Taran Driver

All Publications

• Fragment Correlation Mass Spectrometry Enables Direct Characterization of Disulfide Bond Cleavage Pathways of Therapeutic Peptides. Analytical chemistry Li, Y., Cavet, G., Zare, R. N., Driver, T. 2024

  Abstract

  Therapeutic peptides that are connected by disulfide bonds are often difficult to analyze by traditional tandem mass spectrometry without chemical modification. Using fragment correlation mass spectrometry, we analyzed 56 pairs of fragment ions generated from an equimolar (10 μM) mixture of three cyclic peptides, achieving sequence coverage of 86%, 100%, and 75% for octreotide, desmopressin, and the structural analogue of desmopressin, respectively. In all detected fragment ion pairs, only 20% of the fragment ions are terminal ions, with most of the measured ions only detected by fragment correlation mass spectrometry. From the peak volumes in the covariance map, we calculated branching ratios of each disulfide bond fragmentation pathway, providing a direct measurement of the probability of each fragmentation without requiring alteration of the chemical structure of the analytes.

  View details for DOI 10.1021/acs.analchem.4c03202

  View details for PubMedID 39248333

• Fragment correlation mass spectrometry: Determining the structures of biopolymers in a complex mixture without isolating individual components. Proceedings of the National Academy of Sciences of the United States of America Li, Y., Cavet, G., Zare, R. N., Driver, T. 2024; 121 (32): e2409676121

  Abstract

  Fragment correlation mass spectrometry correlates ion pairs generated from the same fragmentation pathway, achieved by covariance mapping of tandem mass spectra generated with an unmodified linear ion trap without preseparation. We enable the identification of different precursors at different charge states in a complex mixture from a large isolation window, empowering an analytical approach for data-independent acquisition. The method resolves and matches isobaric fragments, internal ions, and disulfide bond fragments. We suggest that this method represents a major advance for analyzing structures of biopolymers in mixtures.

  View details for DOI 10.1073/pnas.2409676121

  View details for PubMedID 39074273

• Attosecond delays in X-ray molecular ionization. Nature Driver, T., Mountney, M., Wang, J., Ortmann, L., Al-Haddad, A., Berrah, N., Bostedt, C., Champenois, E. G., DiMauro, L. F., Duris, J., Garratt, D., Glownia, J. M., Guo, Z., Haxton, D., Isele, E., Ivanov, I., Ji, J., Kamalov, A., Li, S., Lin, M. F., Marangos, J. P., Obaid, R., O'Neal, J. T., Rosenberger, P., Shivaram, N. H., Wang, A. L., Walter, P., Wolf, T. J., Wörner, H. J., Zhang, Z., Bucksbaum, P. H., Kling, M. F., Landsman, A. S., Lucchese, R. R., Emmanouilidou, A., Marinelli, A., Cryan, J. P. 2024; 632 (8026): 762-767

  Abstract

  The photoelectric effect is not truly instantaneous but exhibits attosecond delays that can reveal complex molecular dynamics1-7. Sub-femtosecond-duration light pulses provide the requisite tools to resolve the dynamics of photoionization8-12. Accordingly, the past decade has produced a large volume of work on photoionization delays following single-photon absorption of an extreme ultraviolet photon. However, the measurement of time-resolved core-level photoionization remained out of reach. The required X-ray photon energies needed for core-level photoionization were not available with attosecond tabletop sources. Here we report measurements of the X-ray photoemission delay of core-level electrons, with unexpectedly large delays, ranging up to 700 as in NO near the oxygen K-shell threshold. These measurements exploit attosecond soft X-ray pulses from a free-electron laser to scan across the entire region near the K-shell threshold. Furthermore, we find that the delay spectrum is richly modulated, suggesting several contributions, including transient trapping of the photoelectron owing to shape resonances, collisions with the Auger-Meitner electron that is emitted in the rapid non-radiative relaxation of the molecule and multi-electron scattering effects. The results demonstrate how X-ray attosecond experiments, supported by comprehensive theoretical modelling, can unravel the complex correlated dynamics of core-level photoionization.

  View details for DOI 10.1038/s41586-024-07771-9

  View details for PubMedID 39169246

  View details for PubMedCentralID 7399650

• Terawatt-scale attosecond X-ray pulses from a cascaded superradiant free-electron laser NATURE PHOTONICS Franz, P., Li, S., Driver, T., Robles, R. R., Cesar, D., Isele, E., Guo, Z., Wang, J., Duris, J. P., Larsen, K., Glownia, J. M., Cheng, X., Hoffmann, M. C., Li, X., Lin, M., Kamalov, A., Obaid, R., Summers, A., Sudar, N., Thierstein, E., Zhang, Z., Kling, M. F., Huang, Z., Cryan, J. P., Marinelli, A. 2024

  View details for DOI 10.1038/s41566-024-01427-w

  View details for Web of Science ID 001220935700001

• Experimental demonstration of attosecond pump-probe spectroscopy with an X-ray free-electron laser NATURE PHOTONICS Guo, Z., Driver, T., Beauvarlet, S., Cesar, D., Duris, J., Franz, P. L., Alexander, O., Bohler, D., Bostedt, C., Averbukh, V., Cheng, X., Dimauro, L. F., Doumy, G., Forbes, R., Gessner, O., Glownia, J. M., Isele, E., Kamalov, A., Larsen, K. A., Li, S., Li, X., Lin, M., Mccracken, G. A., Obaid, R., O'Neal, J. T., Robles, R. R., Rolles, D., Ruberti, M., Rudenko, A., Slaughter, D. S., Sudar, N. S., Thierstein, E., Tuthill, D., Ueda, K., Wang, E., Wang, A. L., Wang, J., Weber, T., Wolf, T. A., Young, L., Zhang, Z., Bucksbaum, P. H., Marangos, J. P., Kling, M. F., Huang, Z., Walter, P., Inhester, L., Berrah, N., Cryan, J. P., Marinelli, A. 2024

  View details for DOI 10.1038/s41566-024-01419-w

  View details for Web of Science ID 001200371400001

• Compact single-shot soft X-ray photon spectrometer for free-electron laser diagnostics OPTICS EXPRESS Larsen, K. A., Borne, K., Obaid, R., Kamalov, A., Liu, Y., Cheng, X., James, J., Driver, T., Li, K., Liu, Y., Sakdinawat, A., David, C., Wolf, T. A., Cryan, J. P., Walter, P., Lin, M. 2023; 31 (22): 35822-35834

  Abstract

  The photon spectrum from free-electron laser (FEL) light sources offers valuable information in time-resolved experiments and machine optimization in the spectral and temporal domains. We have developed a compact single-shot photon spectrometer to diagnose soft X-ray spectra. The spectrometer consists of an array of off-axis Fresnel zone plates (FZP) that act as transmission-imaging gratings, a Ce:YAG scintillator, and a microscope objective to image the scintillation target onto a two-dimensional imaging detector. This spectrometer operates in segmented energy ranges which covers tens of electronvolts for each absorption edge associated with several atomic constituents: carbon, nitrogen, oxygen, and neon. The spectrometer's performance is demonstrated at a repetition rate of 120 Hz, but our detection scheme can be easily extended to 200 kHz spectral collection by employing a fast complementary metal oxide semiconductor (CMOS) line-scan camera to detect the light from the scintillator. This compact photon spectrometer provides an opportunity for monitoring the spectrum downstream of an endstation in a limited space environment with sub-electronvolt energy resolution.

  View details for DOI 10.1364/OE.502105

  View details for Web of Science ID 001106418000001

  View details for PubMedID 38017746

• X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS₂ COMMUNICATIONS PHYSICS Unwin, J., Allum, F., Britton, M., Gabalski, I., Bromberger, H., Brouard, M., Bucksbaum, P. H., Driver, T., Ekanayake, N., Garg, D., Gougoula, E., Heathcote, D., Howard, A. J., Hockett, P., Holland, D. P., Kumar, S., Lam, C., Lee, J. L., Mcmanus, J., Mikosch, J., Milesevic, D., Minns, R. S., Papadopoulou, C. C., Passow, C., Razmus, W. O., Roeder, A., Rouzee, A., Schuurman, M., Simao, A., Stolow, A., Tul-Noor, A., Vallance, C., Walmsley, T., Rolles, D., Erk, B., Burt, M., Forbes, R. 2023; 6 (1)

  View details for DOI 10.1038/s42005-023-01414-7

  View details for Web of Science ID 001095830300001

• Time-Resolved X-ray Photoelectron Spectroscopy: Ultrafast Dynamics in CS2 Probed at the S 2p Edge. The journal of physical chemistry letters Gabalski, I., Allum, F., Seidu, I., Britton, M., Brenner, G., Bromberger, H., Brouard, M., Bucksbaum, P. H., Burt, M., Cryan, J. P., Driver, T., Ekanayake, N., Erk, B., Garg, D., Gougoula, E., Heathcote, D., Hockett, P., Holland, D. M., Howard, A. J., Kumar, S., Lee, J. W., Li, S., McManus, J., Mikosch, J., Milesevic, D., Minns, R. S., Neville, S., Papadopoulou, C. C., Passow, C., Razmus, W. O., Röder, A., Rouzée, A., Simao, A., Unwin, J., Vallance, C., Walmsley, T., Wang, J., Rolles, D., Stolow, A., Schuurman, M. S., Forbes, R. 2023: 7126-7133

  Abstract

  Recent developments in X-ray free-electron lasers have enabled a novel site-selective probe of coupled nuclear and electronic dynamics in photoexcited molecules, time-resolved X-ray photoelectron spectroscopy (TRXPS). We present results from a joint experimental and theoretical TRXPS study of the well-characterized ultraviolet photodissociation of CS2, a prototypical system for understanding non-adiabatic dynamics. These results demonstrate that the sulfur 2p binding energy is sensitive to changes in the nuclear structure following photoexcitation, which ultimately leads to dissociation into CS and S photoproducts. We are able to assign the main X-ray spectroscopic features to the CS and S products via comparison to a first-principles determination of the TRXPS based on ab initio multiple-spawning simulations. Our results demonstrate the use of TRXPS as a local probe of complex ultrafast photodissociation dynamics involving multimodal vibrational coupling, nonradiative transitions between electronic states, and multiple final product channels.

  View details for DOI 10.1021/acs.jpclett.3c01447

  View details for PubMedID 37534743

• Effect of the shot-to-shot variation on charge migration induced by sub-fs x-ray free-electron laser pulses PHYSICAL REVIEW RESEARCH Grell, G., Guo, Z., Driver, T., Decleva, P., Plesiat, E., Picon, A., Gonzalez-Vazquez, J., Walter, P., Marangos, J. P., Cryan, J. P., Marinelli, A., Palacios, A., Martin, F. 2023; 5 (2)

  View details for DOI 10.1103/PhysRevResearch.5.023092

  View details for Web of Science ID 000995777100002

• Photon energy-resolved velocity map imaging from spectral domain ghost imaging NEW JOURNAL OF PHYSICS Wang, J., Driver, T., Allum, F., Papadopoulou, C. C., Passow, C., Brenner, G., Li, S., Duesterer, S., Tul Noor, A., Kumar, S., Bucksbaum, P. H., Erk, B., Forbes, R., Cryan, J. P. 2023; 25 (3)

  View details for DOI 10.1088/1367-2630/acc201

  View details for Web of Science ID 000956244500001

• Disentangling sequential and concerted fragmentations of molecular polycations with covariant native frame analysis. Physical chemistry chemical physics : PCCP McManus, J. W., Walmsley, T., Nagaya, K., Harries, J. R., Kumagai, Y., Iwayama, H., Ashfold, M. N., Britton, M., Bucksbaum, P. H., Downes-Ward, B., Driver, T., Heathcote, D., Hockett, P., Howard, A. J., Kukk, E., Lee, J. W., Liu, Y., Milesevic, D., Minns, R. S., Niozu, A., Niskanen, J., Orr-Ewing, A. J., Owada, S., Rolles, D., Robertson, P. A., Rudenko, A., Ueda, K., Unwin, J., Vallance, C., Burt, M., Brouard, M., Forbes, R., Allum, F. 2022

  Abstract

  We present results from an experimental ion imaging study into the fragmentation dynamics of 1-iodopropane and 2-iodopropane following interaction with extreme ultraviolet intense femtosecond laser pulses with a photon energy of 95 eV. Using covariance imaging analysis, a range of observed fragmentation pathways of the resulting polycations can be isolated and interrogated in detail at relatively high ion count rates (12 ions shot-1). By incorporating the recently developed native frames analysis approach into the three-dimensional covariance imaging procedure, contributions from three-body concerted and sequential fragmentation mechanisms can be isolated. The angular distribution of the fragment ions is much more complex than in previously reported studies for triatomic polycations, and differs substantially between the two isomeric species. With support of simple simulations of the dissociation channels of interest, detailed physical insights into the fragmentation dynamics are obtained, including how the initial dissociation step in a sequential mechanism influences rovibrational dynamics in the metastable intermediate ion and how signatures of this nuclear motion manifest in the measured signals.

  View details for DOI 10.1039/d2cp03029b

  View details for PubMedID 36106844

• The time-resolved atomic, molecular and optical science instrument at the Linac Coherent Light Source. Journal of synchrotron radiation Walter, P., Osipov, T., Lin, M. F., Cryan, J., Driver, T., Kamalov, A., Marinelli, A., Robinson, J., Seaberg, M. H., Wolf, T. J., Aldrich, J., Brown, N., Champenois, E. G., Cheng, X., Cocco, D., Conder, A., Curiel, I., Egger, A., Glownia, J. M., Heimann, P., Holmes, M., Johnson, T., Lee, L., Li, X., Moeller, S., Morton, D. S., Ng, M. L., Ninh, K., O'Neal, J. T., Obaid, R., Pai, A., Schlotter, W., Shepard, J., Shivaram, N., Stefan, P., Van, X., Wang, A. L., Wang, H., Yin, J., Yunus, S., Fritz, D., James, J., Castagna, J. C. 2022; 29 (Pt 4): 957-968

  Abstract

  The newly constructed time-resolved atomic, molecular and optical science instrument (TMO) is configured to take full advantage of both linear accelerators at SLAC National Accelerator Laboratory, the copper accelerator operating at a repetition rate of 120 Hz providing high per-pulse energy as well as the superconducting accelerator operating at a repetition rate of about 1 MHz providing high average intensity. Both accelerators power a soft X-ray free-electron laser with the new variable-gap undulator section. With this flexible light source, TMO supports many experimental techniques not previously available at LCLS and will have two X-ray beam focus spots in line. Thereby, TMO supports atomic, molecular and optical, strong-field and nonlinear science and will also host a designated new dynamic reaction microscope with a sub-micrometer X-ray focus spot. The flexible instrument design is optimized for studying ultrafast electronic and molecular phenomena and can take full advantage of the sub-femtosecond soft X-ray pulse generation program.

  View details for DOI 10.1107/S1600577522004283

  View details for PubMedID 35787561

• Characterization of single-shot attosecond pulses with angular streaking photoelectron spectra PHYSICAL REVIEW A Zhao, X., Li, S., Driver, T., Van-Hung Hoang, Anh-Thu Le, Cryan, J. P., Marinelli, A., Lin, C. D. 2022; 105 (1)

  View details for DOI 10.1103/PhysRevA.105.013111

  View details for Web of Science ID 000747560000006

• Attosecond coherent electron motion in Auger-Meitner decay. Science (New York, N.Y.) Li, S., Driver, T., Rosenberger, P., Champenois, E. G., Duris, J., Al-Haddad, A., Averbukh, V., Barnard, J. C., Berrah, N., Bostedt, C., Bucksbaum, P. H., Coffee, R. N., DiMauro, L. F., Fang, L., Garratt, D., Gatton, A., Guo, Z., Hartmann, G., Haxton, D., Helml, W., Huang, Z., LaForge, A. C., Kamalov, A., Knurr, J., Lin, M., Lutman, A. A., MacArthur, J. P., Marangos, J. P., Nantel, M., Natan, A., Obaid, R., O'Neal, J. T., Shivaram, N. H., Schori, A., Walter, P., Wang, A. L., Wolf, T. J., Zhang, Z., Kling, M. F., Marinelli, A., Cryan, J. P. 1800: eabj2096

  Abstract

  [Figure: see text].

  View details for DOI 10.1126/science.abj2096

  View details for PubMedID 34990213

• The development of attosecond XFELs for understanding ultrafast electron motion ADVANCES IN ATOMIC, MOLECULAR, AND OPTICAL PHYSICS, VOL. 71 Cryan, J. P., Driver, T., Duris, J., Guo, Z., Li, S., O'Neal, J. T., Marinelli, A., DiMauro, L. F., Perrin, H., Yelin, S. F. 2022; 71: 1-64

  View details for DOI 10.1016/bs.aamop.2022.05.001

  View details for Web of Science ID 000877680100002

• Multi-resolution electron spectrometer array for future free-electron laser experiments. Journal of synchrotron radiation Walter, P., Kamalov, A., Gatton, A., Driver, T., Bhogadi, D., Castagna, J. C., Cheng, X., Shi, H., Obaid, R., Cryan, J., Helml, W., Ilchen, M., Coffee, R. N. 2021; 28 (Pt 5): 1364-1376

  Abstract

  The design of an angular array of electron time-of-flight (eToF) spectrometers is reported, intended for non-invasive spectral, temporal, and polarization characterization of single shots of high-repetition rate, quasi-continuous, short-wavelength free-electron lasers (FELs) such as the LCLS II at SLAC. This array also enables angle-resolved, high-resolution eToF spectroscopy to address a variety of scientific questions on ultrafast and nonlinear light-matter interactions at FELs. The presented device is specifically designed for the time-resolved atomic, molecular and optical science endstation (TMO) at LCLS II. In its final version, the spectrometer comprises up to 20 eToF spectrometers aligned to collect electrons from the interaction point, which is defined by the intersection of the incoming FEL radiation and a gaseous target. The full composition involves 16 spectrometers forming a circular equiangular array in the plane normal to the X-ray propagation and four spectrometers at 54.7° angle relative to the principle linear X-ray polarization axis with orientations in the forward and backward direction of the light propagation. The spectrometers are capable of independent and minimally chromatic electrostatic lensing and retardation, in order to enable simultaneous angle-resolved photo- and Auger-Meitner electron spectroscopy with high energy resolution. They are designed to ensure an energy resolution of 0.25 eV across an energy window of up to 75 eV, which can be individually centered via the adjustable retardation to cover the full range of electron kinetic energies relevant to soft X-ray methods, 0-2 keV. The full spectrometer array will enable non-invasive and online spectral-polarimetry measurements, polarization-sensitive attoclock spectroscopy for characterizing the full time-energy structure of SASE or seeded LCLS II pulses, and support emerging trends in molecular-frame spectroscopy measurements.

  View details for DOI 10.1107/S1600577521007700

  View details for PubMedID 34475285

• Chimera Spectrum Diagnostics for Peptides Using Two-Dimensional Partial Covariance Mass Spectrometry MOLECULES Driver, T., Bachhawat, N., Frasinski, L. J., Marangos, J. P., Averbukh, V., Edelson-Averbukh, M. 2021; 26 (12)

  Abstract

  The rate of successful identification of peptide sequences by tandem mass spectrometry (MS/MS) is adversely affected by the common occurrence of co-isolation and co-fragmentation of two or more isobaric or isomeric parent ions. This results in so-called `chimera spectra', which feature peaks of the fragment ions from more than a single precursor ion. The totality of the fragment ion peaks in chimera spectra cannot be assigned to a single peptide sequence, which contradicts a fundamental assumption of the standard automated MS/MS spectra analysis tools, such as protein database search engines. This calls for a diagnostic method able to identify chimera spectra to single out the cases where this assumption is not valid. Here, we demonstrate that, within the recently developed two-dimensional partial covariance mass spectrometry (2D-PC-MS), it is possible to reliably identify chimera spectra directly from the two-dimensional fragment ion spectrum, irrespective of whether the co-isolated peptide ions are isobaric up to a finite mass accuracy or isomeric. We introduce '3-57 chimera tag' technique for chimera spectrum diagnostics based on 2D-PC-MS and perform numerical simulations to examine its efficiency. We experimentally demonstrate the detection of a mixture of two isomeric parent ions, even under conditions when one isomeric peptide is at one five-hundredth of the molar concentration of the second isomer.

  View details for DOI 10.3390/molecules26123728

  View details for Web of Science ID 000666733800001

  View details for PubMedID 34207274

  View details for PubMedCentralID PMC8234510

• Multi-channel photodissociation and XUV-induced charge transfer dynamics in strong-field-ionized methyl iodide studied with time-resolved recoil-frame covariance imaging. Faraday discussions Allum, F., Anders, N., Brouard, M., Bucksbaum, P., Burt, M., Downes-Ward, B., Grundmann, S., Harries, J., Ishimura, Y., Iwayama, H., Kaiser, L., Kukk, E., Lee, J., Liu, X., Minns, R. S., Nagaya, K., Niozu, A., Niskanen, J., O'Neal, J., Owada, S., Pickering, J., Rolles, D., Rudenko, A., Saito, S., Ueda, K., Vallance, C., Werby, N., Woodhouse, J., You, D., Ziaee, F., Driver, T., Forbes, R. 2021

  Abstract

  The photodissociation dynamics of strong-field ionized methyl iodide (CH3I) were probed using intense extreme ultraviolet (XUV) radiation produced by the SPring-8 Angstrom Compact free electron LAser (SACLA). Strong-field ionization and subsequent fragmentation of CH3I was initiated by an intense femtosecond infrared (IR) pulse. The ensuing fragmentation and charge transfer processes following multiple ionization by the XUV pulse at a range of pump-probe delays were followed in a multi-mass ion velocity-map imaging (VMI) experiment. Simultaneous imaging of a wide range of resultant ions allowed for additional insight into the complex dynamics by elucidating correlations between the momenta of different fragment ions using time-resolved recoil-frame covariance imaging analysis. The comprehensive picture of the photodynamics that can be extracted provides promising evidence that the techniques described here could be applied to study ultrafast photochemistry in a range of molecular systems at high count rates using state-of-the-art advanced light sources.

  View details for DOI 10.1039/d0fd00115e

  View details for PubMedID 33629700

• Time-resolved pump-probe spectroscopy with spectral domain ghost imaging. Faraday discussions Li, S., Driver, T., Alexander, O., Cooper, B., Garratt, D., Marinelli, A., Cryan, J. P., Marangos, J. P. 2021

  Abstract

  An atomic-level picture of molecular and bulk processes, such as chemical bonding and charge transfer, necessitates an understanding of the dynamical evolution of these systems. On the ultrafast timescales associated with nuclear and electronic motion, the temporal behaviour of a system is often interrogated in a 'pump-probe' scheme. Here, an initial 'pump' pulse triggers dynamics through photoexcitation, and after a carefully controlled delay a 'probe' pulse initiates projection of the instantaneous state of the evolving system onto an informative measurable quantity, such as electron binding energy. In this paper, we apply spectral ghost imaging to a pump-probe time-resolved experiment at an X-ray free-electron laser (XFEL) facility, where the observable is spectral absorption in the X-ray regime. By exploiting the correlation present in the shot-to-shot fluctuations in the incoming X-ray pulses and measured electron kinetic energies, we show that spectral ghost imaging can be applied to time-resolved pump-probe measurements. In the experiment presented, interpretation of the measurement is simplified because spectral ghost imaging separates the overlapping contributions to the photoelectron spectrum from the pump and probe pulse.

  View details for DOI 10.1039/d0fd00122h

  View details for PubMedID 33625412

• Inner Valence Hole Migration in Isopropanol Alexander, O., Barillot, T., Cooper, B., Driver, T., Garratt, D., Li, S., Marinelli, A., Cryan, J. P., Marangos, J. P., LR25 Collaboration, IEEE IEEE. 2021

  View details for DOI 10.1109/CLEO/Europe-EQEC52157.2021.9542202

  View details for Web of Science ID 000728078300580

• Tunable isolated attosecond X-ray pulses with gigawatt peak power from a free-electron laser NATURE PHOTONICS Duris, J., Li, S., Driver, T., Champenois, E. G., MacArthur, J. P., Lutman, A. A., Zhang, Z., Rosenberger, P., Aldrich, J. W., Coffee, R., Coslovich, G., Decker, F., Glownia, J. M., Hartmann, G., Helml, W., Kamalov, A., Knurr, J., Krzywinski, J., Lin, M., Nantel, M., Natan, A., O'Neal, J., Shivaram, N., Walter, P., Wang, A., Welch, J. J., Wolf, T. A., Xu, J. Z., Kling, M. F., Bucksbaum, P. H., Zholents, A., Huang, Z., Cryan, J. P., Marinelli, A., Marangos, J. P. 2020; 14 (1): 30-+

  View details for DOI 10.1038/s41566-019-0549-5

  View details for Web of Science ID 000504727600007

• Attosecond transient absorption spooktroscopy: a ghost imaging approach to ultrafast absorption spectroscopy. Physical chemistry chemical physics : PCCP Driver, T., Li, S., Champenois, E. G., Duris, J., Ratner, D., Lane, T. J., Rosenberger, P., Al-Haddad, A., Averbukh, V., Barnard, T., Berrah, N., Bostedt, C., Bucksbaum, P. H., Coffee, R., DiMauro, L. F., Fang, L., Garratt, D., Gatton, A., Guo, Z., Hartmann, G., Haxton, D., Helml, W., Huang, Z., LaForge, A., Kamalov, A., Kling, M. F., Knurr, J., Lin, M., Lutman, A. A., MacArthur, J. P., Marangos, J. P., Nantel, M., Natan, A., Obaid, R., O'Neal, J. T., Shivaram, N. H., Schori, A., Walter, P., Li Wang, A., Wolf, T. J., Marinelli, A., Cryan, J. P. 2019

  Abstract

  The recent demonstration of isolated attosecond pulses from an X-ray free-electron laser (XFEL) opens the possibility for probing ultrafast electron dynamics at X-ray wavelengths. An established experimental method for probing ultrafast dynamics is X-ray transient absorption spectroscopy, where the X-ray absorption spectrum is measured by scanning the central photon energy and recording the resultant photoproducts. The spectral bandwidth inherent to attosecond pulses is wide compared to the resonant features typically probed, which generally precludes the application of this technique in the attosecond regime. In this paper we propose and demonstrate a new technique to conduct transient absorption spectroscopy with broad bandwidth attosecond pulses with the aid of ghost imaging, recovering sub-bandwidth resolution in photoproduct-based absorption measurements.

  View details for DOI 10.1039/c9cp03951a

  View details for PubMedID 31793561

• Negative Ion Mode Collision-Induced Dissociation for Analysis of Protein Arginine Methylation JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY Katsanovskaja, K., Driver, T., Pipkorn, R., Edelson-Averbukh, M. 2019; 30 (7): 1229–41

  Abstract

  Arginine methylation is a common protein post-translational modification (PTM) that plays a key role in eukaryotic cells. Three distinct types of this modification are found in mammals: asymmetric Nη1Nη1-dimethylarginine (aDMA), symmetric Nη1Nη2-dimethylarginine (sDMA), and an intermediate Nη1-monomethylarginine (MMA). Elucidation of regulatory mechanisms of arginine methylation in living organisms requires precise information on both the type of the modified residues and their location inside the protein amino acid sequences. Despite mass spectrometry (MS) being the method of choice for analysis of multiple protein PTMs, unambiguous characterization of protein arginine methylation may not be always straightforward. Indeed, frequent internal basic residues of Arg methylated tryptic peptides hamper their sequencing under positive ion mode collision-induced dissociation (CID), the standardly used tandem mass spectrometry method, while the relative stability of the aDMA and sDMA side chains under alternative non-ergodic electron-based fragmentation techniques, electron-capture and electron transfer dissociations (ECD and ETD), may impede differentiation between the isobaric residues. Here, for the first time, we demonstrate the potential of the negative ion mode collision-induced dissociation MS for analysis of protein arginine methylation and present data revealing that the negative polarity approach can deliver both an unambiguous identification of the arginine methylation type and extensive information on the modified peptide sequences.

  View details for DOI 10.1007/s13361-019-02176-9

  View details for Web of Science ID 000472938000012

  View details for PubMedID 30915654

  View details for PubMedCentralID PMC6591203

• Partial covariance two-dimensional mass spectrometry for determination of biomolecular primary structure arXiv:1904.05946 Driver, T., Ayers, R., Pipkorn, R., Cooper, B., Bachhawat, N., Patchkovskii, S., Averbukh, V., Klug, D. R., Marangos, J. P., Frasinski, L. J., Edelson-Averbukh, M. 2019
• Generation and Characterization of Attosecond Pulses from an X-ray Free-electron Laser Li, S., Rosenberger, P., Champenois, E. G., Driver, T., Bucksbaum, P. H., Coffee, R., Gatton, A., Hartmann, G., Helml, W., Huang, Z., Knurr, J., Kling, M. F., Lin, M., MacArthur, J. P., Maxwell, T. J., Nantel, M., Natan, A., Oneal, J. T., Shivaram, N. H., Walter, P., Wolf, T. A., Cryan, J. P., Marinelli, A., IEEE IEEE. 2019

  View details for Web of Science ID 000482226301273

• Angle-resolved coherent wave mixing using a 4 fs ultra-broad bandwidth laser OPTICS LETTERS Mercer, I. P., Witting, T., Driver, T., Cogdell, R. J., Marangos, J. P., Tisch, J. G. 2017; 42 (4): 859–62

  Abstract

  We demonstrate angle-resolved coherent (ARC) wave mixing using 4 fs light pulses derived from a laser source that spans 550-1000 nm. We believe this to be the shortest pulse duration used to date in coherent multi-dimensional spectroscopy. The marriage of this ultra-broad band, few-cycle coherent source with the ARC technique will permit new investigations of the interplay between energy transfers and quantum superposition states spanning 8200  cm^-1. We applied this configuration to measurements on the photosynthetic low light (LL) complex from Rhodopseudomonas palustris in solution at ambient temperature. We observe bi-exponential population dynamics for energy transfer across 5500  cm^-1 (0.65 eV), which we attribute to energy transfer from the Q_x transition of bacteriochlorophylls to the B850 pigment of the complex. We believe for the first time, to the best of our knowledge, we demonstrate that ARC maps can be recorded using a single laser pulse.

  View details for DOI 10.1364/OL.42.000859

  View details for Web of Science ID 000394039500052

  View details for PubMedID 28198883