{"title":"Insights into nonlinear absorption transitions in a silver-incorporated reduced graphene oxide–molybdenum disulfide (Ag–rGO–MoS2) hybrid†","authors":"M. Abith and T. C. Sabari Girisun","doi":"10.1039/D4CP03039G","DOIUrl":null,"url":null,"abstract":"<p >Optical nonlinearity in a silver-decorated reduced graphene oxide–molybdenum disulfide (Ag–rGO–MoS<small><sub>2</sub></small>) nanocomposite was experimentally investigated <em>via</em> the <em>Z</em>-scan technique using a Q-switched Nd:YAG nanopulsed green laser. An interesting switching behaviour from saturable to reverse saturable absorption with varying input on-axis intensity of the laser was demonstrated. Under low-intensity laser excitation, Ag–rGO–MoS<small><sub>2</sub></small> displayed ground-state bleaching, which resulted in saturable absorption (SA) behaviour. Here, the prominent SPR phenomenon of Ag enforced plasmon absorption and is assigned to the SA process. Interestingly at higher intensity, the material switched its nonlinearity to reverse saturable absorption (RSA), attributed to two different mechanisms of two-photon absorption (2PA). At moderate laser pulse energies, the sample underwent sequential 2PA, which is underpinned by calculated varying nonlinear optical parameters and excited-state absorption cross-sections. However, at higher intensities, nonlinear absorption coefficients and excited-state absorption cross-sections remained constant, indicating the occurrence of genuine 2PA. In addition, theoretical estimation of the 2PA cross-section validates the observed transition. Thus, experimental evidence for the validity of nonlinear absorption theory (intensity-dependent transition from linear to nonlinear SA to nonlinear RSA to genuine 2PA <em>via</em> sequential 2PA) is provided for the first time in the literature.</p>","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":" 38","pages":" 25169-25180"},"PeriodicalIF":2.9000,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Physical Chemistry Chemical Physics","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/cp/d4cp03039g","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Optical nonlinearity in a silver-decorated reduced graphene oxide–molybdenum disulfide (Ag–rGO–MoS2) nanocomposite was experimentally investigated via the Z-scan technique using a Q-switched Nd:YAG nanopulsed green laser. An interesting switching behaviour from saturable to reverse saturable absorption with varying input on-axis intensity of the laser was demonstrated. Under low-intensity laser excitation, Ag–rGO–MoS2 displayed ground-state bleaching, which resulted in saturable absorption (SA) behaviour. Here, the prominent SPR phenomenon of Ag enforced plasmon absorption and is assigned to the SA process. Interestingly at higher intensity, the material switched its nonlinearity to reverse saturable absorption (RSA), attributed to two different mechanisms of two-photon absorption (2PA). At moderate laser pulse energies, the sample underwent sequential 2PA, which is underpinned by calculated varying nonlinear optical parameters and excited-state absorption cross-sections. However, at higher intensities, nonlinear absorption coefficients and excited-state absorption cross-sections remained constant, indicating the occurrence of genuine 2PA. In addition, theoretical estimation of the 2PA cross-section validates the observed transition. Thus, experimental evidence for the validity of nonlinear absorption theory (intensity-dependent transition from linear to nonlinear SA to nonlinear RSA to genuine 2PA via sequential 2PA) is provided for the first time in the literature.
期刊介绍:
Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions.
The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.