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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

We present experimental evidence for spin-orbit interaction of an electron as it scatters from a neutral atom. The scattering process takes place within a Rb$_2$ ultralong-range Rydberg molecule, consisting of a Rydberg atomic core, a…

Coherent x-ray diffractive imaging is extended to high resolution strain analysis in crystalline nanostructured devices. The application potential is demonstrated by determining the strain distribution in (Ga,Mn)As/GaAs nanowires. By…

Established x-ray diffraction methods allow for high-resolution structure determination of crystals, crystallized protein structures or even single molecules. While these techniques rely on coherent scattering, incoherent processes like…

We report an experimental and theoretical study of the evolution of vibrational coherence in a thermal ensemble of nitrogen molecules. Rotational dephasing and rephasing of the vibrational coherence is detected by coherent anti-Stokes Raman…

Quantum Physics · Physics 2015-06-04 Martin Bitter , Evgeny A. Shapiro , Valery Milner

The requirement of high space-time resolution and brightness is a great challenge for imaging atomic motion and making molecular movies. Important breakthroughs in ultrabright tabletop laser, x-ray and electron sources have enabled the…

Atomic Physics · Physics 2022-02-10 Ming Zhang , Zhenning Guo , Xiaoyu Mi , Zheng Li , Yunquan Liu

Ultrafast-optical-pump -- structural-probe measurements, including ultrafast electron and x-ray scattering, provide direct experimental access to the fundamental timescales of atomic motion, and are thus foundational techniques for studying…

We present a quantum mechanical theory of optically induced dynamic nuclear polarization applicable to quantum dots and other interacting spin systems. The exact steady state of the optically driven coupled electron-nuclear system is…

Mesoscale and Nanoscale Physics · Physics 2019-02-04 Thomas Nutz , Edwin Barnes , Sophia E. Economou

Time-resolved ultrafast x-ray scattering from photo-excited matter is an emerging method to image ultrafast dynamics in matter with atomic-scale spatial and temporal resolutions. For a correct and rigorous understanding of current and…

Chemical Physics · Physics 2017-11-16 Gopal Dixit , Robin Santra

Molecules present a versatile platform for quantum information science, and are candidates for sensing and computation applications. Robust spin-optical interfaces are key to harnessing the quantum resources of materials. To date,…

We show that quantum rotational wavepacket dynamics in molecules can be described by a new system-environment model, which consists of a rotational subsystem coupled to a magnetically tunable spin bath formed by the nuclear spins within the…

Quantum Physics · Physics 2025-02-25 Timur V. Tscherbul , Lincoln D. Carr

Ultrafast spectroscopies constitute a fundamental tool to investigate the dynamics of non-equilibrium many-body states in correlated materials. Two-pulses (pump-probe) experiments have shed new light on the interplay between high-energy…

Strongly Correlated Electrons · Physics 2016-09-01 Claudio Giannetti

Recording molecular movies on ultrafast timescales has been a longstanding goal for unravelling detailed information about molecular dynamics. We present the direct experimental recording of very-high-resolution and -fidelity molecular…

Structured x-rays carrying an orbital angular momentum break spatial inversion symmetry and have been proposed as a means to probe chirality. We theoretically investigate twisted non-resonant x-ray diffraction from chiral molecules and…

Optics · Physics 2026-03-02 Akilesh Venkatesh , Phay J. Ho , Jérémy R. Rouxel

Quantum entanglement has emerged as a great resource for interactions between molecules and radiation. We propose a new paradigm of stimulated Raman scattering with entangled photons. A quantum ultrafast Raman spectroscopy is developed for…

Quantum Physics · Physics 2023-05-26 Joel Jiahao Fan , Zhe-Yu Jeff Ou , Zhedong Zhang

Molecular rotational spectroscopy based on strong-field-ionization-induced nitrogen laser is employed to investigate the time evolution of the rotational wave packet composed by a coherent superposition of quantum rotational states created…

Unique intensity features arising from dynamical diffraction arise in coherent x-ray nanobeam diffraction patterns of crystals having thicknesses larger than the x-ray extinction depth or exhibiting combinations of nanoscale and mesoscale…

Materials Science · Physics 2020-02-27 A. Pateras , J. Park , Y. Ahn , J. A. Tilka , M. V. Holt , H. Kim , L. J. Mawst , P. G. Evans

The development of X-ray free-electron lasers (XFELs) has enabled ultrafast X-ray diffraction (XRD) experiments, which are capable of resolving electronic/vibrational transitions and structural changes in molecules, or capturing molecular…

Chemical Physics · Physics 2024-08-29 Sebastian V. Pios , Jiaji Zhang , Maxim F. Gelin , Hong-Guang Duan , Lipeng Chen

We introduce a new optical tool - a "two-dimensional optical centrifuge", capable of aligning molecules in extreme rotational states. Unlike the conventional centrifuge, which confines the molecules in the plane of their rotation, its…

Chemical Physics · Physics 2016-05-18 A. A. Milner , A. Korobenko , V. Milner

We propose and demonstrate a novel technique that combines Raman scattering and optical cycling in molecules with diagonal Franck-Condon factors. This resonance Raman optical cycling manipulates molecules to behave like efficient…

Atomic Physics · Physics 2021-08-26 J. C. Shaw , J. C. Schnaubelt , D. J. McCarron
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