相关论文: Characterization and quantification of the role of…
A remarkable amount of theoretical research has been carried out to elucidate the physical origins of the recently observed long-lived quantum coherence in the electronic energy transfer process in biological photosynthetic systems.…
A fundamental task in photonics is to characterise an unknown optical process, defined by properties such as birefringence, spectral response, thickness and flatness. Amongst many ways to achieve this, single-photon probes can be used in a…
Photosynthetic antenna complexes capture and concentrate solar radiation by transferring the excitation to the reaction center which stores energy from the photon in chemical bonds. This process occurs with near-perfect quantum efficiency.…
The idea that excitonic state (electronic) coherences are of fundamental importance to natural photosynthesis gained popularity when, a decade ago, slowly dephasing quantum beats were observed in the two-dimensional electronic spectra of…
This thesis looks at the electronic energy transfer in the Fenna-Matthews-Olson complex, in which evidence of long-lived coherence has been observed in 2-dimensional infrared experiments. I use three techniques: the numerically exact…
The presence of quantum effects in photosynthetic excitation energy transfer has been intensely debated over the past decade. Nonlinear spectroscopy cannot unambiguously distinguish coherent electronic dynamics from underdamped vibrational…
The role of quantum coherence and the environment in the dynamics of excitation energy transfer is not fully understood. In this work, we introduce the concept of dynamical contributions of various physical processes to the energy transfer…
Attosecond science offers unprecedented precision in probing the initial moments of chemical reactions, revealing the dynamics of molecular electrons that shape reaction pathways. A fundamental question emerges: what role, if any, do…
Quantum Process Tomography (QPT) methods aim at identifying, i.e. estimating, a quantum process. QPT is a major quantum information processing tool, since it especially allows one to experimentally characterize the actual behavior of…
An arbitrary quantum-optical process (channel) can be completely characterized by probing it with coherent states using the recently developed coherent-state quantum process tomography (QPT) [Lobino et al., Science 322, 563 (2008)]. In…
Revealing possible long-living coherence in ultrafast processes allows detecting genuine quantum mechanical effects in molecules. To investigate such effects from a quantum chemistry perspective, we have developed a method for simulating…
During the first steps of photosynthesis, the energy of impinging solar photons is transformed into electronic excitation energy of the light-harvesting biomolecular complexes. The subsequent energy transfer to the reaction center is…
The description of excited state dynamics in multichromophoric systems constitutes both a theoretical and experimental challenge in modern physical chemistry. An experimental protocol which can systematically characterize both coherent and…
Quantum state tomography (QST) is the gold standard technique for obtaining an estimate for the state of small quantum systems in the laboratory. Its application to systems with more than a few constituents (e.g. particles) soon becomes…
We present a detailed theoretical study of the transfer of electronic excitation energy through the Fenna-Matthews-Olson (FMO) pigment-protein complex, using the new developed modified scaled hierarchical approach [Shi Q. et al, J Chem Phys…
The quantum dynamics of transport networks in the presence of noisy environments have recently received renewed attention with the discovery of long-lived coherences in different photosynthetic complexes. This experimental evidence has…
Recent advances in the spectroscopy of biomolecules have highlighted the possibility of quantum coherence playing an active role in biological energy transport. The revelation that quantum coherence can survive in the hot and wet…
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…
Photosystem II (PSII) reaction center is a unique protein-chromophore complex that is capable of efficiently separating electronic charges across the membrane after photoexcitation. In the PSII reaction center, the primary energy- and…
Quantum coherence is a fundamental property of quantum systems, separating quantum from classical physics. Recently, there has been significant interest in the characterization of quantum coherence as a resource, investigating how coherence…