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We report a novel experimental technique to investigate ultrafast dynamics in photoexcited molecules by probing the third-order nonlinear optical susceptibility. A non-colinear 3-pulse scheme is developed to probe the ultrafast dynamics of…

We investigate ultrafast dynamics of the lowest singlet excited electronic state in liquid nitrobenzene using Ultrafast Transient Polarization Spectroscopy (UTPS), extending the well-known technique of Optical-Kerr Effect (OKE) spectroscopy…

As the simplest nitroaromatic compound, nitrobenzene is an interesting model system to explore the rich photochemistry of nitroaromatic compounds. Previous measurements of nitrobenzene's photochemical dynamics have probed structural and…

We report the first coherent excitation of intramolecular vibrational modes via the nonlinear interaction of a TeraHertz (THz) light field with molecular liquids. A terahertz-terahertz-Raman pulse sequence prepares the coherences with a…

化学物理 · 物理学 2015-12-29 Marco A. Allodi , Ian A. Finneran , Geoffrey A. Blake

The correlated behavior of electrons determines the structure and optical properties of molecules, semiconductor and other systems. Valuable information on these correlations is provided by measuring the response to femtosecond laser…

介观与纳米尺度物理 · 物理学 2009-11-13 Shaul Mukamel , Rafal Oszwaldowski , Lijun Yang

Controlling nonequilibrium dynamics in quantum materials requires ultrafast probes with spectral selectivity. We report femtosecond reflectivity measurements on the cuprate superconductor Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$ using…

We report an experiment to measure the femtosecond electric field of the signal emitted from an optical third-order nonlinear interaction in carbon dioxide molecules. Using degenerate four-wave mixing with femtosecond near infrared laser…

量子物理 · 物理学 2022-10-05 Francis Walz , Siddhant Pandey , Liang Z. Tan , Niranjan Shivaram

The ultrafast optical Kerr effect (OKE) is widely used to investigate the structural dynamics and interactions of liquids, solutions and solids by observing their intrinsic nonlinear temporal responses through nearly-collinear four-wave…

光学 · 物理学 2021-03-15 Lucas Huber , Sebastian Maehrlein , Feifan Wang , Yufeng Liu , Xiaoyang Zhu

We present a theoretical study of the ultrafast electron dynamics in transition metals using ultrashort pulsed laser beams. The significant influence of the contribution of the dynamics of produced nonthermal electrons to electron…

材料科学 · 物理学 2016-12-14 George D. Tsibidis

We introduce and experimentally demonstrate a method, where the two intrinsic time scales of a molecule, the slow nuclear motion and the fast electronic motion, are simultaneously measured in a photo-electron photo-ion coincidence…

Among polycyclic aromatic hydrocarbons, pyrene is widely used as an optical probe thanks to peculiar ultraviolet absorption and infrared emission features. Interestingly, this molecule is also an abundant component of the interstellar…

化学物理 · 物理学 2021-11-19 Katherine R. Herperger , Jannis Krumland , Caterina Cocchi

Coherent light pulses of few to hundreds of femtoseconds (fs) duration have prolifically served the field of ultrafast phenomena. While fs pulses address mainly dynamics of nuclear motion in molecules or lattices in the gas, liquid or…

化学物理 · 物理学 2013-04-26 P. A. Carpeggiani , P. Tzallas , A. Palacios , D. Gray , F. Martín , D. Charalambidis

Femtosecond laser pulses interacting with LiNbO3 has been widely applied in intense terahertz generation, excitation and imaging of phonon polaritons and modulating light. It is of great importance to study the nonlinearities induced by…

光学 · 物理学 2019-06-26 Bo Wang , Chun Wang , Li Wang , Xiaojun Wu

We resolve the real-time electric field of a femtosecond third-order nonlinear optical signal in the molecular frame. The electric field emitted by the induced third-order polarization from impulsively pre-aligned gas-phase molecules at…

We investigate ultrafast vibronic dynamics triggered by intense femtosecond infrared pulses in small molecules. Our study is based on numerical simulations performed with 2D model molecules, and analyzed in the perspective of the renown…

Ultrashort pulses can excite or ionize molecules and populate coherent electronic wavepackets, inducing complex dynamics. In this work, we simulate the coupled electron-nuclear dynamics upon ionization to different electronic wavepackets of…

We use a quantum-dynamical model to investigate the optical response of graphene under low excitation power. Ultrafast carrier relaxation processes, which play an important role for understanding the optical response of graphene, are…

介观与纳米尺度物理 · 物理学 2011-06-27 Zheshen Zhang , Paul L. Voss

We investigate the interplay of diffraction and nonlinear effects during propagation of very short light pulses. Adapting the factorization approach to the problem at hand by keeping the transverse-derivative terms apart from the residual…

光学 · 物理学 2016-02-17 C. L. Korpa , Gy. Toth , J. Hebling

The nonlinear interaction between Near-Infrared (NIR) and Terahertz pulses is principally investigated as a means for the detection of radiation in the hardly accessible THz spectral region. Most studies have targeted second-order nonlinear…

The coherent interaction with ultrashort light pulses is a powerful strategy for monitoring and controlling the dynamics of wave packets in all states of matter. As light presents an oscillation period of a few femtoseconds ($T=2.6$~fs in…

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