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1.
Phys Chem Chem Phys ; 23(38): 21521-21531, 2021 Oct 06.
Artigo em Inglês | MEDLINE | ID: mdl-34549209

RESUMO

We introduce a novel and sensitive ns-resolved atomic magnetometer, which is at least three orders of magnitude faster than conventional magnetometers. We use the magnetic field dependence of the hyperfine beating of high-density spin-polarized H atoms, produced from the rapid photodissociation of HCl gas with sub-ns laser pulses and measured with a pick-up coil, to demonstrate ns-resolved magnetometry, and project sensitivity of a few nT for a spin-projection-limited sensor with 10 nl measurement volume after 1 ns measurement time. The magnetometer will allow ultrafast continuous B-field measurements in many fields, including spin chemistry, spin physics, and plasma physics.

2.
Nature ; 514(7520): 76-9, 2014 Oct 02.
Artigo em Inglês | MEDLINE | ID: mdl-25209661

RESUMO

Detecting and quantifying chirality is important in fields ranging from analytical and biological chemistry to pharmacology and fundamental physics: it can aid drug design and synthesis, contribute to protein structure determination, and help detect parity violation of the weak force. Recent developments employ microwaves, femtosecond pulses, superchiral light or photoionization to determine chirality, yet the most widely used methods remain the traditional methods of measuring circular dichroism and optical rotation. However, these signals are typically very weak against larger time-dependent backgrounds. Cavity-enhanced optical methods can be used to amplify weak signals by passing them repeatedly through an optical cavity, and two-mirror cavities achieving up to 10(5) cavity passes have enabled absorption and birefringence measurements with record sensitivities. But chiral signals cancel when passing back and forth through a cavity, while the ubiquitous spurious linear birefringence background is enhanced. Even when intracavity optics overcome these problems, absolute chirality measurements remain difficult and sometimes impossible. Here we use a pulsed-laser bowtie cavity ringdown polarimeter with counter-propagating beams to enhance chiral signals by a factor equal to the number of cavity passes (typically >10(3)); to suppress the effects of linear birefringence by means of a large induced intracavity Faraday rotation; and to effect rapid signal reversals by reversing the Faraday rotation and subtracting signals from the counter-propagating beams. These features allow absolute chiral signal measurements in environments where background subtraction is not feasible: we determine optical rotation from α-pinene vapour in open air, and from maltodextrin and fructose solutions in the evanescent wave produced by total internal reflection at a prism surface. The limits of the present polarimeter, when using a continuous-wave laser locked to a stable, high-finesse cavity, should match the sensitivity of linear birefringence measurements (3 × 10(-13) radians), which is several orders of magnitude more sensitive than current chiral detection limits and is expected to transform chiral sensing in many fields.

3.
J Chem Phys ; 147(1): 013948, 2017 Jul 07.
Artigo em Inglês | MEDLINE | ID: mdl-28688451

RESUMO

Alignment of the electronically excited E,F state of the H2 molecule is studied using the velocity mapping imaging technique. Photofragment images of H+ due to the dissociation mechanism that follows the 2-photon excitation into the (E,F; ν = 0, J = 0) electronic state show a strong dependence on laser intensity, which is attributed to the high polarizability anisotropy of the H2 (E,F) state. We observe a marked structure in the angular distribution, which we explain as the interference between the prepared J = 0 and Stark-mixed J = 2 rovibrational states of H2, as the laser intensity increases. Quantification of these effects allows us to extract the polarizability anisotropy of the H2 (E,F J = 0) state yielding a value of 312 ± 82 a.u. (46 Å3). By comparison, CS2 has 10 Å3, I2 has 7 Å3, and hydrochlorothiazide (C7H8ClN3O4S2) has about 25 Å3 meaning that we have created the most easily aligned molecule ever measured, by creating a mixed superposition state that is highly anisotropic in its polarizability.

4.
J Chem Phys ; 143(10): 104202, 2015 Sep 14.
Artigo em Inglês | MEDLINE | ID: mdl-26374026

RESUMO

We present the theory and experimental details for chiral-cavity-ring-down polarimetry and magnetometry, based on ring cavities supporting counterpropagating laser beams. The optical-rotation symmetry is broken by the presence of both chiral and Faraday birefringence, giving rise to signal reversals which allow rapid background subtractions. We present the measurement of the specific rotation at 800 nm of vapors of α-pinene, 2-butanol, and α-phellandrene, the measurement of optical rotation of sucrose solutions in a flow cell, the measurement of the Verdet constant of fused silica, and measurements and theoretical treatment of evanescent-wave optical rotation at a prism surface. Therefore, these signal-enhancing and signal-reversing methods open the way for ultrasensitive polarimetry measurements in gases, liquids and solids, and at surfaces.

5.
Light Sci Appl ; 10(1): 35, 2021 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-33579898

RESUMO

Recently, our group produced spin-polarized hydrogen (SPH) atoms at densities of at least 1019 cm-3 from the photodissociation of hydrogen halide molecules with circularly polarized UV light and measured them via magnetization-quantum beats with a pickup coil. These densities are approximately 7 orders of magnitude higher than those produced using conventional methods, opening up new fields of application, such as ultrafast magnetometry, the production of polarized MeV and GeV particle beams, such as electron beams with intensities approximately 104 higher than current sources, and the study of polarized nuclear fusion, for which the reaction cross sections of D-T and D-3He reactions are expected to increase by 50% for fully polarized nuclear spins. We review the production, detection, depolarization mechanisms, and potential applications of high-density SPH.

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