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Vibrational sum frequency generation (SFG) spectroscopy is a powerful technique for investigating molecular structures, orientations, and dynamics at surfaces. However, its spatial resolution is fundamentally restricted to the micrometer…

Sum-frequency generation (SFG) is a powerful second-order nonlinear spectroscopic technique that provides detailed insights into molecular structures and absolute orientations at surfaces and interfaces. However, conventional SFG based on…

Sum-frequency generation (SFG) is a second-order nonlinear process widely used for characterizing surfaces and interfaces with monolayer sensitivity. Recently, optical field enhancement in plasmonic nanocavities has enabled SFG with…

Understanding the molecular-level structure and dynamics of ice surfaces is crucial for deciphering several chemical, physical, and atmospheric processes. Vibrational sum-frequency generation (SFG) spectroscopy is the most prominent tool…

The plasmonic amplification of non-linear vibrational sum frequency spectroscopy (SFG) at the surfaces of gold nanoparticles is systematically investigated by tuning the incident visible wavelength. The SFG spectra of dodecanethiol-coated…

Moving the detection wavelength in vibrational sum-frequency generation (VSFG) spectroscopy to the near-infrared (> 700 nm) can potentially enable the study of molecular interfaces absorbing in the visible and give access to buried…

Optics · Physics 2024-05-10 Zsuzsanna Heiner , Valentin Petrov , Mark Mero

Vibrational sum- and difference-frequency generation (SFG and DFG) spectroscopy probes the nonlinear response of interfaces at mid-infrared (MIR) wavelengths while detecting upconverted signals in the visible. Recent work has moved from…

Nonlinear-optical microscopy and spectroscopy provide detailed spatial and spectroscopic contrast, specifically sensitive to structural symmetry and order. Ferroics, in particular, have been widely studied using second harmonic generation…

Sum-frequency generation (SFG) allows for coherent upconversion of an electromagnetic signal and has applications in mid-infrared vibrational spectroscopy of molecules. Recent experimental and theoretical studies have shown that plasmonic…

We propose non-phase-matched sum frequency generation (SFG) as a method for characterizing broadband multimode light. We demonstrate its advantages using high-gain parametric down conversion (PDC) as an example. By generating the sum…

Quantum Physics · Physics 2019-05-22 Denis A. Kopylov , Kirill Yu. Spasibko , Tatiana V. Murzina , Maria V. Chekhova

Sum-frequency generation (SFG) spectroscopy provides a versatile method for the investigation of non-centrosymmetric media and interfaces. Here, using tunable picosecond infrared (IR) pulses from a free-electron laser, the nonlinear optical…

Materials Science · Physics 2023-08-01 Riko Kiessling , Martin Wolf , Alexander Paarmann

Triple sum-frequency (TSF) spectroscopy is a recently-developed methodology that enables collection of multidimensional spectra by resonantly exciting multiple quantum coherences of vibrational and electronic states. This work reports the…

Optics · Physics 2018-08-23 Darien J. Morrow , Daniel D. Kohler , Kyle J. Czech , John C. Wright

Much work over the last 25 years has demonstrated that the interface-specific, alloptical technique, vibrational sum frequency generation (v-SFG) spectroscopy, is often uniquely capable of characterizing the structure and dynamics of…

Optics · Physics 2018-11-14 Martin Thämer , R. Kramer Campen , Martin Wolf

Sum frequency generation (SFG) has multiple applications, from optical sources to imaging, where efficient conversion requires either long interaction distances or large field concentrations in a quadratic nonlinear material. Metasurfaces…

Optics · Physics 2024-08-22 Neuton Li , Jihua Zhang , Dragomir N. Neshev , Andrey A. Sukhorukov

Plasmonic nanostructures that support surface plasmon (SP) resonance potentially provide a route for the development of nanoengineered nonlinear optical devices. In this work, second-order nonlinear light scattering, specifically…

Computational Physics · Physics 2016-12-20 Xiaoyan Y. Z. Xiong , Li Jun Jiang , Wei E. I. Sha , Yat Hei Lo , Weng Cho Chew

We present a 100 kHz broadband vibrational sum-frequency generation (VSFG) spectrometer operating in the 5.5-10.5 $\mu$m (950-1750 cm$^{-1}$) wavelength range. The mid-infrared beam of the system is obtained from a collinear, type-I…

Instrumentation and Detectors · Physics 2019-06-26 Zsuzsanna Heiner , Li Wang , Valentin Petrov , Mark Mero

The miniaturization of nonlinear light sources is central to the integrated photonic platform, driving a quest for high-efficiency frequency generation and mixing at the nanoscale. In this quest, the high-quality ($Q$) resonant dielectric…

Optics · Physics 2023-11-14 Siqi Feng , Tingting Liu , Wenya Chen , Feng Wu , Shuyuan Xiao

In chiral sum frequency generation (C-SFG), the chiral nature of ${\chi}^{(2)}$ requires the three involved electric fields to be pairwise non-parallel, leading to the traditional non-collinear configuration which is a hindrance for…

Optics · Physics 2016-12-07 Ziheng Ji , Wentao Yu , Hong Yang , Kaihui Liu , Qihuang Gong , Zhiwen Liu , Kebin Shi

We present a near-field optical technique for second harmonic imaging using bare tapered optical fiber tip illuminated with femtosecond laser pulses. Enhancement of electric field at the tip of the fiber results in enhanced second harmonic…

Materials Science · Physics 2009-10-31 I. I. Smolyaninov , H. Y. Liang , S. Aggarwal , R. Ramesh , C. H. Lee , C. C. Davis

Our current understanding of the structure and dynamics of aqueous interfaces at the molecular level has grown substantially in the last few decades due to the continuous development of surface-specific spectroscopies, such as vibrational…

Chemical Physics · Physics 2023-09-27 Yair Litman , Jinggang Lan , Yuki Nagata , David M. Wilkins
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