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Probing the structure and dynamics of molecular clusters using rotational wavepackets  [PDF]
Gediminas Galinis,Cephise Cacho,Richard T. Chapman,Andrew M. Ellis,Marius Lewerenz,Luis G. Mendoza Luna,Russell S. Minns,Mirjana Mladenovic,Arnaud Rouzée,Emma Springate,I. C. Edmond Turcu,Mark J. Watkins,Klaus von Haeften
Physics , 2014, DOI: 10.1103/PhysRevLett.113.043004
Abstract: The chemical and physical properties of molecular clusters can heavily depend on their size, which makes them very attractive for the design of new materials with tailored properties. Deriving the structure and dynamics of clusters is therefore of major interest in science. Weakly bound clusters can be studied using conventional spectroscopic techniques, but the number of lines observed is often too small for a comprehensive structural analysis. Impulsive alignment generates rotational wavepackets, which provides simultaneous information on structure and dynamics, as has been demonstrated successfully for isolated molecules. Here, we apply this technique for the firsttime to clusters comprising of a molecule and a single helium atom. By forcing the population of high rotational levels in intense laser fields we demonstrate the generation of rich rotational line spectra for this system, establishing the highly delocalised structure and the coherence of rotational wavepacket propagation. Our findings enable studies of clusters of different sizes and complexity as well as incipient superfluidity effects using wavepacket methods.
Absorption and wavepackets in optically excited semiconductor superlattices driven by dc-ac fields  [PDF]
W. Yan,F. Claro,Z. Y. Zeng,J. Q. Liang
Physics , 2001, DOI: 10.1088/0953-8984/13/22/307
Abstract: Within the one-dimensional tight-binding minibands and on-site Coloumbic interaction approximation, the absorption spectrum and coherent wavepacket time evolution in an optically excited semiconductor superlattice driven by dc-ac electric fields are investigated using the semiconductor Bloch equations. The dominating roles of the ratios of dc-Stark to external ac frequency, as well as ac-Stark to external ac frequency, is emphasized. If the former is an integer ${\cal N}$, then also ${\cal N}$ harmonics are present within one Stark frequency, while the fractional case leads to the formation of excitonic fractional ladders. The later ratio determines the size and profile of the wavepacket. In the absence of excitonic interaction it controls the maximum size wavepackets reach within one cycle, while the interaction produces a strong anisotropy and tends to palliate the dynamic wavepacket localization.
Rotational dynamics of optically trapped polymeric nanofibers  [PDF]
Antonio Alvaro Ranha Neves,Andrea Camposeo,Stefano Pagliara,Rosalba Saija,Ferdinando Borghese,Paolo Denti,Maria Antonia Iati,Roberto Cingolani,Onofrio M. Marago,Dario Pisignano
Physics , 2009, DOI: 10.1364/OE.18.000822
Abstract: The optical trapping of polymeric nanofibers and the characterization of the rotational dynamics are reported. A strategy to apply a torque to a polymer nanofiber, by tilting the trapped fibers using a symmetrical linear polarized Gaussian beam is demonstrated. Rotation frequencies up to 10 Hz are measured, depending on the trapping power, the fiber length and the tilt angle. A comparison of the experimental rotation frequencies in the different trapping configurations with calculations based on optical trapping and rotation of linear nanostructures through a T-Matrix formalism, accurately reproduce the measured data, providing a comprehensive description of the trapping and rotation dynamics.
Amplified Stimulated Terahertz Emission at Room temperature from Optically Pumped Graphene  [PDF]
Stephane Boubanga Tombet,Silvia Chan,Taiichi Otsuji,Akira Satou,and Victor Ryzhii
Physics , 2010,
Abstract: Room temperature Terahertz stimulated emission and population inversion in optically pumped graphene is reported. We experimentally observe fast relaxation and relatively slow recombination dynamics of photogenerated electrons/holes in an exfoliated graphene on SiO2/Si substrate under pumping with a 1550-nm, 80-fs pulsed fiber laser beam and probing with the corresponding terahertz beam generated by optical rectification in a nonlinear electro optical sensor. The time resolved electric field intensity originating from the coherent terahertz photon emission is electro-optically sampled in an total-reflection geometry. The comparison of terahertz electric fields intensities measured on SiO2/Si substrate and that one from graphene clearly indicate that graphene sheet act like an amplifying medium. The Emission spectra agrees relatively well the pumping photon spectrum and its dependency on the pumping power shows a threshold like behavior, testifying the occurrence of the negative conductivity in the THz spectral range and the population inversion. The threshold pumping intensity > 5*10^6 W/cm^2 is in a good agreement with simulations.
Process tomography of dynamical decoupling in a dense optically trapped atomic ensemble  [PDF]
Yoav Sagi,Ido Almog,Nir Davidson
Physics , 2010, DOI: 10.1103/PhysRevLett.105.053201
Abstract: Atomic ensembles have many potential applications in quantum information science. Owing to collective enhancement, working with ensembles at high densities increases the overall efficiency of quantum operations, but at the same time also increases the collision rate and leads to faster decoherence. Here we report on experiments with optically trapped 87Rb atoms demonstrating a 20-fold increase of the coherence time when a dynamical decoupling sequence with more than 200 pi-pulses is applied. We perform quantum process tomography and demonstrate that using the decoupling scheme a dense ensemble with an optical depth of 230 can be used as an atomic memory with coherence times exceeding 3 sec.
Optically-isotropic responses induced by discrete rotational symmetry of nanoparticle clusters  [PDF]
Ben Hopkins,Wei Liu,Andrey E. Miroshnichenko,Yuri S. Kivshar
Physics , 2012, DOI: 10.1039/c3nr01291c
Abstract: Fostered by the recent progress of the fields of plasmonics and metamaterials, the seminal topic of light scattering by clusters of nanoparticles is attracting enormous renewed interest gaining more attention than ever before. Related studies have not only found various new applications in different branches of physics and chemistry, but also spread rapidly into other fields such as biology and medicine. Despite the significant achievements, there still exists unsolved but vitally important challenges of how to obtain robust polarisation-invariant responses of different types of scattering systems. In this paper, we demonstrate polarisation-independent responses of any scattering system with a rotational symmetry with respect to an axis parallel to the propagation direction of the incident wave. We demonstrate that the optical responses such as extinction, scattering, and absorption, can be made independent of the polarisation of the incident wave for all wavelengths. Such polarisation-independent responses are proven to be a robust and generic feature that is purely due to the rotational symmetry of the whole structure. We anticipate our finding will play a significant role in various applications involving light scattering such as sensing, nanoantennas, optical switches, and photovoltaic devices.
Rotational cooling of trapped polyatomic molecules  [PDF]
Rosa Gl?ckner,Alexander Prehn,Barbara G. U. Englert,Gerhard Rempe,Martin Zeppenfeld
Physics , 2015,
Abstract: Controlling the internal degrees of freedom is a key challenge for applications of cold and ultracold molecules. Here, we demonstrate rotational-state cooling of trapped methyl fluoride molecules (CH3F) by optically pumping the population of 16 M-sublevels in the rotational states J=3,4,5, and 6 into a single level. By combining rotational-state cooling with motional cooling, we increase the relative number of molecules in the state J=4, K=3, M=4 from a few percent to over 70%, thereby generating a translationally cold (~30mK) and nearly pure state ensemble of about 10^6 molecules. Our scheme is extendable to larger sets of initial states, other final states and a variety of molecule species, thus paving the way for internal-state control of ever larger molecules.
Optically detected magnetic resonance of high-density ensemble of NV centers in diamond  [PDF]
Yuichiro Matsuzaki,Hiroki Morishita,Takaaki Shimooka,Toshiyuki Tashima,Kosuke Kakuyanagi,Kouichi Semba,W. J. Munro,Hiroshi Yamaguchi,Norikazu Mizuochi,Shiro Saito
Physics , 2015,
Abstract: Optically detected magnetic resonance (ODMR) is a way to characterize the NV centers. Recently, a remarkably sharp dip was observed in the ODMR with a high-density ensemble of NV centers, and this was reproduced by a theoretical model in [Zhu et al., Nature Communications 5, 3424 (2014)], showing that the dip is a consequence of the spin-1 properties of the NV centers. Here, we present much more details of analysis to show how this model can be applied to investigate the properties of the NV centers. By using our model, we have reproduced the ODMR with and without applied magnetic fields. Also, we theoretically investigate how the ODMR is affected by the typical parameters of the ensemble NV centers such as strain distributions, inhomogeneous magnetic fields, and homogeneous broadening width. Our model could provide a way to estimate these parameters from the ODMR, which would be crucial to realize diamond-based quantum information processing.
Dynamics of a Quantum Control-Not Gate for an Ensemble of Four-Spin Molecules at Room Temperature  [PDF]
Gennady P. Berman,Gary D. Doolen,Gustavo V. Lopez,Vladimir I. Tsifrinovich
Physics , 1998, DOI: 10.1103/PhysRevB.58.11570
Abstract: We investigate numerically a single-pulse implementation of a quantum Control-Not (CN) gate for an ensemble of Ising spin systems at room temperature. For an ensemble of four-spin ``molecules'' we simulate the time-evolution of the density matrix, for both digital and superpositional initial conditions. Our numerical calculations confirm the feasibility of implementation of quantum CN gate in this system at finite temperature, using electromagnetic $\pi$-pulse.
Room-Temperature in situ Nuclear Spin Hyperpolarization from Optically-Pumped Nitrogen Vacancy Centers in Diamond  [PDF]
Jonathan P. King,Keunhong Jeong,Christophoros C. Vassiliou,Chang S. Shin,Ralph H. Page,Claudia E. Avalos,Hai-Jing Wang,Alexander Pines
Physics , 2015,
Abstract: We report bulk, room-temperature hyperpolarization of 13C nuclear spins observed via high-field nuclear magnetic resonance (NMR). The hyperpolarization is achieved by optical pumping (OP) of nitrogen vacancy defect centers in diamond accompanied by dynamic nuclear polarization (DNP). The technique harnesses the large optically-induced spin polarization of NV- centers at room temperature, which is many orders of magnitude greater than thermal equilibrium polarization and typically achievable only at sub-Kelvin temperatures. Transfer of the spin polarization to the 13C nuclear spins is accomplished via a combination of OP and microwave irradiation. The OP/DNP is performed at 420 mT, where inductive detection of NMR is feasible, in contrast to the typically exploited level anticrossing regimes at 100 mT and 50 mT. Here, we report a bulk nuclear spin polarization of 6%. This polarization was generated in situ and detected with a standard, inductive NMR probe without the need for sample shuttling or precise crystal orientation. Hyperpolarization via OP/DNP should operate at arbitrary magnetic fields, enabling orders of magnitude sensitivity enhancement for NMR of solids and liquids at ambient conditions.
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