Search

The predissociation dynamics of lithium iodide (LiI) in the first excited A-state is investigated for molecules in the gas phase and embedded in helium nanodroplets, using femtosecond pump-probe photoionization spectroscopy. In the gas phase, the transient Li+ and LiI+ ion signals feature damped oscillations due to the excitation and decay of a vibrational wave packet. Based on high-level ab initio calculations of the electronic structure of LiI and simulations of the wave packet dynamics, the exponential signal decay is found to result from predissociation predominantly at the lowest avoided X-A potential curve crossing, for which we infer a coupling constant V=650(20) reciprocal cm. The lack of a pump-probe delay dependence for the case of LiI embedded in helium nanodroplets indicates fast droplet-induced relaxation of the vibrational excitation.

We examine the magnetic field dependent excitations of the dimerized spin-1/2 chain, copper nitrate, with antiferromagnetic intra-dimer exchange $J_1=0.44$ meV and exchange alternation $\alpha=J_2/J_1=0.24$. Magnetic excitations in three distinct regimes of magnetization are probed through inelastic neutron scattering at low temperatures. At low and high fields there are three and two long-lived magnon-like modes, respectively. The number of modes and the anti-phase relationship between the wave-vector dependent energy and intensity of magnon scattering reflect the distinct ground states: A singlet ground state at low fields $\mu_0H < \mu_0H_{c1} = 2.8$~T and an $S_z=1/2$ product state at high fields $\mu_0H > \mu_0H_{c2} = 4.2$~T. In the intermediate field regime, a continuum of scattering for $\hbar\omega\approx J_1$ is indicative of a strongly correlated gapless quantum state without coherent magnons., Comment: 15 pages, 13 figures

Optimal control theory is a versatile tool that presents a route to significantly improving figures of merit for quantum information tasks. We combine it here with the geometric theory for local equivalence classes of two-qubit operations to derive an optimization algorithm that determines the best entangling two-qubit gate for a given physical setting. We demonstrate the power of this approach for trapped polar molecules and neutral atoms., Comment: extended version; Phys. Rev. A (2011)

Field-dependent specific heat and neutron scattering measurements were used to explore the antiferromagnetic S=1/2 chain compound CuCl2 * 2((CD3)2SO). At zero field the system acquires magnetic long-range order below TN=0.93K with an ordered moment of 0.44muB. An external field along the b-axis strengthens the zero-field magnetic order, while fields along the a- and c-axes lead to a collapse of the exchange stabilized order at mu0 Hc=6T and mu0 Hc=3.5T, respectively (for T=0.65K) and the formation of an energy gap in the excitation spectrum. We relate the field-induced gap to the presence of a staggered g-tensor and Dzyaloshinskii-Moriya interactions, which lead to effective staggered fields for magnetic fields applied along the a- and c-axes. Competition between anisotropy, inter-chain interactions and staggered fields leads to a succession of three phases as a function of field applied along the c-axis. For fields greater than mu0 Hc, we find a magnetic structure that reflects the symmetry of the staggered fields. The critical exponent, beta, of the temperature driven phase transitions are indistinguishable from those of the three-dimensional Heisenberg magnet, while measurements for transitions driven by quantum fluctuations produce larger values of beta., Comment: revtex 12 pages, 11 figures

We report magnetic susceptibility, specific heat, and neutron scattering measurements as a function of applied magnetic field and temperature to characterize the $S=1/2$ quasi-two-dimensional frustrated magnet piperazinium hexachlorodicuprate (PHCC). The experiments reveal four distinct phases. At low temperatures and fields the material forms a quantum paramagnet with a 1 meV singlet triplet gap and a magnon bandwidth of 1.7 meV. The singlet state involves multiple spin pairs some of which have negative ground state bond energies. Increasing the field at low temperatures induces three dimensional long range antiferromagnetic order at 7.5 Tesla through a continuous phase transition that can be described as magnon Bose-Einstein condensation. The phase transition to a fully polarized ferromagnetic state occurs at 37 Tesla. The ordered antiferromagnetic phase is surrounded by a renormalized classical regime. The crossover to this phase from the quantum paramagnet is marked by a distinct anomaly in the magnetic susceptibility which coincides with closure of the finite temperature singlet-triplet pseudo gap. The phase boundary between the quantum paramagnet and the Bose-Einstein condensate features a finite temperature minimum at $T=0.2$ K, which may be associated with coupling to nuclear spin or lattice degrees of freedom close to quantum criticality., Comment: Submitted to New Journal of Physics

Inelastic neutron scattering measurements are reported for a powder sample of the spin-1/2 quantum paramagnet $\rm Cu(Quinoxaline)Br_2$. Magnetic neutron scattering is identified above an energy gap of 1.9 meV. Analysis of the sharp spectral maximum at the onset indicates that the material is magnetically quasi-one-dimensional. Consideration of the wave vector dependence of the scattering and polymeric structure further identifies the material as a two-legged spin-1/2 ladder. Detailed comparison of the data to various models of magnetism in this material based on the single mode approximation and the continuous unitary transformation are presented. The latter theory provides an excellent account of the data with leg exchange $J_{\parallel}=2.0$ meV and rung exchange $J_{\perp}=3.3$ meV., Comment: 10 pages, 11 figures, 1 table

Exchange interactions between $S=\frac{1}{2}$ sites in piperazinium hexachlorodicuprate produce a frustrated bilayer magnet with a singlet ground state. We have determined the field-temperature phase diagram by high field magnetization and neutron scattering experiments. There are two quantum critical points: $H_{c1}=7.5$ T separates a quantum paramagnet phase from a three dimensional, antiferromagnetically-ordered state while $H_{c2}=37$ T marks the onset of a fully polarized state. The ordered phase, which we describe as a magnon Bose-Einstein condensate (BEC), is embedded in a quantum critical regime with short range correlations. A low temperature anomaly in the BEC phase boundary indicates that additional low energy features of the material become important near $H_{c1}$., Comment: 4 pages, 4 figures, submitted to Phys. Rev. Lett. Replaced original text with additional content

We report an experimental and theoretical study of the antiferromagnetic S=1/2 chain subject to uniform and staggered fields. Using inelastic neutron scattering, we observe a novel bound-spinon state at high energies in the linear chain compound CuCl2 * 2((CD3)2SO). The excitation is explained with a mean-field theory of interacting S=1/2 fermions and arises from the opening of a gap at the Fermi surface due to confining spinon interactions. The mean-field model also describes the wave-vector dependence of the bound-spinon states, particularly in regions where effects of the discrete lattice are important. We calculate the dynamic structure factor using exact diagonalization of finite length chains, obtaining excellent agreement with the experiments., Comment: 16 pages, 7 figures, accepted by Phys. Rev. B

Mechanically bent nickel nanowires show clear features in their room temperature magnetoresistance when a domain wall is pinned at the location of the bend. By varying the direction of an applied magnetic field, the wire can be prepared either in a single-domain state or a two-domain state. The presence or absence of the domain wall acts to shift the switching fields of the nanowire. In addition, a comparison of the magnetoresistance of the nanowire with and without a domain wall shows a shift in the resistance correlated with the presence of a wall. The resistance is decreased by 20-30 milli-Ohms when a wall is present, compared to an overall resistance of 40-60 Ohms. A model of the magnetization was developed that allowed calculation of the magnetostatic energy of the nanowires, giving an estimate for the nucleation energy of a domain wall., Comment: 11 pages, 15 figures

Inelastic neutron scattering was used to measure the magnetic field dependence of spin excitations in the antiferromagnetic S=1/2 chain CuCl_2 2(dimethylsulfoxide) (CDC) in the presence of uniform and staggered fields. Dispersive bound states emerge from a zero-field two-spinon continuum with different finite energy minima at wave numbers q=pi and q_i approx pi (1-2). The ratios of the field dependent excitation energies are in excellent agreement with predictions for breather and soliton solutions to the quantum sine-Gordon model, the proposed low-energy theory for S=1/2 chains in a staggered field. The data are also consistent with the predicted soliton and n=1,2 breather polarizations and scattering cross sections., Comment: 4 pages RevTex4, resubmitted to PRL

Measurements are reported of the magnetic field dependence of excitations in the quantum critical state of the spin S=1/2 linear chain Heisenberg antiferromagnet copper pyrazine dinitrate (CuPzN). The complete spectrum was measured at k_B T/J <= 0.025 for H=0 and H=8.7 Tesla where the system is ~30% magnetized. At H=0, the results are in quantitative agreement with exact calculations of the dynamic spin correlation function for a two-spinon continuum. At high magnetic field, there are multiple overlapping continua with incommensurate soft modes. The boundaries of these continua confirm long-standing predictions, and the intensities are consistent with exact diagonalization and Bethe Ansatz calculations., Comment: 4 pages, 4 figures

We report measurements of the two-magnon states in a dimerized antiferromagnetic chain material, copper nitrate (Cu(NO3)2*2.5D2O). Using inelastic neutron scattering we have measured the one and two magnon excitation spectra in a large single crystal. The data are in excellent agreement with a perturbative expansion of the alternating Heisenberg Hamiltonian from the strongly dimerized limit. The expansion predicts a two-magnon bound state for q ~ (2n+1)pi*d which is consistent with the neutron scattering data., Comment: 11 pages of revtex style with 6 figures included

Inelastic neutron scattering measurements are reported for the quantum antiferromagnetic material Cu_2(C_5H_12N_2)_2Cl_4 (CuHpCl). The magnetic excitation spectrum forms a band extending from 0.9 meV to 1.4 meV. The spectrum contains two modes that disperse throughout the a-c plane of the monoclinic unit cell with less dispersion along the unique b-axis. Simple arguments based on the measured dispersion relations and the crystal structure show that a spin ladder model is inappropriate for describing CuHpCl. Instead, it is proposed that hydrogen bond mediated exchange interactions between the bi-nuclear molecular units yield a three-dimensional interacting spin system with a recurrent triangular motif similar to the Shastry-Sutherland Model (SSM). Model independent analysis based on the first moment sum rule shows that at least four distinct spin pairs are strongly correlated and that two of these, including the dimer bond of the corresponding SSM, are magnetically frustrated. These results show that CuHpCl should be classified as a frustration induced three dimensional quantum spin liquid., Comment: 13 pages, 17 figures (Color) ReSubmitted to Phys. Rev. B 9/21/2001 resubmission has new content email comments to dhr@pha.jhu.edu or mstone@pha.jhu.edu