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We develop a detailed theoretical model of photo-induced proton-coupled electron transfer (PPCET) processes, which are at the basis of solar energy harvesting in biological systems and photovoltaic materials. Our model enables to analyze…

Chemical Physics · Physics 2021-04-13 Jiaji Zhang , Raffaele Borrelli , Yoshitaka Tanimura

Light interacting with metals elicits an ultrafast coherent many-body screening response on sub- to few-femtosecond time-scales, which makes its experimental observation challenging. Here, we describe the coherent two-dimensional (2D)…

Optics · Physics 2019-03-13 Marcel Reutzel , Andi Li , Hrvoje Petek

The transient signals derived from femtosecond pump-probe experiments are analyzed in terms of the coherent evolution of the energy levels perturbed by the excitation pulse. The model system is treated as the sum of independent two-level…

Atomic Physics · Physics 2016-09-13 A. Peralta Conde , R. Montero , A. Longarte

We demonstrate coherent control of multiphoton and above-threshold photoemission from a single solid-state nanoemitter driven by a fundamental and a weak second harmonic laser pulse. Depending on the relative phase of the two pulses,…

We describe optimized coherent control methods for two-photon transitions in atoms of a ladder-type three-state energy configuration. Our approach is based on the spatial coherent control scheme which utilizes counter-propagating ultrashort…

Atomic Physics · Physics 2015-10-28 Woojun Lee , Hyosub Kim , Kyungtae Kim , Jaewook Ahn

Quantum coherence between electronic states of a photoionized molecule and the resulting process of ultrafast electron-hole migration have been put forward as a possible quantum mechanism of charge-directed reactivity governing the…

We investigate the excitation of phonons in photoexcited antimony and demonstrate that the entire electron-lattice interactions, in particular coherent and incoherent electron-phonon coupling, can be probed simultaneously. Using femtosecond…

Detecting coherent phonons pose different challenges compared to coherent photons due to the much stronger interaction between phonons and matter. This is especially true for high frequency heat carrying phonons, which are intrinsic lattice…

Mesoscale and Nanoscale Physics · Physics 2018-03-14 Ding Ding , Xiaobo Yin , Baowen Li

The last two decades experimentally affirmed the quantum nature of free electron wavepackets by the rapid development of transmission electron microscopes into ultrafast, quantum-coherent systems. In particular, ultrafast electron pulses…

Optics · Physics 2022-09-30 Roy Shiloh , Tomas Chlouba , Peter Hommelhoff

Optical two-dimensional coherent spectroscopy (2DCS) is a powerful ultrafast spectroscopic technique that can greatly benefit from the unique features of a femtosecond laser operating at a kHz repetition rate. However, isolating specific…

Optics · Physics 2024-08-08 Stephen Revesz , Rustam Gatamov , Adolfo Misiara , Hebin Li

Light generation through optical harmonics plays a pivotal role in photonics, driving innovations in coherent light sources, biological imaging, and spectroscopy. Traditional methods for tuning optical harmonics, including electrostatic…

Optics · Physics 2025-04-01 George Trivizas , Matthew D. Feinstein , Euclides Almeida

When two-color femtosecond laser pulses interact with matter, electrons can be emitted through various multiphoton excitation pathways. Quantum interference between these pathways gives rise to a strong oscillation of the photoemitted…

Optics · Physics 2022-05-24 Ang Li , Yiming Pan , Philip Dienstbier , Peter Hommelhoff

The femtosecond optical pump-probe technique was used to study dynamics of photoexcited electrons and coherent optical phonons in transition metals Zn and Cd as a function of temperature and excitation level. The optical response in time…

Strongly Correlated Electrons · Physics 2009-11-11 Muneaki Hase , Kunie Ishioka , Jure Demsar , Kiminori Ushida , Masahiro Kitajima

Electron spin resonance (ESR) pulsed dipolar spectroscopy (PDS) is used in protein 3D structure determination. However, the accuracy of the signal analysis depends heavily on the background correction process. In this work, we derive the…

Quantitative Methods · Quantitative Biology 2021-07-01 Aritro Sinha Roy

We introduce and demonstrate a new approach to measuring coherent electron wave packets using high-harmonic spectroscopy. By preparing a molecule in a coherent superposition of electronic states, we show that electronic coherence opens…

Chemical Physics · Physics 2014-07-09 P. M. Kraus , S. B. Zhang , A. Gijsbertsen , R. R. Lucchese , N. Rohringer , H. J. Wörner

Two-dimensional (2D) spectroscopy combines high temporal and spectral resolution, allowing the observation of ultrafast energy transfer and the separation of homogeneous and inhomogeneous broadening. Typically, 2D spectroscopy is dominated…

Ab initio computation of two-dimensional electronic spectra is an expanding field, whose goal is improving upon simple, few-dimensional models often employed to explain experiments. Here, we propose an accurate and computationally…

Chemical Physics · Physics 2024-09-26 Tomislav Begušić , Jiří Vaníček

We report results regarding the electron transport in vertical quasi-2D layered 1T-TaS2 charge-density-wave devices. The low-frequency noise spectroscopy was used as a tool to study changes in the cross-plane electrical characteristics of…

The coupling between a two-level system and its environment leads to decoherence. Within the context of coherent manipulation of electronic or quasiparticle states in nanostructures, it is crucial to understand the sources of decoherence.…

Mesoscale and Nanoscale Physics · Physics 2015-05-27 P. Roulleau , S. Baer , T. Choi , F. Molitor , J. Güttinger , T. Müller , S. Dröscher , K. Ensslin , T. Ihn

In high-performance solar cells based on polymeric semiconductors, the mechanism of photocarrier generation on $<100$-fs timescales is yet to be unravelled. In particular the dynamics of early-time electronic coupling between excitons on…