相关论文: A witness for coherent electronic oscillations in …
The origin of the coherences in two-dimensional spectroscopy of photosynthetic complexes remains disputed. Recently it has been shown that in the ultrashort-pulse limit, oscillations in a frequency-integrated pump-probe signal correspond…
Coherent dynamics of coupled molecules are effectively characterized by the two-dimensional (2D) electronic coherent spectroscopy. Depending on the coupling between electronic and vibrational states, oscillating signals of purely…
We demonstrate that the coupling of excitonic and vibrational motion in biological complexes can provide mechanisms to explain the long-lived oscillations that have been obtained in non linear spectroscopic signals of different…
Electronic energy transfer in photosynthesis occurs over a range of time scales and under a variety of intermolecular coupling conditions. Recent work has shown that electronic coupling between chromophores can lead to coherent oscillations…
Identifying signatures of quantum coherent behaviour in photoactive systems that are maintained in stationary states away from thermal equilibrium is an open problem of wide interest in a variety of physical scenarios, including single…
The light-harvesting efficiency of a photoactive molecular complex is largely determined by the properties of its electronic quantum states. Those, in turn, are influenced by molecular vibrational states of the nuclear degrees of freedom.…
Time-resolved spectroscopies using intense THz pulses appear as a promising tool to address collective electronic excitations in condensed matter. In particular recent experiments showed the possibility to selectively excite collective…
Until recently it was believed that photosynthesis, a fundamental process for life on earth, could be fully understood with semi-classical models. However, puzzling quantum phenomena have been observed in several photosynthetic…
Two-dimensional electronic spectroscopy provides information on coupling and energy transfer between excited states on ultrafast timescales. Only recently, incoherent fluorescence detection has made it possible to combine this method with…
The prevalence of long-lasting oscillatory signals in the 2d echo-spectroscopy of light-harvesting complexes has led to a search for possible mechanisms. We investigate how two causes of oscillatory signals are intertwined: (i) electronic…
Non-equilibrium photon correlations of coherently excited single quantum systems can reveal their internal quantum dynamics and provide spectroscopic access. Here we propose and discuss the fundamentals of a coherent photon coincidence…
Multidimensional coherent optical spectroscopy is one of the most powerful tools for investigating complex quantum mechanical systems. While it was conceived decades ago in magnetic resonance spectroscopy using micro- and radio-waves, it…
The homogeneous spectral linewidth associated with light-matter interactions is a fundamental descriptor of the optical properties of materials, governed by the quantum dynamics of the condensed-matter system. We discuss here that the…
A femtosecond pump-probe setup is described that is optimised for broadband transient reflectivity experiments on solid samples over a wide range of temperatures. By combining a temporal resolution of 45 fs and a broad detection range…
Coherent collective oscillations of electrons excited in metallic nanostructures (localized surface plasmons) can confine incident light to atomic scales and enable strong light-matter interactions, which depend nonlinearly on the local…
We have previously demonstrated that in the context of two-dimensional (2D) coherent electronic spectroscopy measured by phase modulation and phase-sensitive detection, an \emph{incoherent} nonlinear response, due to pairs of…
Oscillatory signals from coherently excited phonons are regularly observed in ultrafast pump-probe experiments on condensed matter samples. Electron-phonon coupling implies that coherent phonons also modulate the electronic band structure.…
The two-dimensional spectroscopy has recently revealed oscillatory behavior of excitation dynamics in molecular systems. However, in the majority of cases it is strongly debated if excitonic or vibrational wavepackets, or evidences of…
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…
Electronic coherence is of utmost importance for the access and control of quantum-mechanical solid-state properties. Using a purely electronic observable, the photocurrent, we measure an electronic coherence time of 22 +/- 4 fs in…