Relevant bibliographies by topics / Electronic quantum coherence

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Academic literature on the topic 'Electronic quantum coherence'

Author: Grafiati
Published: 4 May 2024

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Journal articles on the topic "Electronic quantum coherence"

1

Fassioli, Francesca, Rayomond Dinshaw, Paul C. Arpin, and Gregory D. Scholes. "Photosynthetic light harvesting: excitons and coherence." Journal of The Royal Society Interface 11, no. 92 (2014): 20130901. http://dx.doi.org/10.1098/rsif.2013.0901.

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Photosynthesis begins with light harvesting, where specialized pigment–protein complexes transform sunlight into electronic excitations delivered to reaction centres to initiate charge separation. There is evidence that quantum coherence between electronic excited states plays a role in energy transfer. In this review, we discuss how quantum coherence manifests in photosynthetic light harvesting and its implications. We begin by examining the concept of an exciton, an excited electronic state delocalized over several spatially separated molecules, which is the most widely available signature of quantum coherence in light harvesting. We then discuss recent results concerning the possibility that quantum coherence between electronically excited states of donors and acceptors may give rise to a quantum coherent evolution of excitations, modifying the traditional incoherent picture of energy transfer. Key to this (partially) coherent energy transfer appears to be the structure of the environment, in particular the participation of non-equilibrium vibrational modes. We discuss the open questions and controversies regarding quantum coherent energy transfer and how these can be addressed using new experimental techniques.
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2

Palato, Samuel, Hélène Seiler, Parmeet Nijjar, Oleg Prezhdo, and Patanjali Kambhampati. "Atomic fluctuations in electronic materials revealed by dephasing." Proceedings of the National Academy of Sciences 117, no. 22 (2020): 11940–46. http://dx.doi.org/10.1073/pnas.1916792117.

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The microscopic origin and timescale of the fluctuations of the energies of electronic states has a significant impact on the properties of interest of electronic materials, with implication in fields ranging from photovoltaic devices to quantum information processing. Spectroscopic investigations of coherent dynamics provide a direct measurement of electronic fluctuations. Modern multidimensional spectroscopy techniques allow the mapping of coherent processes along multiple time or frequency axes and thus allow unprecedented discrimination between different sources of electronic dephasing. Exploiting modern abilities in coherence mapping in both amplitude and phase, we unravel dissipative processes of electronic coherences in the model system of CdSe quantum dots (QDs). The method allows the assignment of the nature of the observed coherence as vibrational or electronic. The expected coherence maps are obtained for the coherent longitudinal optical (LO) phonon, which serves as an internal standard and confirms the sensitivity of the technique. Fast dephasing is observed between the first two exciton states, despite their shared electron state and common environment. This result is contrary to predictions of the standard effective mass model for these materials, in which the exciton levels are strongly correlated through a common size dependence. In contrast, the experiment is in agreement with ab initio molecular dynamics of a single QD. Electronic dephasing in these materials is thus dominated by the realistic electronic structure arising from fluctuations at the atomic level rather than static size distribution. The analysis of electronic dephasing thereby uniquely enables the study of electronic fluctuations in complex materials.
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3

Zhu, Ruidan, Meixia Ruan, Hao Li, et al. "Vibrational and vibronic coherences in the energy transfer process of light-harvesting complex II revealed by two-dimensional electronic spectroscopy." Journal of Chemical Physics 156, no. 12 (2022): 125101. http://dx.doi.org/10.1063/5.0082280.

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The presence of quantum coherence in light-harvesting complex II (LHCII) as a mechanism to understand the efficiency of the light-harvesting function in natural photosynthetic systems is still debated due to its structural complexity and weak-amplitude coherent oscillations. Here, we revisit the coherent dynamics and clarify different types of coherences in the energy transfer processes of LHCII using a joint method of the high-S/N transient grating and two-dimensional electronic spectroscopy. We find that the electronic coherence decays completely within 50 fs at room temperature. The vibrational coherences of chlorophyll a dominate over oscillations within 1 ps, whereas a low-frequency mode of 340 cm−1 with a vibronic mixing character may participate in vibrationally assisted energy transfer between chlorophylls a. Our results may suggest that vibronic mixing is relevant for rapid energy transfer processes among chlorophylls in LHCII.
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4

Wu, Yanling, Qiong Wu, Fei Sun, Cai Cheng, Sheng Meng, and Jimin Zhao. "Emergence of electron coherence and two-color all-optical switching in MoS2 based on spatial self-phase modulation." Proceedings of the National Academy of Sciences 112, no. 38 (2015): 11800–11805. http://dx.doi.org/10.1073/pnas.1504920112.

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Generating electron coherence in quantum materials is essential in optimal control of many-body interactions and correlations. In a multidomain system this signifies nonlocal coherence and emergence of collective phenomena, particularly in layered 2D quantum materials possessing novel electronic structures and high carrier mobilities. Here we report nonlocal ac electron coherence induced in dispersed MoS2 flake domains, using coherent spatial self-phase modulation (SSPM). The gap-dependent nonlinear dielectric susceptibility χ(3) measured is surprisingly large, where direct interband transition and two-photon SSPM are responsible for excitations above and below the bandgap, respectively. A wind-chime model is proposed to account for the emergence of the ac electron coherence. Furthermore, all-optical switching is achieved based on SSPM, especially with two-color intraband coherence, demonstrating that electron coherence generation is a ubiquitous property of layered quantum materials.
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5

Schwickert, David, Marco Ruberti, Přemysl Kolorenč, et al. "Charge-induced chemical dynamics in glycine probed with time-resolved Auger electron spectroscopy." Structural Dynamics 9, no. 6 (2022): 064301. http://dx.doi.org/10.1063/4.0000165.

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In the present contribution, we use x-rays to monitor charge-induced chemical dynamics in the photoionized amino acid glycine with femtosecond time resolution. The outgoing photoelectron leaves behind the cation in a coherent superposition of quantum mechanical eigenstates. Delayed x-ray pulses track the induced coherence through resonant x-ray absorption that induces Auger decay. Temporal modulation of the Auger electron signal correlated with specific ions is observed, which is governed by the initial electronic coherence and subsequent vibronic coupling to nuclear degrees of freedom. In the time-resolved x-ray absorption measurement, we monitor the time-frequency spectra of the resulting many-body quantum wave packets for a period of 175 fs along different reaction coordinates. Our experiment proves that by measuring specific fragments associated with the glycine dication as a function of the pump-probe delay, one can selectively probe electronic coherences at early times associated with a few distinguishable components of the broad electronic wave packet created initially by the pump pulse in the cation. The corresponding coherent superpositions formed by subsets of electronic eigenstates and evolving along parallel dynamical pathways show different phases and time periods in the range of [Formula: see text] and [Formula: see text] fs. Furthermore, for long delays, the data allow us to pinpoint the driving vibrational modes of chemical dynamics mediating charge-induced bond cleavage along different reaction coordinates.
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6

Lombardi, Federico, Alessandro Lodi, Ji Ma, et al. "Quantum units from the topological engineering of molecular graphenoids." Science 366, no. 6469 (2019): 1107–10. http://dx.doi.org/10.1126/science.aay7203.

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Robustly coherent spin centers that can be integrated into devices are a key ingredient of quantum technologies. Vacancies in semiconductors are excellent candidates, and theory predicts that defects in conjugated carbon materials should also display long coherence times. However, the quantum performance of carbon nanostructures has remained stunted by an inability to alter the sp2-carbon lattice with atomic precision. Here, we demonstrate that topological tailoring leads to superior quantum performance in molecular graphene nanostructures. We unravel the decoherence mechanisms, quantify nuclear and environmental effects, and observe spin-coherence times that outclass most nanomaterials. These results validate long-standing assumptions on the coherent behavior of topological defects in graphene and open up the possibility of introducing controlled quantum-coherent centers in the upcoming generation of carbon-based optoelectronic, electronic, and bioactive systems.
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7

Novelli, Fabio, Jonathan O. Tollerud, Dharmalingam Prabhakaran, and Jeffrey A. Davis. "Persistent coherence of quantum superpositions in an optimally doped cuprate revealed by 2D spectroscopy." Science Advances 6, no. 9 (2020): eaaw9932. http://dx.doi.org/10.1126/sciadv.aaw9932.

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Quantum materials displaying intriguing magnetic and electronic properties could be key to the development of future technologies. However, it is poorly understood how the macroscopic behavior emerges in complex materials with strong electronic correlations. While measurements of the dynamics of excited electronic populations have been able to give some insight, they have largely neglected the intricate dynamics of quantum coherence. Here, we apply multidimensional coherent spectroscopy to a prototypical cuprate and report unprecedented coherent dynamics persisting for ~500 fs, originating directly from the quantum superposition of optically excited states separated by 20 to 60 meV. These results reveal that the states in this energy range are correlated with the optically excited states at ~1.5 eV and point to nontrivial interactions between quantum many-body states on the different energy scales. In revealing these dynamics and correlations, we demonstrate that multidimensional coherent spectroscopy can interrogate complex quantum materials in unprecedented ways.
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8

Kim, Jeongho, Shaul Mukamel, and Gregory D. Scholes. "Two-Dimensional Electronic Double-Quantum Coherence Spectroscopy." Accounts of Chemical Research 42, no. 9 (2009): 1375–84. http://dx.doi.org/10.1021/ar9000795.

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9

Hamilton, James R., Edoardo Amarotti, Carlo N. Dibenedetto, et al. "Time–Frequency Signatures of Electronic Coherence of Colloidal CdSe Quantum Dot Dimer Assemblies Probed at Room Temperature by Two-Dimensional Electronic Spectroscopy." Nanomaterials 13, no. 14 (2023): 2096. http://dx.doi.org/10.3390/nano13142096.

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Electronic coherence signatures can be directly identified in the time–frequency maps measured in two-dimensional electronic spectroscopy (2DES). Here, we demonstrate the theory and discuss the advantages of this approach via the detailed application to the fast-femtosecond beatings of a wide variety of electronic coherences in ensemble dimers of quantum dots (QDs), assembled from QDs of 3 nm in diameter, with 8% size dispersion in diameter. The observed and computed results can be consistently characterized directly in the time–frequency domain by probing the polarization in the 2DES setup. The experimental and computed time–frequency maps are found in very good agreement, and several electronic coherences are characterized at room temperature in solution, before the extensive dephasing due to the size dispersion begins. As compared to the frequency–frequency maps that are commonly used in 2DES, the time–frequency maps allow exploiting electronic coherences without additional post-processing and with fewer 2DES measurements. Towards quantum technology applications, we also report on the modeling of the time–frequency photocurrent response of these electronic coherences, which paves the way to integrating QD devices with classical architectures, thereby enhancing the quantum advantage of such technologies for parallel information processing at room temperature.
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10

Kobayashi, Yuki, and Stephen R. Leone. "Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy." Journal of Chemical Physics 157, no. 18 (2022): 180901. http://dx.doi.org/10.1063/5.0119942.

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Coherence can drive wave-like motion of electrons and nuclei in photoexcited systems, which can yield fast and efficient ways to exert materials’ functionalities beyond the thermodynamic limit. The search for coherent phenomena has been a central topic in chemical physics although their direct characterization is often elusive. Here, we highlight recent advances in time-resolved x-ray absorption spectroscopy (tr-XAS) to investigate coherent phenomena, especially those that utilize the eminent light source of isolated attosecond pulses. The unparalleled time and state sensitivities of tr-XAS in tandem with the unique element specificity render the method suitable to study valence electronic dynamics in a wide variety of materials. The latest studies have demonstrated the capabilities of tr-XAS to characterize coupled electronic–structural coherence in small molecules and coherent light–matter interactions of core-excited excitons in solids. We address current opportunities and challenges in the exploration of coherent phenomena, with potential applications for energy- and bio-related systems, potential crossings, strongly driven solids, and quantum materials. With the ongoing developments in both theory and light sources, tr-XAS holds great promise for revealing the role of coherences in chemical dynamics.
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