys with <i>x</i> ∈ [0.5−0.7] are suitable for top cell absorbers in two-terminal tandem solar cells assuming a Si bottom cell.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"13 36","pages":""},"PeriodicalIF":7.2,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145792512","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In the Research Article (DOI: 10.1002/adom.202502484), Jianya Zhang, Yonglin Huang, Yukun Zhao, and co-workers report a controllable method to integrate single nanowire into synaptic nano-device with ultralow power consumption. It can mimic multiple functions of biological synapses for learning, corresponding to those in cover image. Due to the advantages of simplicity and cost-efficiency, this method has a promising prospect.