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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 develop a Hamiltonian formalism to study energy and position/momentum correlations between a single Stokes photon and a single material excitation that are created as a pair in the spontaneous Raman scattering process. Our approach…

Quantum Physics · Physics 2020-01-16 Kai Shinbrough , Yanting Teng , Bin Fang , Virginia O. Lorenz , Offir Cohen

Statistical properties of light produced in spontaneous Raman scattering on an ensemble of molecules indicate the quantum nature of this phenomenon. The scattered light is non-classical and has high non-classical intensity correlations…

Optics · Physics 2026-05-15 Ivan V. Panyukov , Evgeny S. Andrianov

Time-resolved Raman spectroscopy techniques offer various ways to study the dynamics of molecular vibrations in liquids or gases and optical phonons in crystals. While these techniques give access to the coherence time of the vibrational…

Quantum Physics · Physics 2021-04-06 Santiago Tarrago Velez , Vivishek Sudhir , Nicolas Sangouard , Christophe Galland

Single-shot time resolved Coherent Anti-Stokes Raman Scattering (CARS) is presented as a viable method for fast measurements of molecular spectra. The method is based on the short spatial extension of femtosecond pulses and maps time delays…

Optics · Physics 2009-11-13 Yuri Paskover , I. Sh. Averbukh , Yehiam Prior

In spontaneous Raman process in atomic cell at high gain, both the Stokes field and the accompanying collective atomic excitation (atomic spin wave) are coherent. We find that, due to the spontaneous nature of the process, the phases of the…

Quantum Physics · Physics 2015-05-28 Cheng-ling Bian , Li-Qing Chen , Guo-Wan Zhang , Z. Y. Ou , Weiping Zhang

The spatial coherence of an atomic wavepacket can be detected in the scattered photons, even when the center-of-mass motion is in the quantum coherent superposition of two distant, non-overlapping wave packets. Spatial coherence manifests…

Due to their sub picosecond temporal resolution, coherent Raman spectroscopies have been proposed as a viable extension of Spontaneous Raman (SR) thermometry, to determine dynamics of mode specific vibrational energy content during out of…

A theoretical model describing the Raman scattering process in atomic vapors is constructed. The treatment investigates the low-excitation regime suitable for modern experimental applications. Despite the incorporated decoherence effects…

Quantum Physics · Physics 2012-07-16 Jan Kolodynski , Jan Chwedenczuk , Wojciech Wasilewski

In this work we develop an experimental procedure to interrogate the single- and multiphoton scattering matrices of an unknown quantum system interacting with propagating photons. Our proposal requires coherent state laser or microwave…

Quantum Physics · Physics 2017-10-17 Tomás Ramos , Juan José García-Ripoll

The process in which Raman scattering produces correlated Stokes and anti-Stokes radiation is known as Stokes--anti-Stokes (SaS) scattering. It has been shown recently that this process can generate entangled photon pairs, making it a…

Quantum Physics · Physics 2025-09-30 Raul Corrêa , Marcelo F. Santos , Carlos H. Monken , Ado Jorio

Coherent anti-Stokes Raman scattering is a widely used imaging technique that provides chemical contrast without the need for labels, making it an extremely valuable tool in physics, chemistry, and biology. In this work, we explore its…

Quantum Physics · Physics 2025-08-05 Giacomo Sorelli , Manuel Gessner , Frank Schlawin

We propose a scheme of generating and verifying mesoscopic-level entanglement between two atomic ensembles using non-resonant stimulated Raman scattering. Entanglement can be generated by direct detection or balanced homodyne detection of…

Quantum Physics · Physics 2007-05-23 Wenhai Ji , Chunbai Wu , S. J. van Enk , M. G. Raymer

We simulate a third-order nonlinear signal in a pump-probe spectroscopy from the interference between first- and second-order wavepackets (WPs), as well as from a state-to-state transition for Stokes and coherent anti-Stokes pathways in the…

Chemical Physics · Physics 2026-04-14 Subho Mitra , Arijit K. De

When a quantum system is put into an excited state, it will decay back to the ground state through a process termed spontaneous emission. It is generally assumed that spontaneous emission between different individual emitters would not be…

Quantum Physics · Physics 2024-05-09 D. C. Gold , P. Huft , C. Young , A. Safari , T. G. Walker , M. Saffman , D. D. Yavuz

Spin-polarised atomic ensembles probed by light based on the Faraday interaction are a versatile platform for numerous applications in quantum metrology and quantum information processing. Here we consider an ensemble of Alkali atoms that…

Quantum Physics · Physics 2022-05-11 Alexander Roth , Klemens Hammerer , Kirill S. Tikhonov

The Photon wave function Formalism provides an alternative description of some quantum optical phenomena in a more intuitive way. We use this formalism to describe the process of correlated Stokes--anti-Stokes Raman scattering. In this…

Quantum Physics · Physics 2020-12-08 A. V. A. Guimarães , M. F. Santos , A. Jorio , C. H. Monken

Nonlinear optical methods, such as coherent anti-Stokes Raman scattering (CARS) and stimulated Raman scattering (SRS), are able to perform label free imaging, with chemical bonds specificity. Here, we demonstrate that the use of circularly…

Raman scattering spectroscopy is widely used as an analytical technique in various fields, but its measurement process tends to be slow due to the low scattering cross-section. In the last decade, various broadband coherent Raman scattering…

Optics · Physics 2025-05-06 Takuma Nakamura , Kazuki Hashimoto , Takuro Ideguchi

Coherent Raman scattering spectroscopy is studied purposely, with the Gaussian ultrashort pulses as a hands-on elucidatory extraction tool of the clean coherent Raman resonant spectra from the overall measured data contaminated with the…

Optics · Physics 2017-04-05 Gombojav O. Ariunbold , Narangerel Altangerel
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