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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

Excited-state vibrations are crucial for determining photophysical and photochemical properties of molecular compounds. Stimulated Raman scattering can coherently stimulate and probe molecular vibrations with optical pulses, but it is…

光学 · 物理学 2020-10-13 Giovanni Batignani , Carino Ferrante , Tullio Scopigno

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…

化学物理 · 物理学 2026-04-14 Subho Mitra , Arijit K. De

Nonstationary molecular states which contain electronic coherences can be impulsively created and manipulated by using recently-developed ultrashort optical and X-ray pulses via photoexcitation, photoionization and Auger processes. We…

化学物理 · 物理学 2015-09-02 Konstantin E. Dorfman , Kochise Bennett , Shaul Mukamel

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

A coherent control scheme for the population distribution in the vibrational states of nonpolar molecules is proposed. Our theoretical analysis and results of numerical simulations for the interaction of the hydrogen molecular ion in its…

量子物理 · 物理学 2011-02-17 A. Picón , J. Biegert , A. Jaron-Becker , A. Becker

In this study, we demonstrate coherent optical excitation of the electronic Raman transition between the $1s\left(A_1\right)$ and $1s\left(E\right)$ split states of phosphorus donor in crystalline silicon. The dynamics of the generated…

介观与纳米尺度物理 · 物理学 2026-02-05 Adam Gindl , Martin Čmel , František Trojánek , Petr Malý , Zbyněk Šobáň , Alexandr Pošta , Martin Kozák

Vibrational coherences in ultrafast pump-probe (PP) and 2D electronic spectroscopy (2DES) provide insight into the excited state dynamics of molecules. Femtosecond coherence spectra (FCS) and 2D beat maps yield information about…

化学物理 · 物理学 2024-06-07 Dale Green , Giovanni Bressan , Ismael A. Heisler , Stephen R. Meech , Garth A. Jones

We present a novel approach to transient Raman spectroscopy, which combines stochastic probe pulses and a covariance-based detection to measure stimulated Raman signals in alpha-quartz. A coherent broadband pump is used to simultaneously…

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

We show theoretically that it is possible to coherently transfer vibrational excitation between trapped neutral atoms over a micrometer apart. To this end we consider three atoms, where two are in the electronic ground state and one is…

原子物理 · 物理学 2024-12-30 Abhijit Pendse , Sebastian Wüster , Matthew T. Eiles , Alexander Eisfeld

Raman heterodyne spectroscopy is a powerful tool for characterizing the energy and dynamics of spins. The technique uses an optical pump to transfer coherence from a spin transition to an optical transition where the coherent emission is…

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…

We demonstrate experimentally how the process of Stimulated Raman Adiabatic Passage (STIRAP) can be utilized for efficient coherent internal state transfer in single trapped and laser-cooled $^{40}$Ca$^+$ ions. The transfer from the…

Vibrational spectroscopy, comprised of infrared absorption and Raman scattering spectroscopy, is widely used for label-free optical sensing and imaging in various scientific and industrial fields. The group theory states that the two…

化学物理 · 物理学 2019-10-09 Kazuki Hashimoto , Venkata Ramaiah Badarla , Akira Kawai , Takuro Ideguchi

We used optically detected magnetic resonance (ODMR) technique to directly probe electron-spin resonance transitions in the excited state of negatively-charged boron vacancy (VB-) defects in hexagonal boron nitride (hBN) at room…

We report on the first demonstration of nonlinear dual-frequency-comb spectroscopy. In multi-heterodyne femtosecond Raman-induced Kerr-effect spectroscopy, the Raman gain resulting from the coherent excitation of molecular vibrations by a…

Coherent manipulation of quantum states is of crucial importance in accurate control of a quantum system. A fundamental goal is coherently transferring the population of a desired state with near-unit fidelity. For this propose, we…

原子物理 · 物理学 2018-12-05 Luyao Yan , Dandan Ma , Dongmin Yu , Jing Qian

Efficient preparation and detection of the motional state of trapped ions is important in many experiments ranging from quantum computation to precision spectroscopy. We investigate the stimulated Raman adiabatic passage (STIRAP) technique…

量子物理 · 物理学 2016-02-17 Florian Gebert , Yong Wan , Fabian Wolf , Jan C. Heip , Piet O. Schmidt

Excitation of four coherent phonon modes of different symmetries has been realized in copper metaborate CuB$_2$O$_4$ via impulsive stimulated Raman scattering (ISRS). Phonons were detected by monitoring changes in the linear optical…

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