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1.
Chem Sci ; 13(6): 1789-1800, 2022 Feb 09.
Article in English | MEDLINE | ID: mdl-35282626

ABSTRACT

We investigate interatomic Coulombic decay in NeKr dimers after neon inner-valence photoionization [Ne+(2s-1)] using a synchrotron light source. We measure with high energy resolution the two singly charged ions of the Coulomb-exploding dimer dication and the photoelectron in coincidence. By carefully tracing the post-collision interaction between the photoelectron and the emitted ICD electron we are able to probe the temporal evolution of the state as it decays. Although the ionizing light pulses are 80 picoseconds long, we determine the lifetime of the intermediate dimer cation state and visualize the contraction of the nuclear structure on the femtosecond time scale.

2.
Phys Chem Chem Phys ; 20(32): 21075-21084, 2018 Aug 15.
Article in English | MEDLINE | ID: mdl-30074041

ABSTRACT

We present a combined experimental and theoretical investigation of the electron dynamics and body-frame angular dependence of valence photo-single ionization of CF4 and subsequent dissociation into CF3+ and F. Ionization from a valence t2 orbital shows overlapping shape resonances close to threshold that couple to the same total symmetry, leading to striking changes in the photoelectron angular distributions when viewed in the body-frame.

3.
Nature ; 505(7485): 664-6, 2014 Jan 30.
Article in English | MEDLINE | ID: mdl-24362568

ABSTRACT

In 1997, it was predicted that an electronically excited atom or molecule placed in a loosely bound chemical system (such as a hydrogen-bonded or van-der-Waals-bonded cluster) could efficiently decay by transferring its excess energy to a neighbouring species that would then emit a low-energy electron. This intermolecular Coulombic decay (ICD) process has since been shown to be a common phenomenon, raising questions about its role in DNA damage induced by ionizing radiation, in which low-energy electrons are known to play an important part. It was recently suggested that ICD can be triggered efficiently and site-selectively by resonantly core-exciting a target atom, which then transforms through Auger decay into an ionic species with sufficiently high excitation energy to permit ICD to occur. Here we show experimentally that resonant Auger decay can indeed trigger ICD in dimers of both molecular nitrogen and carbon monoxide. By using ion and electron momentum spectroscopy to measure simultaneously the charged species created in the resonant-Auger-driven ICD cascade, we find that ICD occurs in less time than the 20 femtoseconds it would take for individual molecules to undergo dissociation. Our experimental confirmation of this process and its efficiency may trigger renewed efforts to develop resonant X-ray excitation schemes for more localized and targeted cancer radiation therapy.


Subject(s)
Electrons , Carbon Monoxide/chemistry , DNA Damage/radiation effects , Electrons/therapeutic use , Ions , Kinetics , Neoplasms/radiotherapy , Nitrogen/chemistry , Spectrum Analysis , Time Factors , X-Rays
4.
Phys Rev Lett ; 111(1): 013003, 2013 Jul 05.
Article in English | MEDLINE | ID: mdl-23862999

ABSTRACT

We investigate the single-photon double ionization of helium at photon energies of 440 and 800 eV. We observe doubly charged ions with close to zero momentum corresponding to electrons emitted back to back with equal energy. These slow ions are the unique fingerprint of an elusive quasifree photon double ionization mechanism predicted by Amusia et al. nearly four decades ago [J. Phys. B 8, 1248 (1975)]. It results from the nondipole part of the electromagnetic interaction. Our experimental data are supported by calculations performed using the convergent close-coupling and time-dependent close-coupling methods.

5.
Rev Sci Instrum ; 84(3): 033104, 2013 Mar.
Article in English | MEDLINE | ID: mdl-23556804

ABSTRACT

An ion-momentum spectrometer is used to study the dissociative dynamics of electron attachment to molecules. A skimmed, supersonic gas jet is crossed with a pulsed beam of low-energy electrons, and the resulting negative ions are extracted toward a time- and position-sensitive detector. Calculations of the momentum in three dimensions may be used to determine the angular dependence of dissociative attachment as well as the energetics of the reaction.


Subject(s)
DNA Damage , DNA/chemistry , Spectrophotometry/instrumentation , Biotechnology/instrumentation , Biotechnology/methods , Electrons , Equipment Design , Gases , Ions , Kinetics , Semiconductors , Spectrophotometry/methods , Spectrum Analysis/methods , Static Electricity
6.
Phys Rev Lett ; 108(23): 233002, 2012 Jun 08.
Article in English | MEDLINE | ID: mdl-23003951

ABSTRACT

We demonstrate a method for determining the full three-dimensional molecular-frame photoelectron angular distribution in polyatomic molecules using methane as a prototype. Simultaneous double Auger decay and subsequent dissociation allow measurement of the initial momentum vectors of the ionic fragments and the photoelectron in coincidence, allowing full orientation by observing a three-ion decay pathway, (H+, H+, CH2(+)). We find the striking result that at low photoelectron energies the molecule is effectively imaged by the focusing of photoelectrons along bond directions.

7.
Intern Med J ; 40(7): 530-3, 2010 Jul.
Article in English | MEDLINE | ID: mdl-20633063

ABSTRACT

Palliative medicine trainees are currently required to complete 36 months of core and non-core training, including a 6-month oncology module. There are presently few published data from palliative medicine trainees regarding the structure and appropriateness of their curriculum. The aim of this study was to evaluate skills related to the Royal Australasian College of Physicians essential learning objectives and the experiences gained by the individuals during their oncology training. An investigator-designed questionnaire was emailed out to all current Australasian trainees or first year consultants. A 45% response rate was achieved. Women were significantly more negative in their responses to the improvement of communication skills and the understanding of ethics. Chapter trainees rated improved leadership and future management skills lower than other respondents. Fifty-eight per cent of the respondents believed the oncology module should remain mandatory. Although valuable, a more tailored and flexible approach to this part of training should be considered.


Subject(s)
Internship and Residency , Mandatory Programs , Medical Oncology/education , Palliative Care , Australia , Female , Humans , Internship and Residency/methods , Male , Medical Oncology/methods , New Zealand , Palliative Care/methods , Physicians , Surveys and Questionnaires
8.
J Agric Saf Health ; 15(4): 311-26, 2009 Oct.
Article in English | MEDLINE | ID: mdl-19967906

ABSTRACT

A convenience survey of 702 certified pesticide applicators was conducted in three states to assess the use of 16 types of engineering controls and 13 types of personal protective equipment (PPE). Results showed that 8 out of 16 engineering devices were adopted by more than 50% of the respondents. The type of crop, size of agricultural operation, and the type of pesticide application equipment were found to influence the adoption of engineering controls. Applicators working on large farms, users of boom and hydraulic sprayers, and growers of field crops were more likely to use engineering devices. Respondents reported a high level of PPE use, with chemical-resistant gloves showing the highest level of compliance. An increase in pesticide applicators wearing appropriate headgear was reported. The majority of respondents did not wear less PPE simply because they used engineering controls. Those who did modify their PPE choices when employing engineering controls used tractors with enclosed cabs and/or were vegetable growers.


Subject(s)
Agriculture , Occupational Exposure/prevention & control , Pesticides , Protective Clothing/statistics & numerical data , Safety Management/methods , Safety Management/statistics & numerical data , Adult , Agricultural Workers' Diseases/prevention & control , Health Surveys , Humans , Middle Aged , Surveys and Questionnaires , United States , Young Adult
9.
Phys Rev Lett ; 102(22): 223001, 2009 Jun 05.
Article in English | MEDLINE | ID: mdl-19658860

ABSTRACT

We have used cold target recoil ion momentum spectroscopy to study the continuum correlation between the photoelectron of core-photoionized neon and the subsequent Auger electron. We observe a strong angular correlation between the two electrons. Classical trajectory Monte Carlo calculations agree quite well with the photoelectron energy distribution that is shifted due to the potential change associated with Auger decay. However, a striking discrepancy results in the distribution of the relative angle between Auger and photoelectron. The classical model predicts a shift in photoelectron flux away from the Auger emission direction, and the data strikingly reveal that the flux is lost rather than diverted, indicating that the two-step interpretation of photoionization followed by Auger emission is insufficient to fully describe the core-photoionization process.

10.
Phys Rev Lett ; 100(13): 133005, 2008 Apr 04.
Article in English | MEDLINE | ID: mdl-18517946

ABSTRACT

We investigate single-photon double ionization of H(2) by 130 to 240 eV circularly polarized photons. We find a double slitlike interference pattern in the sum momentum of both electrons in the molecular frame which survives integration over all other degrees of freedom. The difference momentum and the individual electron momentum distributions do not show such a robust interference pattern. We show that this interference results from a non-Heitler-London fraction of the H(2) ground state where both electrons are at the same atomic center.

11.
Science ; 320(5878): 920-3, 2008 May 16.
Article in English | MEDLINE | ID: mdl-18487190

ABSTRACT

Although valence electrons are clearly delocalized in molecular bonding frameworks, chemists and physicists have long debated the question of whether the core vacancy created in a homonuclear diatomic molecule by absorption of a single x-ray photon is localized on one atom or delocalized over both. We have been able to clarify this question with an experiment that uses Auger electron angular emission patterns from molecular nitrogen after inner-shell ionization as an ultrafast probe of hole localization. The experiment, along with the accompanying theory, shows that observation of symmetry breaking (localization) or preservation (delocalization) depends on how the quantum entangled Bell state created by Auger decay is detected by the measurement.

12.
Science ; 318(5852): 949-52, 2007 Nov 09.
Article in English | MEDLINE | ID: mdl-17991857

ABSTRACT

The wave nature of particles is rarely observed, in part because of their very short de Broglie wavelengths in most situations. However, even with wavelengths close to the size of their surroundings, the particles couple to their environment (for example, by gravity, Coulomb interaction, or thermal radiation). These couplings shift the wave phases, often in an uncontrolled way, and the resulting decoherence, or loss of phase integrity, is thought to be a main cause of the transition from quantum to classical behavior. How much interaction is needed to induce this transition? Here we show that a photoelectron and two protons form a minimum particle/slit system and that a single additional electron constitutes a minimum environment. Interference fringes observed in the angular distribution of a single electron are lost through its Coulomb interaction with a second electron, though the correlated momenta of the entangled electron pair continue to exhibit quantum interference.

13.
Science ; 315(5812): 629-33, 2007 Feb 02.
Article in English | MEDLINE | ID: mdl-17272717

ABSTRACT

H2, the smallest and most abundant molecule in the universe, has a perfectly symmetric ground state. What does it take to break this symmetry? We found that the inversion symmetry can be broken by absorption of a linearly polarized photon, which itself has inversion symmetry. In particular, the emission of a photoelectron with subsequent dissociation of the remaining H+2 fragment shows no symmetry with respect to the ionic H+ and neutral H atomic fragments. This lack of symmetry results from the entanglement between symmetric and antisymmetric H+2 states that is caused by autoionization. The mechanisms behind this symmetry breaking are general for all molecules.

14.
Phys Rev Lett ; 94(2): 023201, 2005 Jan 21.
Article in English | MEDLINE | ID: mdl-15698173

ABSTRACT

Hollow-state (double K-shell vacancy) production in Li-like Be+, B2+, C3+, and F6+ ions colliding with He has been investigated using high-resolution Auger-electron spectroscopy. The formation of discrete states and their relative intensities show striking dependences on the nuclear charge Z of the ion. From the projectile velocity dependences of these states the contribution of the electron-electron interaction is determined, showing that the hollow states are formed largely by electron correlation with a strength that diminishes for increasing Z.

15.
Mund Kiefer Gesichtschir ; 9(2): 121-5, 2005 Mar.
Article in German | MEDLINE | ID: mdl-15647952

ABSTRACT

CASE REPORT: A 25-year-old patient with fever, dysphagia, and reduced general condition was referred to our department by his dentist after 1 week of antibiotic therapy. He presented with a painful palpable mass in the right lower jaw that had developed 2 weeks before. The orthopantomogram showed a caries and periapical lesion at the right lower wisdom tooth. During extraction of the tooth and putative intra- and extraoral abscess incision, no pus could be drained and the mass persisted. CT scans then revealed lobulated soft tissue masses on both sides of the neck with the main focus on the right side. In an additional operation with excision of the mass, Castleman's disease of the hyaline vascular type was diagnosed. HISTOPATHOLOGIC FINDINGS: Staging could not detect further pathological findings and the patient's postoperative general condition improved continuously. The histological features of the hayline vascular type of Castleman's disease were characterized by multiple germinal centers surrounded by circumferentially arranged layers of small lymphocytes interconnected by a prominent vascular stroma with occasional plasma cells ("onion skin"). CONCLUSION: Castleman's disease is a rare and yet poorly understood disease, characterized by inhomogeneous growth of lymphoid tissue. Mostly benign it remains a diagnostic challenge before histological investigation. In unclear submandibular swellings and neck lumps assumed to be an abscess, this rare differential diagnosis must be considered. Facing recurrence and potential for malignancy, follow-up of the patients over several years is necessary.


Subject(s)
Castleman Disease/diagnosis , Deglutition Disorders/etiology , Fever of Unknown Origin/etiology , Adult , Castleman Disease/surgery , Diagnosis, Differential , Humans , Lymph Nodes/pathology , Lymphocytes/pathology , Male , Mandible , Molar, Third/surgery , Periapical Abscess/diagnosis , Periapical Abscess/surgery , Radiography, Panoramic , Tomography, X-Ray Computed
16.
Nature ; 431(7007): 437-40, 2004 Sep 23.
Article in English | MEDLINE | ID: mdl-15386008

ABSTRACT

All properties of molecules--from binding and excitation energies to their geometry--are determined by the highly correlated initial-state wavefunction of the electrons and nuclei. Details of these correlations can be revealed by studying the break-up of these systems into their constituents. The fragmentation might be initiated by the absorption of a single photon, by collision with a charged particle or by exposure to a strong laser pulse: if the interaction causing the excitation is sufficiently understood, the fragmentation process can then be used as a tool to investigate the bound initial state. The interaction and resulting fragment motions therefore pose formidable challenges to quantum theory. Here we report the coincident measurement of the momenta of both nuclei and both electrons from the single-photon-induced fragmentation of the deuterium molecule. The results reveal that the correlated motion of the electrons is strongly dependent on the inter-nuclear separation in the molecular ground state at the instant of photon absorption.

17.
Phys Rev Lett ; 92(16): 163001, 2004 Apr 23.
Article in English | MEDLINE | ID: mdl-15169223

ABSTRACT

We report the first kinematically complete study of the four-body fragmentation of the D2 molecule following absorption of a single photon. For equal energy sharing of the two electrons and a photon energy of 75.5 eV, we observed the relaxation of one of the selection rules valid for He photo-double-ionization and a strong dependence of the electron angular distribution on the orientation of the molecular axis. This effect is reproduced by a model in which a pair of photoionization amplitudes is introduced for the light polarization parallel and perpendicular to the molecular axis.

18.
Phys Rev Lett ; 92(13): 133201, 2004 Apr 02.
Article in English | MEDLINE | ID: mdl-15089606

ABSTRACT

Single- and double-electron transfer to autoionizing 1s2l2l(') configurations in fluorine ions have been investigated for 1.1 MeV/u collisions of F7+ and F8+ with He and Ne. The resulting Auger electron emission spectra show anomolously large intensities for the formation of the metastable 1s(2s2p 3P) 4P state compared to the similarly configured 1s(2s2p 3P) 2P- and 1s(2s2p 1P) 2P+ states. The large 4P intensity, which cannot be explained on the basis of spin statistics, is attributed instead to the Pauli exchange of similarly aligned electrons.

19.
Phys Rev Lett ; 90(23): 233002, 2003 Jun 13.
Article in English | MEDLINE | ID: mdl-12857254

ABSTRACT

We have used complete correlated momentum mapping of the photoelectron and heavy ion products from the dissociation of the di-cation of acetylene, induced by photoionizing the carbon K shell of one of the atoms, to map out the angular correlation between the electron and the axis of the target molecule. The (quasi-) symmetric decay is found to proceed through both acetylene and vinylidene configurations. By using the strongly peaked photoelectron emission to "start a clock," an upper limit of 60 fs is placed on the isomerization time from the acetylene to the vinylidene configuration.

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