اشترك بالحزمة الذهبية واحصل على وصول غير محدود شمرا أكاديميا
تسجيل مستخدم جديدLinear, third- and fifth-order nonlinear spectroscopy of a charge transfer system coupled to an underdamped vibration
204
0
0.0
(
0
)
اسأل ChatGPT حول البحث
ﻻ يوجد ملخص باللغة العربية
We study hole, electron and exciton transport in a charge transfer system in the presence of underdamped vibrational motion. We analyze the signature of these processes in the linear and third-, and fifth-order nonlinear electronic spectra. Calculations are performed with a numerically exact hierarchical equations of motion method for an underdamped Brownian oscillator spectral density. We find that combining electron, hole and exciton transfer can lead to non-trivial spectra with more structure than with excitonic coupling alone. Traces taken during the waiting time of a two-dimensional spectrum are dominated by vibrational motion and do not reflect the electron, hole, and exciton dynamics directly. We find that the fifth-order nonlinear response is particularly sensitive to the charge transfer process. While third-order 2D spectroscopy detects the correlation between two coherences, fifth-order 2D spectroscopy (2D population spectroscopy) is here designed to detect correlations between the excited states during two different time periods.
قيم البحث
اقرأ أيضاً
We report nonlinear vibration localisation in a system of two symmetric weakly coupled nonlinear oscillators. A two degree-of-freedom model with piecewise linear stiffness shows bifurcations to localised solutions. An experimental investigation emplo
ying two weakly coupled beams touching against stoppers for large vibration amplitudes confirms the nonlinear localisation.
We investigate photoinduced proton-coupled electron transfer (PI-PCET) reaction through a recently devel- oped quasi-diabatic (QD) quantum dynamics propagation scheme. This scheme enables interfacing accurate diabatic-based quantum dynamics approache
s with adiabatic electronic structure calculations for on-the-fly simulations. Here, we use the QD scheme to directly propagate PI-PCET quantum dynamics with the di- abatic Partial Linearized Density Matrix (PLDM) path-integral approach with the instantaneous adiabatic electron-proton vibronic states. Our numerical results demonstrate the importance of treating proton quan- tum mechanically in order to obtain accurate PI-PCET dynamics, as well as the role of solvent fluctuation and vibrational relaxation on proton tunneling in various reaction regimes that exhibit different kinetic iso- tope effects. This work opens the possibility to study the challenging PI-PCET reactions through accurate diabatic quantum dynamics approaches combined with efficient adiabatic electronic structure calculations.
An experimental setup of three coupled $mathcal{PT}$-symmetric wave guides showing the characteristics of a third-order exceptional point (EP3) has been investigated in an idealized model of three delta-functions wave guides in W.~D. Heiss and G.~Wun
ner, J. Phys. A 49, 495303 (2016). Here we extend these investigations to realistic, extended wave guide systems. We place major focus on the strong parameter sensitivity rendering the discovery of an EP3 a challenging task. We also investigate the vicinity of the EP3 for further branch points of either cubic or square root type behavior.
We investigate the quantum dynamics of energy and charge transfer in a wheel-shaped artificial photosynthetic antenna-reaction center complex.This complex consists of six light-harvesting chromophores and an electron-acceptor fullerene. To describe q
uantum effects on a femtosecond time scale, we derive the set of exact non-Markovian equations for the Heisenberg operators of this photosynthetic complex in contact with a Gaussian heat bath. With these equations we can analyze the regime of strong system-bath interactions, where reorganization energies are of the order of the intersite exciton couplings. We show that the energy of the initially-excited antenna chromophores is efficiently funneled to the porphyrin-fullerene reaction center, where a charge-separated state is set up in a few picoseconds, with a quantum yield of the order of 95%. In the single-exciton regime, with one antenna chromophore being initially excited, we observe quantum beatings of energy between two resonant antenna chromophores with a decoherence time of $sim$ 100 fs. We also analyze the double-exciton regime, when two porphyrin molecules involved in the reaction center are initially excited. In this regime we obtain pronounced quantum oscillations of the charge on the fullerene molecule with a decoherence time of about 20 fs (at liquid nitrogen temperatures). These results show a way to directly detect quantum effects in artificial photosynthetic systems.
When the nonlinearity of nanomechanical resonator is not negligible, the quantum decoherence of charge qubit is studied analytically. Using nonlinear Jaynes-Cummings model, one explores the possibility of being quantum data bus for nonlinear nanomech
anical resonator, the nonlinearity destroys the dynamical quantum information-storage and maintains the revival of quantum coherence of charge qubit. With the calculation of decoherence factor, we demonstrate the influence of the nonlinearity of nanomechanical resonator on engineered decoherence of charge qubit.
سجل دخول لتتمكن من نشر تعليقات
التعليقات
جاري جلب التعليقات
سجل دخول لتتمكن من متابعة معايير البحث التي قمت باختيارها
