Biomedical subjects

Seogjoo Jang

Publications and source records attributed to Seogjoo Jang.

4 recordsLinked to original sources

PubMed2006

Closed-form expressions of quantum electron transfer rate based on the stationary-phase approximation.

Closed-form rate expressions are derived on the basis of the stationary-phase approximation for the Fermi golden rule expression of the quantum electron-transfer (ET) rate. First, on the basis of approximate solutions of the stationary-phase points near DeltaG = 0, -lambda, and lambda, where DeltaG is the reaction free energy and lambda is the reorganization energy, three closed-form rate expressions are derived, which are respectively valid near each value of DeltaG. Numerical tests for a model Ohmic spectral density with an exponential cutoff demonstrate good performance of the derived expressions in the respective regions of their validity. In particular, the expression near DeltaG = -lambda, which differs from the semiclassical approximation only by a prefactor quadratic in DeltaG, works substantially better than the latter. Then, a unified formula is suggested, which interpolates the three approximate expressions and serves as a good approximation in all three regions. We have also demonstrated that the interpolation formula can serve as a good quantitative means for understanding the temperature dependence of the quantum ET rate.

Journal Article↗

PubMed2006

Path-integral centroid dynamics for general initial conditions: a nonequilibrium projection operator formulation.

The formulation of path-integral centroid dynamics is extended to the quantum dynamics of density operators evolving from general initial states by means of the nonequilibrium projection operator technique. It is shown that the new formulation provides a basis for applying the method of centroid dynamics to nonequilibrium situations and that it allows the derivation of new formal relations, which can be useful in improving current equilibrium centroid dynamics methods. A simple approximation of uniform relaxation for the unprojected portion of the Liouville space propagator leads to a class of practically solvable equations of motion for the centroid variables, but with an undetermined parameter of relaxation. This new class of equations encompasses the centroid molecular-dynamics (CMD) method as a limiting case, and can be applied to both equilibrium and nonequilibrium situations. Tests for the equilibrium dynamics of one-dimensional model systems demonstrate that the new equations with appropriate choice of the relaxation parameter are comparable to the CMD method.

Journal Article↗

PubMed2005

Theory of torsional non-Condon electron transfer: a generalized spin-boson Hamiltonian and its nonadiabatic limit solution.

The paper develops a theory of electron transfer with torsionally induced non-Condon (NC) effects. The starting point of the theory is a generalized spin-boson Hamiltonian, where an additional torsional oscillator bilinearly coupled to other bath modes causes a sinusoidal NC modulation. We derive closed form time dependent nonadiabatic rate expressions for both sudden and relaxed initial conditions, which are applicable for general spectral densities and energetic condition. Under the assumption that the torsional motion is not correlated with the polaronic shift of the bath, simple stationary limit rate expression is obtained. Model calculations of this rate expression illustrate the effects of torsional quantization and gating on the driving force and temperature dependences of the electron transfer rate. The classical limit of the rate expression consists of three Marcus-type terms, and is shown to agree very well with the exact numerical result.

Journal Article↗

PubMed2004

Multichromophoric Förster resonance energy transfer.

The theory of Förster resonance energy transfer is generalized for multichromophoric (MC) and nonequilibrium situations. For the first time, it is clarified that the far-field linear spectroscopic information is insufficient for the determination of the reaction rate and that distance dependence of the rate can vary with the disorder and temperature. Application to a light harvesting complex LH2 reveals the important consequences of a MC structure.

Fluorescence Resonance Energy Transfer↗