Quantum trajectory simulations of the fluorescence intensity from a two-level atom driven by a multichromatic field

The quantum trajectories method is illustrated for the resonance fluorescence of a two-level atom driven by a multichromatic field. We discuss the method for the time evolution of the fluorescence intensity in the presence of bichromatic and trichromatic driving fields. We consider the special case wherein one multichromatic field component is strong and resonant with the atomic transition whereas the other components are much weaker and arbitrarily detuned from the atomic resonance. We find that the phase-dependent modulations of the Rabi oscillations, recently observed experimentally [Q. Wu, D. J. Gauthier, and T. W. Mossberg, Phys. Rev. A 49, R1519 (1994)] for the special case when the weaker component of a bichromatic driving field is detuned from the atomic resonance by the strong-field Rabi frequency, appear also for detunings close to the subharmonics of the Rabi frequency. Furthermore, we show that for the atom initially prepared in one of the dressed states of the strong field component the modulations are not sensitive to the phase. We extend the calculations to the case of a trichromatic driving field and find that apart from the modulations of the amplitude there is a modulation of the frequency of the Rabi oscillations. Moreover, the time evolution of the fluorescence intensity depends on the phase regardless of the initial conditions and a phase-dependent suppression of the Rabi oscillations can be observed when the sideband fields are tuned to the subharmonics of the strong-field Rabi frequency. [S1050-2947(98)03501-X].

Anomalous fluorescence spectra in an extremely weak, broadband squeezed vacuum under monochromatic and bichromatic excitation

We show that a two-level atom interacting with an extremely weak squeezed vacuum can display resonance fluorescence spectra that are qualitatively different to those that can be obtained using fields with a classical analogue. We consider first the free space situation with monochromatic excitation, and then discuss a bichromatically driven two-level atom in a cavity as a practical scenario for experimentally detecting the anomalous features predicted. We show that in the bad cavity limit, the anomalous spectral features appear for a weak squeezed vacuum and large frequency differences of the bichromatic field, conditions which are easily accessible in laboratories. The advantage of bichromatic, as opposed to monochromatic, excitation is that there is no coherent scattering at line centre which could obscure the observations. A scaling law is derived, N similar to Omega(4) which relates the squeezed photon number to the Rabi frequency at which the anomalous features appear. (C) 1998 Elsevier Science B.V.

Analytical solution for the Mollow and Autler-Townes probe absorption spectra of a three-level atom in a squeezed vacuum

The Mellow and Autler-Townes probe absorption spectra of a three-level atom in a cascade configuration with the lower transition coherently driven and also coupled to a narrow bandwidth squeezed-vacuum field are studied. Analytical studies of the modifications caused by the finite squeezed-vacuum bandwidth to the spectra are made for the case when the Rabi frequency of the driving field is much larger than the natural linewidth. The squeezed vacuum center frequency and the driving laser frequency are assumed equal. We show that the spectral features depend on the bandwidth of a squeezed vacuum field and whether the sources of the squeezing field are degenerate (DPA) or nondegenerate (NDPA) parametric amplifiers. In a broadband or narrow bandwidth squeezed vacuum generated by a NDPA, the central component of the Mellow spectrum can be significantly narrower than that in the normal vacuum. When the source of the squeezed vacuum is a DPA, the central feature is insensitive to squeezing. The Rabi sidebands, however, can be significantly narrowed only in the squeezed vacuum produced by the DPA. The two lines of the Autler-Townes absorption spectrum can be narrowed only in a narrow bandwidth squeezed vacuum, whereas they are independent of the phase and are always broadened in a broadband squeezed vacuum.

Iron(III) and iron(II) complexes of 1-thia-4,7-diazacyclononane ([9]aneN(2)S) and 1,4-dithia-7-azacyclononane ([9]aneNS(2)). X-Ray structural analyses, magnetic susceptibility, Mossbauer, EPR and electronic spectroscopy

The complexes [Fe([9]aneN(2)S)(2)][ClO4](2), [Fe([9]aneN(2)S)(2)][ClO4](3) and [Fe([9]aneNS(2))(2)][ClO4](2) ([9]aneN(2)S = 1-thia-4. 7-diazacyclononane and [9]aneNS(2) = 1,4-dithia-7-azacyclononane) have been prepared and the latter two characterised by X-ray crystallography. The Mossbauer spectra (isomer shift/mm s(-1), quadrupole splitting/mm s(-1), 4.2 K) for [Fe([9]aneN(2)S)(2)][ClO4](2) (0.52, 0.57), [Fe([9]aneN(2)S)(2)][ClO4](3) (0.25, 2.72) and [Fe([9]aneNS(2))(2)][ClO4](2) (0.43, 0.28) are typical for iron(II) and iron(III) complexes. Variable-temperature susceptibility measurements for [Fe([9]aneN(2)S)(2)][ClO4](2) (2-300 K) revealed temperature-dependent behaviour in both the solid state [2.95 mu(B) (300 K)-0.5 mu(B) (4.2 K)] and solution (Delta H degrees 20-22 kJ mol(-1), Delta S degrees 53-60 J mol(-1) K-1). For [Fe([9]aneN(2)S)(2)][ClO4](3) in the solid state [2.3 mu(B) (300 K)-1.9 mu(B) (4.2 K)] the magnetic data were fit to a simple model (H = -lambda L . S + mu L-z) to give the spin-orbit coupling constant (lambda) of -260 +/- 10 cm(-1). The solid-state X-band EPR spectrum of [Fe([9]aneN(2)S)(2)][ClO4](3) revealed axial symmetry (g(perpendicular to) = 2.607, g(parallel to) = 1.599). Resolution of g(perpendicular to) into two components at Q-band frequencies indicated a rhombic distortion. The low-temperature single-crystal absorption spectra of [Fe([9]aneN(2)S)(2)][ClO4](2) and [Fe([9]aneNS(2))(2)][ClO4](2) exhibited additional bands which resembled pseudotetragonal low-symmetry splitting of the parent octahedral (1)A(1g) --> T-1(2g) and (1)A(1g) ---> T-1(1g) transitions. However, the magnitude of these splittings was too large, requiring 10Dq for the thioether donors to be significantly larger than for the amine donors. Instead, these bands were tentatively assigned to weak, low-energy S --> Fe-II charge-transfer transitions. Above 200 K, thermal occupation of the high-spin T-5(2g) ground state resulted in observation of the T-5(2g) --> E-5(g) transition in the crystal spectrum of [Fe([9]aneN(2)S)(2)][ClO4](2). From a temperature-dependence study, the separation of the low-spin (1)A(1g) and high-spin T-5(2g) ground states was approximately 1700 cm(-1). The spectrum of the iron(III) complex [Fe([9]aneN(2)S)(2)][ClO4](3) is consistent with a low-spin d(5) configuration.

Shift of the subharmonic resonances and suppression of fluorescence in a two-level atom driven by a bichromatic field

We study the behavior of a two-level atom that is driven by a bichromatic field consisting of a strong resonant component and a weaker tunable component. In addition to the splitting of the energy levels (the multiphoton AC Stark effect), we find that the weaker component also shifts the subharmonic resonances, an effect we attribute to a dynamic Stark shift. When the weaker component is tuned to a shifted resonance, no fluorescence occurs at either the frequency of the strong component or the three-photon mixing frequency. Results are obtained with numerical techniques and explained in terms of the dressed-atom model of the system. (C) 1998 Optical Society of America [S0740-3224(98)01508-2] OCIS codes: 270.4180, 270.6620, 270.0270.

Resonance fluorescence spectrum in a weak squeezed field with an arbitrary bandwidth

We analyze the linewidth narrowing in the fluorescence spectrum of a two-level atom driven by a squeezed vacuum field of a finite bandwidth. It is found that the fluorescence spectrum in a low-intensity squeezed field can exhibit a (omega - omega(0))(-6) frequency dependence in the wings. We show that this fast fall-off behavior is intimately related to the properties of a narrow-bandwidth squeezed field and does not extend into the region of broadband excitation. We apply the Linear response model and find that the narrowing results from a convolution of the atom response with the spectrum of the incident field. On the experimental side, we emphasize that the linewidth narrowing is not sensitive to the solid angle of the squeezed modes coupled to the atom. We also compare the fluorescence spectrum with the quadrature-noise spectrum and find that the fluorescence spectrum for an off-resonance excitation does not reveal the noise spectrum. We show that this difference arises from the competing three-photon scattering processes. [S1050-2947(98)04308-X].

Interference pattern with a dark center in resonance fluorescence from two atoms driven by a squeezed vacuum field

We study the resonance fluorescence from two interacting atoms driven by a squeezed vacuum field and show that this system produces an interference pattern with a dark center. We discuss the role of the interatomic interactions in this process and find that the interference pattern results from an unequal population of the symmetric and antisymmetric states of the two-atom system. We also identify intrinsically nonclassical effects versus classical squeezed field effects, (C) 1998 Elsevier Science B.V. All rights reserved.

Phosphorylation of the C-terminal sites of human p53 reduces non-sequence-specific DNA binding as modeled with synthetic peptides

Phosphorylation of the tumor suppressor p53 is generally thought to modify the properties of the protein in four of its five independent domains. We used synthetic peptides to directly study the effects of phosphorylation on the non-sequence-specific DNA binding and conformation of the C-terminal, basic domain. The peptides corresponded to amino acids 361-393 and were either nonphosphorylated or phosphorylated at the protein kinase C (PKC) site, Ser378, or the casein kinase II (CKII) site, Ser392, or bis-phosphorylated on both the PKC and the CKII sites. A fluorescence polarization analysis revealed that either the recombinant p53 protein or the synthetic peptides bound to two unrelated target DNA fragments. Phosphorylation of the peptide at the PKC or the CKII sites clearly decreased DNA binding, and addition of a second phosphate group almost completely abolished binding. Circular dichroism spectroscopy showed that the peptides assumed identical unordered structures in aqueous solutions. The unmodified peptide, unlike the Ser378 phosphorylated peptide, changed conformation in the presence of DNA. The inherent ability of the peptides to form an alpha-helix could be detected when circular dichroism and nuclear magnetic resonance spectra were: taken in trifluoroethanol-water mixtures. A single or double phosphorylation destabilized the helix around the phosphorylated Ser378 residue but stabilized the helix downstream in the sequence.

Three-dimensional solution structure of alpha-conotoxin MII by NMR spectroscopy: Effects of solution environment on helicity

alpha-Conotoxin MII, a 16-residue polypeptide from the venom of the piscivorous cone snail Conus magus, is a potent and highly specific blocker of mammalian neuronal nicotinic acetylcholine receptors composed of alpha 3 beta 2 subunits. The role of this receptor type in the modulation of neurotransmitter release and its relevance to the problems of addiction and psychosis emphasize the importance of a structural understanding of the mode of interaction of MII with the alpha 3 beta 2 interface. Here we describe the three-dimensional solution structure of MIT determined using 2D H-1 NMR spectroscopy. Structural restraints consisting of 376 interproton distances inferred from NOEs and 12 dihedral restraints derived from spin-spin coupling constants were used as input for simulated annealing calculations and energy minimization in the program X-PLOR. The final set of 20 structures is exceptionally well-defined with mean pairwise rms differences over the whole molecule of 0.07 Angstrom for the backbone atoms and 0.34 Angstrom for all heavy atoms. MII adopts a compact structure incorporating a central segment of alpha-helix and beta-turns at the N- and C-termini. The molecule is stabilized by two disulfide bonds, which provide cross-links between the N-terminus and both the middle and C-terminus of the structure. The susceptibility of the structure to conformational change was examined using several different solvent conditions. While the global fold of MII remains the same, the structure is stabilized in a more hydrophobic environment provided by the addition of acetonitrile or trifluoroethanol to the aqueous solution. The distribution of amino acid side chains in MII creates distinct hydrophobic and polar patches on its surface that may be important for the specific interaction with the alpha 3 beta 2 neuronal nAChR. A comparison of the structure of MII with other neuronal-specific alpha-conotoxins provides insights into their mode of interaction with these receptors.

The solution structure of a copper(II) compound of a new cyclic octapeptide by EPR spectroscopy and force field calculations

A new cyclic octapeptide, cyclo(Ile-Ser-(Gly)Thz-Ile-Thr-(Gly)Thz) (PatN), related to patellamide A, has been synthesized and reacted with copper(II) and base to form mono- and dinuclear complexes. The coordination environments around copper(TI) have been characterized by EPR spectroscopy. The solution structure of the thermodynamically most stable product, a purple dicopper(TI) compound, has been examined by simulating weakly dipole-dipole coupled EPR spectra based upon structural parameters obtained from force field (MM and MD) calculations. The MM-EPR method produces a saddle-shaped structure for [Cu-2(PatN)(OH2)(6)] that is similar to the known solution structure of patellamide A and the known solid-state structure of [Cu-2(AscidH(2))CO3(OH2)(2)]. Compared with the latter, [Cu-2(PatN)] has no carbonate bridge and a significantly flatter topology. The MM-EPR approach to solution-structure determination for paramagnetic metallopeptides may find wide applications to other metallopeptides and metalloproteins.

Atoms in squeezed light fields

Squeezed light is of interest as an example of a non-classical state of the electromagnetic field and because of its applications both in technology and in fundamental quantum physics. This review concentrates on one aspect of squeezed light, namely its application in atomic spectroscopy. The general properties, detection and application of squeezed light are first reviewed. The basic features of the main theoretical methods (master equations, quantum Langevin equations, coupled systems) used to treat squeezed light spectroscopy are then outlined. The physics of squeezed light interactions with atomic systems is dealt with first for the simpler case of two-level atoms and then for the more complex situation of multi-level atoms and multi-atom systems. Finally the specific applications of squeezed light spectroscopy are reviewed.

Synthesis of [Cu-2(Me-2[9]aneN(2)S)(2)(OH)(2)] (PF6)(2), a hydroxo-bridged copper(II) complex of N,N '-dimethyl-1-thia-4,7-diazacyclononane (Me-2[9]aneN(2)S). X-ray structural analysis, magnetic susceptibility, EPR and visible spectroscopy

The bis(mu-hydroxo) complex [Cu-2(Me-2[9]aneN(2)S)(2)(OH)(2)](PF6)(2) (Me-2[9]aneN(2)S = N,N'-dimethyl-1-thia-4,7-diazacyclononane) results after reaction of [Cu(Me-2[9]aneN(2)S)(MeCN)] (PF6) with dioxygen at -78 degrees C in acetonitrile. The complex has been characterized by X-ray crystallography: orthorhombic, space group Pnma, with a 18.710(3), b 16.758(2), c 9.593(2) Angstrom, and Z = 4. The structure refined to a final R value of 0.051. The complex contains two copper(II) ions bridged by two hydroxo groups with Cu ... Cu 2.866(1) Angstrom. The solid-state magnetic susceptibility study reveals ferromagnetic coupling, the fitting parameters being J = +46+/-5 cm(-1), g = 2.01+/-0.01 and theta = -0.58+/-0.03 K. The frozen-solution e.p.r. spectrum in dimethyl sulfoxide is characteristic of a monomeric copper(II) ion (g(parallel to) 2.300, g(perpendicular to) 2.063; A(parallel to) 156.2 x 10(-4) cm(-1), A(perpendicular to) 9.0 x 10(-4) cm(-1)) with an N2O2 donor set. Thioether coordination to the copper(II) in solution is supported by the presence of an intense absorption assigned to a sigma(S)-->Cu-II LMCT transition at c. 34000 cm(-1). The single-crystal spectrum of [Cu-2(Me-2[9]aneN(2)S)(2)(OH)(2)] (PF6)(2) (273 K) reveals d-->d transitions at 14500 and 18300 cm(-1) and a weak pi(S)-->Cu-II charge-transfer band at approximately 25000 cm(-1).

Detection of dimethyl sulfone in the human brain by in vivo proton magnetic resonance spectroscopy

We wish to report the detection of dimethyl sulfone (methylsulfonylmethane, C2H6O2S) in the brain of a normal 62-year-old male using in vivo proton magnetic resonance spectroscopy. The presence of this exogenous metabolite resulted from ingestion of a dietary supplement containing dimethyl sulfone. The concentration of this compound in the brain was measured to be 2.4 mmol, with a washout half life of approximately 7.5 days. The in vivo T-1 and T-2 relaxation times of dimethyl sulfone were measured to be 2180 ms and 385 ms, respectively. The concentration of major brain metabolites, namely N-acetylaspartate, total Creatine and Choline, and myo-Inositol were within normal limits. (C) 2000 Elsevier Science Inc. All rights reserved.

Characterization of the sequential non-covalent and covalent interactions of the antitumour antibiotic hedamycin with double stranded DNA by NMR spectroscopy

Hedamycin, a member of the pluramycin class of antitumour antibiotics, consists of a planar anthrapyrantrione chromophore to which is attached two aminosugar rings at one end and a bisepoxide-containing sidechain at the other end, Binding to double-stranded DNA is known to involve both reversible and non-reversible modes of interaction. As a part of studies directed towards elucidating the structural basis for the observed 5'-pyGT-3' sequence selectivity of hedamycin, we conducted one-dimensional NMR titration experiments at low temperature using the hexadeoxyribonucleotide duplexes d(CACGTG)(2) and d(CGTACG)(2). Spectral changes which occurred during these titrations are consistent with hedamycin initially forming a reversible complex in slow exchange on the NMR timescale and binding through intercalation of the chromophore. Monitoring of this reversible complex over a period of hours revealed a second type of spectral change which corresponds with formation of a non-reversible complex. Copyright (C) 1999 John Wiley & Sons, Ltd.