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We demonstrate low-frequency interferometric impulsive stimulated Raman scattering (ISRS) imaging with high robustness to distortions by optical scattering. ISRS is a pump-probe coherent Raman spectroscopy that can capture Raman vibrational…

Photophysical and photochemical processes are ruled by the interplay between transient vibrational and electronic degrees of freedom, which are ultimately determined by the multidimensional potential energy surfaces (PESs). Differences…

The interaction between ultrashort light pulses and non-absorbing materials is dominated by Impulsive Stimulated Raman Scattering (ISRS). The description of ISRS in the context of pump\&probe experiments is based on effective classical…

Vibrational wavepacket dynamics in the ground (X) and excited (B) electronic states of iodine under impulsive-pump/broadband-probe excitation are revisited. A method for accurate chirp correction, necessary to determine the zero time for…

化学物理 · 物理学 2026-04-28 Ramandeep Kaur , Shaina Dhamija , Garima Bhutani , Amit Kumar , Arijit K. De

Spontaneous vibrational Raman scattering is a ubiquitous form of light-matter interaction whose description necessitates quantization of the electromagnetic field. It is usually considered as an incoherent process because the scattered…

量子物理 · 物理学 2023-07-18 Valeria Vento , Santiago Tarrago Velez , Anna Pogrebna , Christophe Galland

Stimulated Raman scattering, employing a pump and a Stokes beam, exhibits itself through both the Raman loss observed in the pump beam and the Raman gain in the Stokes beam. This phenomenon finds application in spectroscopy for chemical…

光学 · 物理学 2024-08-13 Minhaeng Cho

Coherent Anti-Stokes Raman Scattering (CARS) processes are ``coherent,'' but the phase of the anti-Stokes radiation is usually lost by most incoherent spectroscopic CARS measurements. We propose a novel Raman microscopy imaging method…

光学 · 物理学 2009-11-10 D. L. Marks , S. A. Boppart

Three-color coherent anti-Stokes Raman scattering represents non-degenerate four wave mixing process that includes both a non-resonant and resonant processes, the contributions of which depend on how the molecular vibrational modes are…

光学 · 物理学 2020-10-14 Supriya Nagpal , Bryan Semon , Gombojav O. Ariunbold

A general fundamental relation connecting the correlation of Stokes and anti-Stokes modes to the quantum statistical behavior of vibration and pump modes in Raman-active materials is derived. We show that under certain conditions this…

量子物理 · 物理学 2016-08-15 Özgür E. Müstecaplıoğlu , Alexander S. Shumovsky

Vibrational motions in electronically excited states can be observed by either time and frequency resolved infrared absorption or by off resonant stimulated Raman techniques. Multipoint correlation function expressions are derived for both…

量子物理 · 物理学 2017-09-13 Konstantin E. Dorfman , Benjamin P. Fingerhut , Shaul Mukamel

The operator solution of a completely quantum mechanical Hamiltonian of the Raman processes is used here to investigate the possibility of obtaining intermodal entanglement between different modes involved in the Raman processes (e.g. pump…

量子物理 · 物理学 2022-06-10 Biswajit Sen , Sandip Kumar Giri , Swapan Mandal , C. H. Raymond Ooi , Anirban Pathak

Excited-state vibrational dynamics in molecules can be studied by an electronically off-resonant Raman process induced by a probe pulse with variable delay with respect to an actinic pulse. We establish the connection between several…

化学物理 · 物理学 2013-09-27 Konstantin E. Dorfman , Benjamin P. Fingerhut , Shaul Mukamel

Stimulated Raman scattering (SRS) represents a powerful tool for accessing the vibrational properties of molecular compounds or solid state systems. From a spectroscopic perspective, SRS is able to capture Raman spectra free from incoherent…

We propose a novel femtosecond stimulated Raman spectroscopy (FSRS) technique that combines entangled photons with interference detection to select matter pathways and enhance the resolution. Following photo excitation by an actinic pump,…

量子物理 · 物理学 2014-07-15 Konstantin E. Dorfman , Frank Schlawin , Shaul Mukamel

We propose a method for increasing the Raman scattering from an ensemble of molecules by up to four orders of magnitude. Our method requires an additional coherent source of IR radiation with the half-frequency of the Stokes shift. This…

量子物理 · 物理学 2019-04-24 V. Yu. Shishkov , E. S. Andrianov , A. A. Pukhov , A. P. Vinogradov , A. A. Lisyansky

The development of accurate tools to characterize Intramolecular Vibrational Redistribution (IVR) is of major interest in chemistry. In this context, surface-enhanced vibrational spectroscopies stand up as well-established techniques to…

The motion of chemical bonds within molecules can be observed in real time, in the form of vibrational wavepackets prepared and interrogated through ultrafast nonlinear spectroscopy. Such nonlinear optical measurements are commonly…

We provide conclusive demonstration of vibrational pumping under Surface Enhanced Raman Scattering (SERS) conditions by performing anti-Stokes/Stokes ratio measurements down to 10 K using dried silver colloids, the dye rhodamine 6G and 676…

化学物理 · 物理学 2007-05-23 R. C. Maher , P. G. Etchegoin , E. C. Le Ru , L. F. Cohen

A semiclassical model is used to investigate the possibility of selectively exciting one of two closely spaced, uncoupled Raman transitions. The duration of the intense pump pulse that creates the Raman coherence is shorter than the…

化学物理 · 物理学 2009-11-10 S. A. Malinovskaya , P. H. Bucksbaum , P. R. Berman

A quantum model of the Raman process with the independent Stokes and anti-Stokes nonlinear interactions is developed to study nonclassical correlations between the photons in the Stokes and anti-Stokes fields. The role of the laser pump…

量子物理 · 物理学 2021-03-26 Kishore Thapliyal , Jan Perina
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