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Vibrational sum frequency generation (SFG) is a nonlinear spectroscopic technique widely used to study the molecular structure and dynamics of surface systems. However, the spatial resolution achieved by far-field observations is…

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…

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) 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…

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

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…

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

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…

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…

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

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 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

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

Second-order nonlinear optical interactions such as sum- and difference-frequency generation are widely used for bioimaging and as selective probes of interfacial environments. However, inefficient nonlinear optical conversion often leads…

Optics · Physics 2015-05-07 Aaron J. Goodman , William A. Tisdale

By projecting onto complex optical mode profiles, it is possible to estimate arbitrarily small separations between objects with quantum-limited precision, free of uncertainty arising from overlapping intensity profiles. Here we extend these…

Raman spectroscopy and Second Harmonic Generation (SHG) are complementary, non-destructive techniques that provide rich and distinct insights into the structural and electronic properties of materials. Raman spectroscopy offers detailed…

Optics · Physics 2026-04-30 Volodymyr Multian , Luigi Bonacina , Jérémie Teyssier

Second harmonic generation (SHG) microscopy is a valuable tool for optical microscopy. SHG microscopy is normally performed as a point scanning imaging method, which lacks phase information and is limited in spatial resolution by the…

We introduce sum-frequency generation (SFG) as an effective physical two-photon detector for high power two-mode squeezed coherent states with arbitrary frequency separation, as produced by parametric oscillators well above the threshold.…

Optics · Physics 2013-10-30 Faina Shikerman , Avi Pe'er

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

We report on the experimental observation of non-resonant, second-order optical Sum-Frequency Generation (SFG) in five different atomic and molecular gases. The measured signal is attributed to a SFG process by characterizing its intensity…

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