Parity forbidden excitations of Sr2CuO2Cl2 revealed by optical third-harmonic spectroscopy

We present the first study of nonlinear optical third harmonic generation in the strongly correlated charge-transfer insulator Sr2CuO2Cl2. For fundamental excitation in the near-infrared, the THG spectrum reveals a strongly resonant response for photon energies near 0.7 eV. Polarization analysis reveals this novel resonance to be only partially accounted for by three-photon excitation to the optical charge-transfer exciton, and indicates that an even-parity excitation at 2 eV, with a_1g symmetry, participates in the third harmonic susceptibility.Comment: Requires RevTeX v4.0beta

Photon-energy dissipation caused by an external electric circuit in "virtual" photo-excitation processes

We consider generation of an electrical pulse by an optical pulse in the ``virtual excitation'' regime. The electronic system, which is any electro-optic material including a quantum well structure biased by a dc electric field, is assumed to be coupled to an external circuit. It is found that the photon frequency is subject to an extra red shift in addition to the usual self-phase modulation, whereas the photon number is conserved. The Joule energy consumed in the external circuit is supplied only from the extra red shift.Comment: 4 pages, 1 fugur

Photonic crystals of coated metallic spheres

It is shown that simple face-centered-cubic (fcc) structures of both metallic and coated metallic spheres are ideal candidates to achieve a tunable complete photonic bandgap (CPBG) for optical wavelengths using currently available experimental techniques. For coated microspheres with the coating width to plasma wavelength ratio $l_c/\lambda_p \leq 10$ and the coating and host refractive indices $n_c$ and $n_h$, respectively, between 1 and 1.47, one can always find a sphere radius $r_s$ such that the relative gap width $g_w$ (gap width to the midgap frequency ratio) is larger than 5% and, in some cases, $g_w$ can exceed 9%. Using different coatings and supporting liquids, the width and midgap frequency of a CPBG can be tuned considerably.Comment: 14 pages, plain latex, 3 ps figures, to appear in Europhys. Lett. For more info on this subject see http://www.amolf.nl/research/photonic_materials_theory/moroz/moroz.htm

Collective oscillations driven by correlation in the nonlinear optical regime

We present an analytical and numerical study of the coherent exciton polarization including exciton-exciton correlation. The time evolution after excitation with ultrashort optical pulses can be divided into a slowly varying polarization component and novel ultrafast collective modes. The frequency and damping of the collective modes are determined by the high-frequency properties of the retarded two-exciton correlation function, which includes Coulomb effects beyond the mean-field approximation. The overall time evolution depends on the low-frequency spectral behavior. The collective mode, well separated from the slower coherent density evolution, manifests itself in the coherent emission of a resonantly excited excitonic system, as demonstrated numerically.Comment: 4 pages, 4 figures, accepted for publication in Physical Review Letter

Kinetic and structural mechanism for DNA unwinding by a non-hexameric helicase

UvrD, a model for non-hexameric Superfamily 1 helicases, utilizes ATP hydrolysis to translocate stepwise along single-stranded DNA and unwind the duplex. Previous estimates of its step size have been indirect, and a consensus on its stepping mechanism is lacking. To dissect the mechanism underlying DNA unwinding, we use optical tweezers to measure directly the stepping behavior of UvrD as it processes a DNA hairpin and show that UvrD exhibits a variable step size averaging ~3 base pairs. Analyzing stepping kinetics across ATP reveals the type and number of catalytic events that occur with different step sizes. These single-molecule data reveal a mechanism in which UvrD moves one base pair at a time but sequesters the nascent single strands, releasing them non-uniformly after a variable number of catalytic cycles. Molecular dynamics simulations point to a structural basis for this behavior, identifying the protein-DNA interactions responsible for strand sequestration. Based on structural and sequence alignment data, we propose that this stepping mechanism may be conserved among other non-hexameric helicases

Photocarrier relaxation in the quantum kinetics regime

We present a study of carrier relaxation in GaAs in the quantum- kinetics regime. The results cannot be explained by Bolzmann kinetics. They are in satisfactory agreement with quantum-kinetic theory calculation of the occupation number in k-space

Radiative corrections to the excitonic molecule state in GaAs microcavities

The optical properties of excitonic molecules (XXs) in GaAs-based quantum well microcavities (MCs) are studied, both theoretically and experimentally. We show that the radiative corrections to the XX state, the Lamb shift $\Delta^{\rm MC}_{\rm XX}$ and radiative width $\Gamma^{\rm MC}_{\rm XX}$, are large, about $10-30$ of the molecule binding energy $\epsilon_{\rm XX}$, and definitely cannot be neglected. The optics of excitonic molecules is dominated by the in-plane resonant dissociation of the molecules into outgoing 1$\lambda$-mode and 0$\lambda$-mode cavity polaritons. The later decay channel, ``excitonic molecule $\to$ 0$\lambda$-mode polariton + 0$\lambda$-mode polariton'', deals with the short-wavelength MC polaritons invisible in standard optical experiments, i.e., refers to ``hidden'' optics of microcavities. By using transient four-wave mixing and pump-probe spectroscopies, we infer that the radiative width, associated with excitonic molecules of the binding energy $\epsilon_{\rm XX} \simeq 0.9-1.1$ meV, is $\Gamma^{\rm MC}_{\rm XX} \simeq 0.2-0.3$ meV in the microcavities and $\Gamma^{\rm QW}_{\rm XX} \simeq 0.1$ meV in a reference GaAs single quantum well (QW). We show that for our high-quality quasi-two-dimensional nanostructures the $T_2 = 2 T_1$ limit, relevant to the XX states, holds at temperatures below 10 K, and that the bipolariton model of excitonic molecules explains quantitatively and self-consistently the measured XX radiative widths. We also find and characterize two critical points in the dependence of the radiative corrections against the microcavity detuning, and propose to use the critical points for high-precision measurements of the molecule bindingenergy and microcavity Rabi splitting.Comment: 16 pages, 11 figures, accepted for publication in Phys. Rev.

Decoherence-Free Subspaces for Multiple-Qubit Errors: (I) Characterization

Coherence in an open quantum system is degraded through its interaction with a bath. This decoherence can be avoided by restricting the dynamics of the system to special decoherence-free subspaces. These subspaces are usually constructed under the assumption of spatially symmetric system-bath coupling. Here we show that decoherence-free subspaces may appear without spatial symmetry. Instead, we consider a model of system-bath interactions in which to first order only multiple-qubit coupling to the bath is present, with single-qubit system-bath coupling absent. We derive necessary and sufficient conditions for the appearance of decoherence-free states in this model, and give a number of examples. In a sequel paper we show how to perform universal and fault tolerant quantum computation on the decoherence-free subspaces considered in this paper.Comment: 18 pages, no figures. Major changes. Section on universal fault tolerant computation removed. This section contained a crucial error. A new paper [quant-ph/0007013] presents the correct analysi