Real-time visualization of molecular transformations is a captivating yet challenging frontier of ultrafast optical science and physical chemistry. While ultrafast x-ray and electron diffraction methods can achieve the needed subangstrom spatial resolution, their temporal resolution is still limited to hundreds of femtoseconds, much longer than the few femtoseconds required to probe real-time molecular dynamics. Here, we show that high-order harmonics generated by intense femtosecond lasers can be used to image molecules with few-ten-attosecond temporal resolution and few-picometer spatial resolution.
View Article and Find Full Text PDFThyroid
September 2023
Understanding of changes in salivary and lacrimal gland functions after radioactive iodine therapy (I-therapy) remains limited, and, to date, no studies have evaluated dose-response relationships between absorbed dose from I-therapy and dysfunctions of these glands. This study investigates salivary/lacrimal dysfunctions in differentiated thyroid cancer (DTC) patients six months after I-therapy, identifies I-therapy-related risk factors for salivary/lacrimal dysfunctions, and assesses the relationships between I-therapy radiation dose and these dysfunctions. A cohort study was conducted involving 136 DTC patients treated by I-therapy of whom 44 and 92 patients received 1.
View Article and Find Full Text PDFWe report a combined experimental and theoretical study on the effect of autoionizing resonances in time-resolved photoelectron spectroscopy. The coherent excitation of N_{2} by ∼14.15 eV extreme-ultraviolet photons prepares a superposition of three dominant adjacent vibrational levels (v^{'}=14-16) in the valence b^{'} ^{1}Σ_{u}^{+} state, which are probed by the absorption of two or three near-infrared photons (800 nm).
View Article and Find Full Text PDFObserving changes in molecular structure requires atomic-scale Ångstrom and femtosecond spatio-temporal resolution. We use the Fourier transform (FT) variant of laser-induced electron diffraction (LIED), FT-LIED, to directly retrieve the molecular structure of HO with picometer and femtosecond resolution without a priori knowledge of the molecular structure nor the use of retrieval algorithms or ab initio calculations. We identify a symmetrically stretched HO field-dressed structure that is most likely in the ground electronic state.
View Article and Find Full Text PDFJ Infect
August 2019
Background: Carbapenem-resistant Enterobacteriaceae (CRE) is an increasing problem worldwide, but particularly problematic in low- and middle-income countries (LMIC) due to limitations of resources for surveillance of CRE and infection prevention and control (IPC).
Methods: A point prevalence survey (PPS) with screening for colonisation with CRE was conducted on 2233 patients admitted to neonatal, paediatric and adult care at 12 Vietnamese hospitals located in northern, central and southern Vietnam during 2017 and 2018. CRE colonisation was determined by culturing of faecal specimens on selective agar for CRE.
Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump-probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct structural retrieval of neutral carbonyl disulfide (CS) in the [Formula: see text] excited electronic state using laser-induced electron diffraction (LIED). We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS molecule with combined picometer and attosecond resolution using intrapulse pump-probe excitation and measurement.
View Article and Find Full Text PDFWe demonstrate an angular high-harmonic spectroscopy method to probe the spinning dynamics of a molecular rotation wave packet in real time. With the excitation of two time-delayed, polarization-skewed pump pulses, the molecular ensemble is impulsively kicked to rotate unidirectionally, which is subsequently irradiated by another delayed probe pulse for high-order harmonic generation (HHG). The spatiotemporal evolution of the molecular rotation wave packet is visualized from the time-dependent angular distributions of the HHG yields and frequency shift measured at various polarization directions and time delays of the probe pulse.
View Article and Find Full Text PDFFatty Acid Synthase (FASN), a key enzyme of lipogenesis, is upregulated in many cancers including colorectal cancer (CRC); increased FASN expression is associated with poor prognosis. Potent FASN inhibitors (TVBs) developed by 3-V Biosciences demonstrate anti-tumor activity and and a favorable tolerability profile in a Phase I clinical trial. However, CRC characteristics associated with responsiveness to FASN inhibition are not fully understood.
View Article and Find Full Text PDFA correction to this article has been published and is linked from the HTML and PDF versions of this paper. The error has been fixed in the paper.
View Article and Find Full Text PDFStructural isomers, molecules having the same chemical formula but with atoms bonded in different order, are hard to identify using conventional spectroscopy and mass spectrometry. They exhibit virtually indistinguishable mass spectra when ionized by electrons. Laser mass spectrometry based on photoionization of the isomers has emerged as a promising alternative but requires shaped ultrafast laser pulses.
View Article and Find Full Text PDFColorectal cancer (CRC) is the second leading cause of cancer deaths in the United States; the predominant cause for mortality is metastasis to distant organs (e.g., lung).
View Article and Find Full Text PDFDelivering isotopic tracers for metabolic studies in rodents without overt stress is challenging. Current methods achieve low label enrichment in proteins and lipids. Here, we report noninvasive introduction of C-glucose via a stress-free, ad libitum liquid diet.
View Article and Find Full Text PDFBackground: A significant proportion of patients never receive curative-intent surgery for resectable gastric cancer (GC). The primary aims of this study were to identify disparities and targetable risk factors associated with failure to operate in the context of national trends in surgical rates for resectable GC.
Methods: The National Cancer Database was used to identify patients with resectable GC (adenocarcinoma, clinical stage IA-IIIC, 2004-2013).
Background: Although adjuvant therapy (AT) is a necessary component of multimodality therapy for pancreatic ductal adenocarcinoma (PDAC), its application can be hindered by post-pancreaticoduodenectomy (PD) complications. The primary aim of this study was to evaluate the impact of post-PD complications on AT utilization and overall survival (OS).
Methods: Patients undergoing PD without neoadjuvant therapy for stages I-III PDAC at a single institution (2007-2015) were evaluated.
Through the use of the technique of time-of-flight mass spectroscopy, we obtain strong-field ionization yields for randomly oriented 1,2-dichloroethylene (1,2-DCE) (CHCl) and 2-butene (CH). We are interested in studying the effect of conformal structure in strong-field ionization and, in particular, the role of molecular polarity. That is, we can perform strong-field ionization studies in polar vs non-polar molecules that have the same chemical composition.
View Article and Find Full Text PDFWe measure high order harmonics from the molecule SF over a large range of phase matching conditions and observe several features in the harmonics that are largely independent of such macroscopic conditions. The experimental data are then compared to the quantitative rescattering theory for the generation of harmonics from three orbitals. With this comparison, we are able to assign spectroscopic features in the harmonics to contributions from 1t (HOMO) and 5t (HOMO-1) orbitals.
View Article and Find Full Text PDFBackground: We hypothesized hepato-pancreato-biliary (HPB) surgery patients are more likely to be hypercoagulable than hypocoagulable, and that bleeding risks from VTE chemoprophylaxis are low. This study sought to use thromboelastography (TEG) to compare coagulation profiles with bleeding/thrombotic events in HPB patients receiving standardized perioperative chemoprophylaxis.
Methods: Consecutive patients undergoing HPB resections by three surgeons at one institution (January 2014-December 2015) received preoperative and early postoperative VTE chemoprophylaxis and were evaluated with TEGs.
We have measured the angular distributions of high energy photoelectrons of benzene molecules generated by intense infrared femtosecond laser pulses. These electrons arise from the elastic collisions between the benzene ions with the previously tunnel-ionized electrons that have been driven back by the laser field. Theory shows that laser-free elastic differential cross sections (DCSs) can be extracted from these photoelectrons, and the DCS can be used to retrieve the bond lengths of gas-phase molecules similar to the conventional electron diffraction method.
View Article and Find Full Text PDFThe putative goal of surveillance is the early detection of recurrence while both the cancer and patient are still treatable. To be cost and clinically effective, surveillance requires a tailored approach based on stage, tumor biology, conditional survival, and available treatment options. Although surveillance is the major component of care for cancer patients after potentially curative treatment, current guidelines for surveillance lack the high-level data seen on the treatment side of the patient care continuum.
View Article and Find Full Text PDFWe discuss a scheme to retrieve transient conformational molecular structure information using photoelectron angular distributions (PADs) that have averaged over partial alignments of isolated molecules. The photoelectron is pulled out from a localized inner-shell molecular orbital by an X-ray photon. We show that a transient change in the atomic positions from their equilibrium will lead to a sensitive change in the alignment-averaged PADs, which can be measured and used to retrieve the former.
View Article and Find Full Text PDFImaging the transient process of molecules has been a basic way to investigate photochemical reactions and dynamics. Based on laser-induced electron diffraction and partial one-dimensional molecular alignment, here we provide two effective methods for reconstructing two-dimensional structure of polyatomic molecules. We demonstrate that electron diffraction images in both scattering angles and broadband energy can be utilized to retrieve complementary structure information, including positions of light atoms.
View Article and Find Full Text PDFLaser-induced electron diffraction is an evolving tabletop method that aims to image ultrafast structural changes in gas-phase polyatomic molecules with sub-Ångström spatial and femtosecond temporal resolutions. Here we demonstrate the retrieval of multiple bond lengths from a polyatomic molecule by simultaneously measuring the C-C and C-H bond lengths in aligned acetylene. Our approach takes the method beyond the hitherto achieved imaging of simple diatomic molecules and is based on the combination of a 160 kHz mid-infrared few-cycle laser source with full three-dimensional electron-ion coincidence detection.
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