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2003


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New electro-optic effect: Sum-frequency generation from optically active liquids in the presence of a dc electric field

Fischer, P., Buckingham, A., Beckwitt, K., Wiersma, D., Wise, F.

PHYSICAL REVIEW LETTERS, 91(17), 2003 (article)

Abstract
We report the observation of sum-frequency signals that depend linearly on an applied electrostatic field and that change sign with the handedness of an optically active solute. This recently predicted chiral electro-optic effect exists in the electric-dipole approximation. The static electric field gives rise to an electric-field-induced sum-frequency signal (an achiral third-order process) that interferes with the chirality-specific sum-frequency at second order. The cross-terms linear in the electrostatic field constitute the effect and may be used to determine the absolute sign of second- and third-order nonlinear-optical susceptibilities in isotropic media.

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DOI [BibTex]

2003


DOI [BibTex]


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Chiral and achiral contributions to sum-frequency generation from optically active solutions of binaphthol

Fischer, P., Wise, F., Albrecht, A.

JOURNAL OF PHYSICAL CHEMISTRY A, 107(40):8232-8238, 2003 (article)

Abstract
The nonlinear sum- and difference-frequency generation spectroscopies can be probes of molecular chirality in optically active systems. We present a tensorial analysis of the chirality-specific electric-dipolar sum-frequency-generation susceptibility and the achiral electric-quadrupolar and magnetic-dipolar nonlinearities at second order in isotropic media. The chiral and achiral contributions to the sum-frequency signal from the bulk of optically active solutions of 1,1'-bi-2-naphthol (2,2'-dehydroxy-1,1'-binaphthyl) can be distinguished, and the former dominates. Ab initio computations reveal the dramatic resonance enhancement that the isotropic component of the electric-dipolar three-wave mixing hyperpolarizability experiences. Away from resonance its magnitude rapidly decreases, as-unlike the vector component-it is zero in the static limit. The dispersion of the first hyperpolarizability is computed by a configuration interaction singles sum-over-states approach with explicit regard to the Franck-Condon active vibrational substructure for all resonant electronic states.

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DOI [BibTex]

DOI [BibTex]


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Synthetic gecko foot-hair micro/nano-structures as dry adhesives

Sitti, M., Fearing, R. S.

Journal of adhesion science and technology, 17(8):1055-1073, Taylor & Francis Group, 2003 (article)

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Project Page [BibTex]

Project Page [BibTex]


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Teleoperated touch feedback from the surfaces at the nanoscale: modeling and experiments

Sitti, M., Hashimoto, H.

IEEE/ASME transactions on mechatronics, 8(2):287-298, IEEE, 2003 (article)

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[BibTex]

[BibTex]


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Scaled teleoperation system for nano-scale interaction and manipulation

Sitti, M., Aruk, B., Shintani, H., Hashimoto, H.

Advanced Robotics, 17(3):275-291, Taylor & Francis Group, 2003 (article)

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[BibTex]

[BibTex]


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Atomic force microscope probe based controlled pushing for nano-tribological characterization

Sitti, M.

IEEE/ASME Transactions on Mechatronics, 8(3), 2003 (article)

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[BibTex]


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Efficient charge recovery method for driving piezoelectric actuators with quasi-square waves

Campolo, D., Sitti, M., Fearing, R. S.

IEEE transactions on ultrasonics, ferroelectrics, and frequency control, 50(3):237-244, IEEE, 2003 (article)

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[BibTex]

[BibTex]


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Piezoelectrically actuated four-bar mechanism with two flexible links for micromechanical flying insect thorax

Sitti, M.

IEEE/ASME transactions on mechatronics, 8(1):26-36, IEEE, 2003 (article)

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[BibTex]

2001


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Isotropic second-order nonlinear optical susceptibilities

Fischer, P., Buckingham, A., Albrecht, A.

PHYSICAL REVIEW A, 64(5), 2001 (article)

Abstract
The second-order nonlinear optical susceptibility, in the electric dipole approximation, is only nonvanishing for materials that are noncentrosymmetric. Should the medium be isotropic, then only a chiral system. such as an optically active liquid, satisfies this symmetry requirement. We derive the quantum-mechanical form of the isotropic component of the sum- and difference-frequency susceptibility and discuss its unusual spectral properties. We show that any coherent second-order nonlinear optical process in a system of randomly oriented molecules requires the medium to be chiral. and the incident frequencies to be different and nonzero. Furthermore, a minimum of two nondegenerate excited molecular states are needed for the isotropic part of the susceptibility to be nonvanishing. The rotationally invariant susceptibility is zero in the static field limit and shows exceptionally sensitive resonance and dephasing effects that are particular to chiral centers.

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DOI [BibTex]

2001


DOI [BibTex]


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Reply to “Comment on ‘Phenomenological damping in optical response tensors’”

Buckingham, A., Fischer, P.

PHYSICAL REVIEW A, 63(4), 2001 (article)

Abstract
We show that damping factors must not be incorporated in the perturbation of the ground state by a static electric field. If they are included, as in the theory of Stedman et al. {[}preceding Comment. Phys. Rev. A 63, 047801 (2001)], then there would be an electric dipole in the y direction induced in a hydrogen atom in the M-s = + 1/2 state by a static electric field in the x direction. Such a dipole is excluded by symmetry.

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DOI [BibTex]


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Wing transmission for a micromechanical flying insect

Yan, J., Avadhanula, S., Birch, J., Dickinson, M., Sitti, M., Su, T., Fearing, R.

Journal of Micromechatronics, 1(3):221-237, Brill, 2001 (article)

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[BibTex]

[BibTex]

2000


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Phenomenological damping in optical response tensors

Buckingham, A., Fischer, P.

PHYSICAL REVIEW A, 61(3), 2000 (article)

Abstract
Although perturbation theory applied to the optical response of a molecule or material system is only strictly valid far from resonances, it is often applied to ``near-resonance{''} conditions by means of complex energies incorporating damping. Inconsistent signs of the damping in optical response tensors have appeared in the recent literature, as have errors in the treatment of the perturbation by a static held. The ``equal-sign{''} convention used in a recent publication yields an unphysical material response, and Koroteev's intimation that linear electro-optical circular dichroism may exist in an optically active liquid under resonance conditions is also flawed. We show that the isotropic part of the Pockels tensor vanishes.

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DOI [BibTex]

2000


DOI [BibTex]


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Ab initio investigation of the sum-frequency hyperpolarizability of small chiral molecules

Champagne, B., Fischer, P., Buckingham, A.

CHEMICAL PHYSICS LETTERS, 331(1):83-88, 2000 (article)

Abstract
Using a sum-over-states procedure based on configuration interaction singles /6-311++G{*}{*}, we have computed the sum-frequency hyperpolarizability beta (ijk)(-3 omega; 2 omega, omega) Of two small chiral molecules, R-monofluoro-oxirane and R-(+)-propylene oxide. Excitation energies were scaled to fit experimental UV-absorption data and checked with ab initio values from time-dependent density functional theory. The isotropic part of the computed hyperpolarizabilities, beta(-3 omega; 2 omega, omega), is much smaller than that reported previously from sum-frequency generation experiments on aqueous solutions of arabinose. Comparison is made with a single-centre chiral model. (C) 2000 Elsevier Science B.V. All rights reserved.

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DOI [BibTex]

DOI [BibTex]


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Three-wave mixing in chiral liquids

Fischer, P., Wiersma, D., Righini, R., Champagne, B., Buckingham, A.

PHYSICAL REVIEW LETTERS, 85(20):4253-4256, 2000 (article)

Abstract
Second-order nonlinear optical frequency conversion in isotropic systems is only dipole allowed for sum- and difference-frequency generation in chiral media. We develop a single-center chiral model of the three-wave mixing (sum:frequency generation) nonlinearity and estimate its magnitude. We also report results from ab initio calculations and from three- and four-wave mixing experiments in support of the theoretical estimates. We show that the second-order susceptibility in chiral liquids is much smaller than previously thought.

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DOI [BibTex]

DOI [BibTex]


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Two-dimensional fine particle positioning under an optical microscope using a piezoresistive cantilever as a manipulator

Sitti, M., Hashimoto, H.

journal of Micromechatronics, 1(1):25-48, Brill, 2000 (article)

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[BibTex]


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Investigation of Virtual Reality Interface for AFM-based Nano Manipulation

Horiguchi, S., Sitti, M., Hashimoto, H.

IEEJ Transactions on Electronics, Information and Systems, 120(12):1948-1956, The Institute of Electrical Engineers of Japan, 2000 (article)

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[BibTex]

[BibTex]


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Macro to Nano Tele-Manipulation Towards Nanoelectromec hanical Systems

Sitti, M., Hashimoto, H.

Journal of Robotics and Mechatronics, 12(3):209-217, FUJI TECHNOLOGY PRESS LTD., 2000 (article)

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[BibTex]

[BibTex]


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Controlled pushing of nanoparticles: modeling and experiments

Sitti, M., Hashimoto, H.

IEEE/ASME transactions on mechatronics, 5(2):199-211, IEEE, 2000 (article)

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[BibTex]

[BibTex]

1998


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Surface second-order nonlinear optical activity

Fischer, P., Buckingham, A.

JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS, 15(12):2951-2957, 1998 (article)

Abstract
Following the recent observation of a large second-harmonic intensity difference from a monolayer of chiral molecules with left and right circularly polarized light, the scattering theory is generalized and extended to predict linear and circular intensity differences for the more Versatile sum-frequency spectroscopy. Estimates indicate that intensity differences should be detectable for a typical experimental arrangement. The second-order nonlinear surface susceptibility tensor is given for different surface point groups in the electric dipole approximation; it is shown that nonlinear optical activity phenomena unambiguously probe molecular chirality only for molecular monolayers that are symmetric about the normal. Other surface symmetries can give rise to intensity differences from monolayers composed of achiral molecules. A water surface is predicted to show Linear and nonlinear optical activity in the presence of an electric field parallel to the surface. (C) 1998 Optical Society of America {[}S0740-3224(98)01311-3] OCIS codes: 190.0190, 190.4350, 240.6490.

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DOI [BibTex]

1998


DOI [BibTex]


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Linear electro-optic effect in optically active liquids

Buckingham, A., Fischer, P.

CHEMICAL PHYSICS LETTERS, 297(3-4):239-246, 1998 (article)

Abstract
A linear effect of an electrostatic field F on the intensity of sum- and difference-frequency generation in a chiral liquid is predicted. It arises in the electric dipole approximation. The effect changes sign with the enantiomer and on reversing the direction of the electrostatic field. The sum-frequency generator chi(alpha beta gamma)((2)) (-omega(3);omega(1),omega(2)), where omega(3) = omega(1) + omega(2), and the electric field-induced sum-frequency generator chi(alpha beta gamma delta)((3))(-omega(3);omega(1),omega(2),0)F-delta interfere and their contributions to the scattering power can be distinguished. Encouraging predictions are given for a typical experimental arrangement. (C) 1998 Elsevier Science B.V. All rights reserved.

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DOI [BibTex]

DOI [BibTex]


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Monolayers of hexadecyltrimethylammonium p-tosylate at the air-water interface. 1. Sum-frequency spectroscopy

Bell, G., Li, Z., Bain, C., Fischer, P., Duffy, D.

JOURNAL OF PHYSICAL CHEMISTRY B, 102(47):9461-9472, 1998 (article)

Abstract
Sum-frequency vibrational spectroscopy has been used to determine the structure of monolayers of the cationic surfactant, hexadecyltrimethylammonium p-tosylate (C(16)TA(+)Ts(-)), at the surface of water. Selective deuteration of the cation or the anion allowed the separate detection of sum-frequency spectra of the surfactant and of counterions that are bound to the monolayer. The p-tosylate ions an oriented with their methyl groups pointing away from the aqueous subphase and with the C-2 axis tilted, on average, by 30-40 degrees from the surface normal. The vibrational spectra of C(16)TA(+) indicate that the number of gauche defects in the monolayer does not change dramatically when bromide counterions are replaced by p-tosylate. The ends of the hydrocarbon chains of C16TA+ are, however, tilted much further from the surface normal in the presence of p-tosylate than in the presence of bromide. A quantitative analysis of the sum-frequency spectra requires a knowledge of the molecular hyperpolarizability tensor: the role of ab initio calculations and Raman spectroscopy in determining the components of this tensor is discussed.

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DOI [BibTex]

DOI [BibTex]


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Ultraviolet resonance Raman study of drug binding in dihydrofolate reductase, gyrase, and catechol O-methyltransferase

Couling, V., Fischer, P., Klenerman, D., Huber, W.

BIOPHYSICAL JOURNAL, 75(2):1097-1106, 1998 (article)

Abstract
This paper presents a study of the use of ultraviolet resonance Raman (UVRR) spectroscopic methods as a means of elucidating aspects of drug-protein interactions. Some of the RR vibrational bands of the aromatic amino acids tyrosine and tryptophan are sensitive to the microenvironment, and the use of UV excitation radiation allows selective enhancement of the spectral features of the aromatic amino acids, enabling observation specifically of their change in microenvironment upon drug binding. The three drug-protein systems investigated in this study are dihydrofolate reductase with its inhibitor trimethoprim, gyrase with novobiocin, and catechol O-methyltransferase with dinitrocatechol. It is demonstrated that UVRR spectroscopy has adequate sensitivity to be a useful means of detecting drug-protein interactions in those systems for which the electronic absorption of the aromatic amino acids changes because of hydrogen bonding and/or possible dipole-dipole and dipole-polarizability interactions with the ligand.

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DOI [BibTex]

DOI [BibTex]


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Tele-nanorobotics using an atomic force microscope as a nanorobot and sensor

Sitti, M., Hashimoto, H.

Advanced Robotics, 13(4):417-436, Taylor & Francis, 1998 (article)

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[BibTex]

[BibTex]