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In the last two decades, non-equilibrium spectroscopies have evolved from avant-garde studies to crucial tools for expanding our understanding of the physics of strongly correlated materials. The possibility of obtaining simultaneously…

The recent introduction of coherent optical communications has created a compelling need for ultra-fast phase-sensitive measurement techniques operating at milliwatt peak power levels and in time scales ranging from sub-picoseconds to…

Single molecule spectroscopy aims at unveiling often hidden but potentially very important contributions of single entities to a system's ensemble response. Albeit contributing tremendously to our ever growing understanding of molecular…

Chemical Physics · Physics 2017-12-19 Matz Liebel , Costanza Toninelli , Niek F. van Hulst

Controlling nonequilibrium responses in optically driven quantum materials is essential for advancing applications in energy conversion, ultrafast electronics, and quantum computation. Nonlinear optical spectroscopy serves as a powerful…

We theoretically demonstrate the ability of electron beams to probe the nonlinear photonic response with nanometer spatial resolution, well beyond the capabilities of existing optical techniques. Although the interaction of electron beams…

Mesoscale and Nanoscale Physics · Physics 2020-12-30 Andrea Konečná , Valerio Di Giulio , Vahagn Mkhitaryan , Claus Ropers , F. Javier García de Abajo

We present an alternative approach to pump-probe spectroscopy for measuring fast charge dynamics with an atomic force microscope (AFM). Our approach is based on coherent multifrequency lock-in measurement of the intermodulation between a…

Mesoscale and Nanoscale Physics · Physics 2019-01-30 Riccardo Borgani , David B. Haviland

We present a novel approach to model ultrafast time-dependent nonlinear optical polarization sensitive signals emitted from randomly-oriented molecules. By projecting the laboratory-frame analyzer polarization axis into the molecular frame…

Chemical Physics · Physics 2025-07-17 R. L. Thurston , N. Shivaram , Th. Weber , L. Z. Tan , D. S. Slaughter

In a solid, the electronic subsystem can exhibit incipient order with lower point group symmetry than the crystal lattice. External fields that couple to electronic order parameters have rarely been investigated, however, despite their…

Strongly Correlated Electrons · Physics 2024-01-11 Xinshu Zhang , Tyler Carbin , Adrian B. Culver , Kai Du , Kefeng Wang , Sang-Wook Cheong , Rahul Roy , Anshul Kogar

Attosecond nonlinear Fourier transform (NFT) pump probe spectroscopy is an experimental technique which allows investigation of the electronic excitation, ionization, and unimolecular dissociation processes. The NFT spectroscopy utilizes…

Chemical Physics · Physics 2021-02-11 Sergy Grebenshchikov , Sergio Carbajo

Non-collinear four-wave mixing (FWM) techniques at near-infrared (NIR), visible, and ultraviolet frequencies have been widely used to map vibrational and electronic couplings, typically in complex molecules. However, correlations between…

We report the observation of macroscopic field-free orientation, i.e. more than 73 % of CO molecules pointing in the same direction. This is achieved through an all-optical scheme operating at high particle densities ($>10^{17}$cm$^{-3}$)…

Chemical Physics · Physics 2014-07-09 P. M. Kraus , D. Baykusheva , H. J. Wörner

A new numerically and experimentally tested measurement method for the local electrical light field including its phase is presented. The method is based on Self Referencing Interferograms (SRI) such as shearing interferograms. The complex…

Instrumentation and Detectors · Physics 2016-10-27 Martin Berz , Cordelia Berz

We show how to emulate a conventional pump-probe scheme using a single frequency-chirped ultrashort UV pulse to obtain a time-resolved image of molecular ultrafast dynamics. The chirp introduces a spectral phase in time that encodes the…

Chemical Physics · Physics 2017-05-03 Denis Jelovina , Johannes Feist , Fernando Martín , Alicia Palacios

The rich information content of measurements in the molecular frame rather than the laboratory frame has motivated the development of several methods for aligning gas phase molecules in space. Even so, for asymmetric tops the problem of…

Atomic Physics · Physics 2016-11-23 Varun Makhija , Xiaoming Ren , Drue Gockel , Anh-Thu Le , Vinod Kumarappan

Chiroptical effects using circularly polarized light produce signals that change sign when switching either molecular handedness (enantiosensitivity) or the light helicity (circular dichroism). Here, we break this…

We propose an approach to probe coherent spin-state dynamics of molecules using circularly polarized hard x-ray pulses. For the dynamically aligned nitric oxide molecules in a coherent superposition spin-orbit coupled electronic state that…

Optics · Physics 2024-01-02 Xiaoyu Mi , Ming Zhang , Zheng Li

We study nonlinear interferometry applied to a measurement of atomic spin and demonstrate a sensitivity that cannot be achieved by any linear-optical measurement with the same experimental resources. We use alignment-to-orientation…

Quantum Physics · Physics 2014-09-25 R. J. Sewell , M. Napolitano , N. Behbood , G. Colangelo , F. Martin Ciurana , M. W. Mitchell

A nonlinear interferometry scheme is described theoretically to induce and resolve electron wave- function beating on time scales shorter than the optical cycle of the time-delayed pump and probe pulses. By employing two moderately intense…

Chemical Physics · Physics 2017-08-23 Christian Ott , Philipp Raith , Thomas Pfeifer

We propose an approach to sensitively probe the chirality of molecules by measuring their coherent optical absorption spectra. It is shown that quantum dynamics of the cyclic three-level chiral molecules driven by appropriately-designed…

Quantum Physics · Physics 2015-05-28 W. Z. Jia , L. F. Wei

Alignment and orientation of molecules by intense, ultrashort laser fields are crucial for a variety of applications in physics and chemistry. These include control of high harmonics generation, molecular orbitals tomography, control of…