We present a theoretical study of noise-induced quantum coherences in a model three-level V-type system interacting with incoherent radiation, an important prototype for a wide range of physical systems ranging from trapped ions to biomolecules and quantum dots. By solving the quantum optical equations of motion, we obtain analytic expressions for the noise-induced coherences and show that they exhibit an oscillating behavior in the limit of large excited level spacing Δ (Δ/γ≫1, where γ is the radiative decay width). Most remarkably, we find that in the opposite limit of small level spacing Δ/γ≪1, appropriate for large molecules, (a) the coherences can survive for an extremely long time τ=(2/γ)(Δ/γ)^{-2} before eventually decaying to zero, and (b) coherences at short times can be substantial. We further show that the long-lived coherences can survive environmental relaxation and decoherence, suggesting implications to the design of quantum heat engines and to incoherent light excitation of biological systems.

We present a theoretical study of atom-molecule collisions in superimposed electric and magnetic fields and show that dynamics of electronic spin relaxation in molecules at temperatures below 0.5 K can be manipulated by varying the strength and the relative orientation of the applied fields. The mechanism of electric field control of Zeeman transitions is based on an intricate interplay between intramolecular spin-rotation couplings and molecule-field interactions. We suggest that electric fields may affect chemical reactions through inducing nonadiabatic spin transitions and facilitate evaporative cooling of molecules in a magnetic trap.

Closed-form analytic solutions to non-secular Bloch-Redfield master equations for quantum dynamics of a V-type system driven by weak coupling to a thermal bath, relevant to light harvesting processes, are obtained and discussed. We focus on noise-induced Fano coherences among the excited states induced by incoherent driving of the V-system initially in the ground state. For suddenly turned-on incoherent driving, the time evolution of the coherences is determined by the damping parameter ζ=12(γ1+γ2)/Δp, where γi are the radiative decay rates of the excited levels i = 1, 2, and Δp=Δ(2)+(1-p(2))γ1γ2 depends on the excited-state level splitting Δ > 0 and the angle between the transition dipole moments in the energy basis. The coherences oscillate as a function of time in the underdamped limit (ζ ≫ 1), approach a long-lived quasi-steady state in the overdamped limit (ζ ≪ 1), and display an intermediate behavior at critical damping (ζ = 1). The sudden incoherent turn-on is shown to generate a mixture of excited eigenstates |e1〉 and |e2〉 and their in-phase coherent superposition |ϕ+〉=1r1+r2(r1|e1〉+r2|e2〉), which is remarkably long-lived in the overdamped limit (where r1 and r2 are the incoherent pumping rates). Formation of this coherent superposition enhances the decay rate from the excited states to the ground state. In the strongly asymmetric V-system where the coupling strengths between the ground state and the excited states differ significantly, additional asymptotic quasistationary coherences are identified, which arise due to slow equilibration of one of the excited states. Finally, we demonstrate that noise-induced Fano coherences are maximized with respect to populations when r1 = r2 and the transition dipole moments are fully aligned.

The Harvard community has made this article openly available. Please share how this access benefits you. Your story matters. An efficient method is presented for rigorous quantum calculations of atom-molecule and molecule-molecule collisions in a magnetic field. The method is based on the expansion of the wave function of the collision complex in basis functions with well-defined total angular momentum in the body-fixed coordinate frame. We outline the general theory of the method for collisions of diatomic molecules in the 2 ⌺ and 3 ⌺ electronic states with structureless atoms and with unlike 2 ⌺ and 3 ⌺ molecules. The cross sections for elastic scattering and Zeeman relaxation in low-temperature collisions of CaH͑ 2 ⌺ + ͒ and NH͑ 3 ⌺ − ͒ molecules with 3 He atoms converge quickly with respect to the number of total angular momentum states included in the basis set, leading to a dramatic ͑Ͼ10-fold͒ enhancement in computational efficiency compared to the previously used methods ͓A. Volpi and J. L. Bohn, Phys. Rev. A 65, 052712 ͑2002͒; R. V. Krems and A. Dalgarno, J. Chem. Phys. 120, 2296 ͑2004͔͒. Our approach is thus well suited for theoretical studies of strongly anisotropic molecular collisions in the presence of external electromagnetic fields.