Correlating structural dynamics and catalytic activity of AgAu nanoparticles with ultrafast spectroscopy and all-atom molecular dynamics simulations

Ferbonink, Guilherme Ferreira; Rodrigues, Thenner Silva; Santos, Diego P. dos; Camargo, Pedro H. C.; Albuquerque, Rodrigo Q.; Nome, René A.

doi:10.1039/c7fd00220c

Cited by 9 publications

(16 citation statements)

References 33 publications

(52 reference statements)

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“…Figure 1(left) shows the experimental UV-Vis extinction spectrum of the AgAu nanoshell samples used in this work, which exhibit localized dipolar surface plasmon resonance centered around 800 nm. This SPR wavelength extends well beyond the SPR wavelength of pure Ag (410 nm) and Au nanospheres (520 nm) or solid AgAu bimetallic nanoparticles (SPR wavelength intermediate between 410 and 520 nm,depending on composition), due to a complex interplay of structural, compositional and electronic factors that affect their optical properties[30,35]. Figure1(right) shows electron microscopy images of the AgAu nanoshells investigated in the present work.…”

mentioning

confidence: 63%

Stochastic Thermodynamics Analysis of Ultrafast AgAu Nanoshell Dynamics in the Nonlinear Response Regime

Ferbonink¹,

Rodrigues²,

Camargo³

et al. 2020

Preprint

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The understanding of relaxation dynamics of metallic nanoshells is important for a range of nanotechnological applications. In this work, we present a combined experimental-theoretical study of the relaxation dynamics of AgAu nanoshells. This was investigated using ultrafast pump-probe experiments resonant with the surface plasmon of the nanoshells, as well as via atomistic molecular dynamics simulations of relaxation and temperature-jump (DT-jump) processes. Both techniques were then discussed and complemented using a non-equilibrium statistical mechanical model. Data collected at low energies were consistent with our previously reported work and allowed the characterization of intrinsic electron-phonon coupling times (EPCT) and of the overall relaxation dynamics in terms of a two-temperature model. Data at intermediate and higher energies, in turn, showed a nonlinear dependence of EPCT as a function of the pump power, faster relaxation being observed at higher pump energies. In the limit of small DT-jumps, relaxation based on a two-temperature model is recovered, whereas in the limit of large DT-jumps, the relaxation becomes faster with increasing temperature change. The results reported here give insight on the ultrafast dynamics of AgAu nanoshells and might also be applied to other metallic systems, paving the way to the better understanding of relaxation dynamics of nanoparticles in general.

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confidence: 63%

Stochastic Thermodynamics Analysis of Ultrafast AgAu Nanoshell Dynamics in the Nonlinear Response Regime

Ferbonink¹,

Rodrigues²,

Camargo³

et al. 2020

Preprint

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“…Figure 5 shows the SEC positioned in front of two femtosecond lasers in a homemade setup for measurements involving ultrafast spectroscopy [29,30] . The cell is the same used for Raman, but it is positioned like in the XAFS experiment, i. e., parallel to the bench.…”

Section: Resultsmentioning

confidence: 99%

“…[1,[25][26][27] In Situ Ultrafast Spectroscopy Figure 5 shows the SEC positioned in front of two femtosecond lasers in a homemade setup for measurements involving ultrafast spectroscopy. [29,30] The cell is the same used for Raman, but it is positioned like in the XAFS experiment, i. e., parallel to the bench. As in the case of Raman, the measurements do not need to be performed in the thin layer configuration.…”

Section: In Situ Xas and Xrdmentioning

confidence: 99%

Versatile Spectroelectrochemical Cell for In Situ Experiments: Development, Applications, and Electrochemical Behavior**

et al. 2020

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[a, b] (Photo)electrochemical processes are involved in many fields of science and technology. The use of spectroscopic techniques coupled to (photo)electrochemistry, are mandatory to get information about interfacial processes on scale ranges from millimeters to the nanoscale. The development of spectroelectrochemical cells (SECs) contributes to the progress of the field of (photo)electrochemistry and their impact in science and technology. Therefore, in this work, we describe in detail the development of a versatile SEC that can be used for conventional electrochemical experiments and several in situ techniques just by changing its window. We performed electrochemical and computational experiments to analyze the response of our SEC as a function of the working electrode size, position, and distance to the window. Besides, we show in detail how the cell can be used to perform experiments of in situ FTIR, Raman, XAFS and ultrafast spectroscopy.

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“…We employ a nine-level system to describe Nd III , two-level system for Yb III and seven-level system for Er III . The Nd III system includes absorption to 4 F5/2, relaxation to 4 F3/2 and energy transfer to Yb III in addition to relaxation channels to lower energies and a dense manifold of higher lying electronic states [33][34][35][36]. The Yb III system describes transitions between states 2 F7/2 and 2 F5/2.…”

Section: Resultsmentioning

confidence: 99%

“…For each sample, two such sets of measurements were performed, with the laser either in pulsed femtosecond or in continuous wave (CW) operating modes. Ultrafast pump-probe spectroscopy measurements were performed as described previously [33]. Simulations: Light-matter interaction in the CW and femtosecond excitation modes were modeled with a semi-classical approach treating light classically and matter with discrete energy diagram.…”

Section: Methodsmentioning

confidence: 99%

Femtosecond Laser Induced Luminescence in Hierarchically Structured Nd3+,Yb3+,Er3+ Co-Doped Upconversion Nanoparticles: Light-Matter Interaction Mechanisms from Experiments and Simulations

Oliveira¹,

Ferreira²,

Ferbonink³

et al. 2020

Preprint

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Fundamental studies of light-matter interactions are important for basic knowledge and in applications. Thanks to advances in experimental and theoretical methods, nowadays it is possible to perform such studies in a broad dynamic range, covering timescales from that of elementary interactions to real time. In the present work, we perform an experimental-theoretical study of light intensity-dependent femtosecond and CW-laser induced frequency upconversion in hierarchically structured core-multishell nanoparticles co-doped with NdIII, YbIII, and ErIII. Upconversion spectra recorded with CW and femtosecond excitation are qualitatively similar whereas the intensity dependence of upconversion depends on excitation mode (CW or femtosecond). To further assess the observed intensity dependence, we perform light-matter interaction simulations in the dynamic range from 100 fs to 3 ms for 18-level system describing the UCNPs, including 9 NdIII levels, 2 YbIII, and 7 ErIII levels and a classical model for the excitation source. The calculated time- and intensity-dependent energy level population are compared with measured spectra to understand CW vs femtosecond laser-induced upconversion. To further discuss the differences between CW and femtosecond laser-induced light-matter interactions for the systems studied here, we perform semi-classical pulse propagation simulations and ultrafast pump-probe measurements to study how the light source bandwidth, relative to the absorption linewidth, influence light absorption and transmission and further connect these results with the intensity dependence. Overall, we report our progress toward mechanistic studies of light-matter interaction and photophysical pathways following femtosecond excitation and UCNPs.

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Correlating structural dynamics and catalytic activity of AgAu nanoparticles with ultrafast spectroscopy and all-atom molecular dynamics simulations

Cited by 9 publications

References 33 publications

Stochastic Thermodynamics Analysis of Ultrafast AgAu Nanoshell Dynamics in the Nonlinear Response Regime

Stochastic Thermodynamics Analysis of Ultrafast AgAu Nanoshell Dynamics in the Nonlinear Response Regime

Versatile Spectroelectrochemical Cell for In Situ Experiments: Development, Applications, and Electrochemical Behavior**

Femtosecond Laser Induced Luminescence in Hierarchically Structured Nd3+,Yb3+,Er3+ Co-Doped Upconversion Nanoparticles: Light-Matter Interaction Mechanisms from Experiments and Simulations

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