Search results for "Sum-frequency generation"
showing 10 items of 19 documents
Surface charges at the CaF2/water interface allow very fast intermolecular vibrational-energy transfer
2020
Abstract We investigate the dynamics of water in contact with solid calcium fluoride, where at low pH, localized charges can develop upon fluorite dissolution. We use 2D surface‐specific vibrational spectroscopy to quantify the heterogeneity of the interfacial water (D2O) molecules and provide information about the sub‐picosecond vibrational‐energy‐relaxation dynamics at the buried solid/liquid interface. We find that strongly H‐bonded OD groups, with a vibrational frequency below 2500 cm−1, display very rapid spectral diffusion and vibrational relaxation; for weakly H‐bonded OD groups, above 2500 cm−1, the dynamics slows down substantially. Atomistic simulations based on electronic‐structu…
Control of signal coherence in parametric frequency mixing with incoherent pumps: Narrowband mid-infrared light generation by downconversion of broad…
2012
International audience; We study, with numerical simulations using the generalized nonlinear envelope equation, the processes of optical parametric and difference- and sum-frequency generation (SFG) with incoherent pumps in optical media with both quadratic and third-order nonlinearity, such as periodically poled lithium niobate. With ultrabroadband amplified spontaneous emission pumps or continua (spectral widths > 10 THz), group-velocity matching of a near-IR pump and a short-wavelength mid-IR (MIR) idler in optical parametric generation may lead to more than 15-fold relative spectral narrowing of the generated MIR signal. Moreover, the SFG process may also lead to 6-fold signal coherence…
Vibrational Sum Frequency Generation Spectroscopy of the Water Liquid–Vapor Interface from Density Functional Theory-Based Molecular Dynamics Simulat…
2013
International audience; The vibrational sum frequency generation (VSFG) spectrum of the water liquid-vapor (LV) interface is calculated using density functional theory-based molecular dynamics simulations. The real and imaginary parts of the spectrum are in good agreement with the experimental data, and we provide an assignment of the SFG bands according to the dipole orientation of the interfacial water molecules. We use an instantaneous definition of the surface, which is more adapted to the study of interfacial phenomena than the Gibbs dividing surface. By calculating the vibrational (infrared, Raman) properties for interfaces of varying thickness, we show that the bulk spectra signature…
Surface-Specific Spectroscopy of Water at a Potentiostatically Controlled Supported Graphene Monolayer
2019
Knowledge of the structure of interfacial water molecules at electrified solid materials is the first step toward a better understanding of important processes at such surfaces, in, e.g., electrochemistry, atmospheric chemistry, and membrane biophysics. As graphene is an interesting material with multiple potential applications such as in transistors or sensors, we specifically investigate the graphene–water interface. We use sum-frequency generation spectroscopy to investigate the pH- and potential-dependence of the interfacial water structure in contact with a chemical vapor deposited (CVD) grown graphene surface. Our results show that the SFG signal from the interfacial water molecules a…
Optimized blue light generation in optically contacted walk-off compensated RbTiOAsO4 and KTiOP1−yAsyO4
1999
Abstract We study type II 1.32 μm second harmonic generation (SHG) in a RbTiOAsO 4 optically contacted walk-off compensated device. The reduction of the effective walk-off angle by a factor of 3.7 with respect to KTiOPO 4 for the same interaction leads to an enhancement by a factor of 10 of the conversion efficiency. A model is proposed for both type I and type II SHG in such a structure. The angular tuning curve is a multi-peaked one, as predicted by the model. The enhancement of the SHG conversion efficiency allows us to optimize the generation of blue laser light at 440 nm: a specially designed KTiOP 0.98 As 0.02 O 4 solid solution crystal achieves angular non-critical phase matching at …
The Fluorite/Water Interfaces: Structure and Spectroscopy from First Principles Simulations
2014
Despite its relevance to industrial, environmental and medical application, the fluorite/water interface still lacks a microscopic/atomistic characterization. In this contribution we provide the first atomistic description of such interface using first principles molecular dynamics simulations. Our models, which explore a wide range of pH, are able to provide a rational of the recent vibrational spectroscopy experiments. In particular we find that at neutral pH the water at the interface is disordered, in agreement with the experimental data, and explaining why no Vibrational Sum Frequency Generation (VSFG) signal is recorded. At high pH, OH groups which localize at the interface are respon…
Experimental and theoretical evidence for bilayer-by-bilayer surface melting of crystalline ice
2017
On the surface of water ice, a quasi-liquid layer (QLL) has been extensively reported at temperatures below its bulk melting point at 273 K. Approaching the bulk melting temperature from below, the thickness of the QLL is known to increase. To elucidate the precise temperature variation of the QLL, and its nature, we investigate the surface melting of hexagonal ice by combining noncontact, surface-specific vibrational sum frequency generation (SFG) spectroscopy and spectra calculated from molecular dynamics simulations. Using SFG, we probe the outermost water layers of distinct single crystalline ice faces at different temperatures. For the basal face, a stepwise, sudden weakening of the hy…
Counter-propagating difference-frequency generation in diamond with terahertz fields
2013
The nonlinear interaction of terahertz (THz) pulses with optical fields in Kerr, gaseous media is a key ingredient for broadband THz detection schemes [1]. Terahertz field-induced second harmonic generation in solid-state media has also been considered for THz detection and as a tool e.g. for liquid dynamics investigations [2,3], while four-wave mixing has been addressed as a possible mechanism for THz generation [4,5]. © 2013 IEEE.
Experimental observation of incoherent modulation instability in standard optical fibers
2005
In this work, we demonstrate theoretically and experimentally that a partially temporally incoherent light can exhibit modulational instability when propagating in an optical fiber with instantaneous nonlinear Kerr response.
Broadband Second-Harmonic Generation via Random Quasi-Phase-Matching in PPLT
2010
We demonstrated broadband second-harmonic generation via random Quasi-Phase-Matching in periodically poled Lithium Tantalate.