FEL2015 - Classification: FEL Applications

Paper

Title

Page

Lebra Free-Electron Laser Elicits Electrical Spikes from the Retina and Optic Nerve of the Slugs Limax Valentianus

550

F. Shishikura, K. Hayakawa, Y. Hayakawa, M. Inagaki, K. Nakao, K. Nogami, T. Sakai, T. Tanaka
LEBRA, Funabashi, Japan
Y. Komatsuzaki
Nihon University, Tokyo, Japan

Since 2001, the Laboratory for Electron Beam Research and Application (LEBRA) has been providing tunable free-electron lasers (FELs) encompassing the near-IR region and some of the mid-IR region (0.9-6 microns), and generating visible wavelengths up to 400 nm by means of nonlinear optical crystals. We are investigating the efficiency of LEBRA-FELs for triggering photoreactions in living organisms. Last year we described the effects of LEBRA-FELs in controlling the photoreaction of lettuce seeds; red FEL (660 nm) and far-red FEL (740 nm) activate and inhibit germination, respectively. Here we used LEBRA-FEL to illuminate the retina of slugs (Limax valentianus), and determined which FEL wavelengths generate electrical spikes from the retina-optic nerve. Blue FEL light (wavelength: 470 nm) efficiently produced electrical spikes from the retina. The results are consistent with a previous study, where a xenon arc lamp with interference filters was used to produce monochromatic visible light. We plan to extend the wavelengths to the near- and mid-IR regions of LEBRA-FEL. We summarize our current results for the use of FEL in investigating the electrophysiology of the retina of slugs.
We thank Mr. T. Kuwabara (a graduate of Departments of Physics, College of Science and Technolgy, Nihon University) for helpful assistance.

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WEP010

Development of Phonon Dynamics Measurement System by MIR-FEL and Pico-second Laser

615

T. Murata, T. Katsurayama, T. Kii, T. Konstantin, K. Masuda, T. Nogi, H. Ohgaki, S. Suphakul, K. Torgasin, H. Zen
Kyoto University, Kyoto, Japan
K. Hachiya
Kyoto University Graduate School of Energy Science, Kyoto, Japan
K. Yoshida
Kumamoto University, Department of Applied Chemistry and Biochemistry, Kumamoto, Japan

Coherent control of a lattice vibration in bulk solid (mode-selective phonon excitation: MSPE) is one of the attractive methods in the solid state physics because it becomes a powerful tool for the study of ultrafast lattice dynamics (e.g. electron-phonon interaction and phonon-phonon interaction). Not only for that, MSPE can control electronic, magnetic, and structural phases of materials. In 2013, we have directly demonstrated MSPE of a bulk material with MIR-FEL (KU-FEL) by anti-Stokes Raman scattering spectroscopy. For the next step, we are starting a phonon dynamics measurement to investigate the difference of physical property between thermally excited phonon (phonon of equilibrium state) and optically excited phonon (phonon of non-equilibrium state) by time-resolved method in combination with a pico-second VIS laser. By using pico-second laser, we also expect to perform the anti-Stokes hyper-Raman scattering spectroscopy to extend MSPE method to the phonon mode which has Raman inactive . As the first step, we have commissioned the time-resolved phonon measurement system and started measurement on 6H-SiC. In this conference, we will present the outline of measurement system, and experimental results.

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FRA01

Radiation Damage Free Structure of Photosystem II at 1.95A Resolution

M. Suga, F. Akita, Y. Nakajima, J.R. Shen, T. Shimizu
Okayama University, Okayama, Japan
H. Ago, K. Hirata, H. Murakami, G. Ueno, M. Yamamoto, K. Yamashita
JASRI/RIKEN, Hyogo, Japan

The initial reaction of photosynthesis takes place in Photosystem II (PSII), a 700kD membrane protein complex which catalyses photo-oxidation of water into dioxygen through an S-state cycle of the oxygen evolving complex (OEC). The structure of PSII has been solved by XRD at 1.9Å resolution, which revealed the OEC is a Mn4CaO5-cluster*. However, EXAFS studies showed that the manganese atoms in the OEC are easily reduced by X-ray irradiation, and slight differences were found in the Mn-Mn distances between the results of XRD, EXAFS and theoretical studies. We present a radiation-damage-free structure of PSII from Thermosynechococcus vulcanus in the S1 state at 1.95Å resolution using femtosecond X-ray pulses of SACLA. Compared with the structure from XRD, the OEC in the XFEL structure has Mn-Mn distances that are shorter by 0.1-0.2Å. The valences of each manganese atom were assigned as Mn1D(III), Mn2C(IV), Mn3B(IV) and Mn4A(III). One of the oxo-bridged oxygens, O5, has significantly longer Mn-O distances in contrast to the other oxo-oxygen atoms, suggesting that it is a hydroxide ion instead of a normal oxygen dianion and therefore may serve as one of the substrate oxygen atoms**.
* Y. Umena et al., Nature, 473(7545): 55-60 (2011).
** M. Suga et al., Nature, 517(7532): 99-103 (2015).

Slides FRA01 [135.184 MB]

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FRA02

Direct Observation of Bond Formation in Solution with Femtosecond X-Ray Scattering

K.H. Kim
IBS, Daejeon, Republic of Korea
H. Ihee, J.G. Kim
KAIST, Daejeon, Republic of Korea

Funding: This work was supported by IBS-R004-G2.
Bond breaking and bond making are essential processes in chemical reactions. While ultrafast dynamics of bond breaking have been studied intensively using time time-resolved techniques, it is challenging to keep track of structural dynamics of bond making due to its bimolecular nature. Time-resolved X-ray liquidography (TRXL) has been developed by using the X-ray pulse, instead of optical pulse, as a probe and gives the time-resolved scattering response sensitive to global molecular structure.(*, **) The time resolution of 3rd generation source is 100 ps and due to this limited time resolution, ultrafast structural dynamics involved in ultrafast excited-state dynamics and direct observation of bond-breaking and -making processes cannot yet be accomplished with TRXL. This limit is improved with X-ray free electron lasers (XFELs), which deliver 100 fs long X-ray pulses with ~10¹³ photons per pulse. With the advent of X-ray free electron laser (XFEL) generating ultrashort X-ray pulses, the exploration of chemical processes occurring on femtosecond time scale with pump-probe X-ray solution scattering is possible. With the aid of 4th generation X-ray sources (SACLA, Japan), ultrafast tight Au-Au bond formation process of [Au(CN)2-]3 oligomer upon 267 nm laser excitation was directly observed using TRXL.
* K.H. Kim et al., Nature, 2015, 518, 385-389.
** H. Ihee et al., Science, 2005, 309, 1223-1227.

Slides FRA02 [29.203 MB]

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FRA03

Where are the Electrons? New Opportunities for Mapping Local Chemical Interaction Dynamics with Time-resolved Soft X-ray Spectroscopy at FELs

Ph. Wernet
HZB, Berlin, Germany

Photochemically activated molecules catalyze chemical reactions, but a molecular-level understanding of how these short-lived and reactive intermediates catalyze reactions has remained elusive. I will discuss how time-resolved soft x-ray spectroscopy at free-electron lasers enables a fundamental understanding of local atomic and intermolecular interactions and their dynamics b on atomic length and time scales of Ångströms and femtoseconds[1]. In a recent application[2], we used femtosecond resonant inelastic x-ray scattering (RIXS) at the LINAC Coherent Light Source (LCLS, Stanford, USA)[3] to probe the reaction dynamics of the benchmark transition-metal complex Fe(CO)5 in solution. This highlights the ability of femtosecond soft x-ray spectroscopy at free-electron lasers to probe frontier-orbital interactions with atom specificity. I will end by discussing how the currently available methodology can be extended towards probing complex biomolecules in physiological conditions[4]. I will show how in particular high-repetition rate x-ray free-electron laser sources such as the planned LCLS-II will enable probing the local chemistry and it dynamical evolution in metalloproteins.
[1] Ph. Wernet. Phys. Chem. Chem. Phys. 13, 16941 (2011).
[2] Ph. Wernet et al., Nature, 520, 78-81 (2015).
[3] K. Kunnus et al., Rev. Sci. Instrum. 83, 123109 (2012).
[4] R. Mitzner et al., J. Phys. Chem. Lett. 4, 3641 (2013).

Slides FRA03 [61.138 MB]

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FRA04

Measurements and Future Prospects for Coherent Control with FEL Radiation

K.C. Prince
Elettra-Sincrotrone Trieste S.C.p.A., Basovizza, Italy

FELs produce ultrafast, intense, polarised and coherent pulses of light, similar to optical lasers, and these properties have been exploited in FEL experiments, with one exception, namely longitudinal coherence. There have been few if any FEL applications of this property. The FERMI FEL is longitudinally coherent, and can be configured to produce simultaneous, different wavelengths which are mutually coherent, with a well-defined phase relationship. We have exploited this in recent experiments to produce overlapping pulses of first and second harmonic light with a tunable phase delay, and perform an experiment on neon atoms. The first harmonic was set to about 63 nm and high intensity, and the second harmonic to lower intensity and half of this wavelength. The first harmonic gave rise to two-photon photoemission, while the second harmonic caused single photon emission. At appropriate relative intensities of the two beams, the emitted photoelectrons interfered to give asymmetric angular distributions (Brumer-Shapiro type experiment.) The asymmetry depended on the value of the phase difference between the two wavelengths, thus demonstrating their correlation in phase. The relative phase was controlled with a precision of 3 attoseconds. This result opens the way to coherent control experiments in the short wavelength region, and some planned applications will be illustrated.

Slides FRA04 [4.216 MB]

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Paper	Title	Page
TUP085	Lebra Free-Electron Laser Elicits Electrical Spikes from the Retina and Optic Nerve of the Slugs Limax Valentianus	550
	F. Shishikura, K. Hayakawa, Y. Hayakawa, M. Inagaki, K. Nakao, K. Nogami, T. Sakai, T. Tanaka LEBRA, Funabashi, Japan Y. Komatsuzaki Nihon University, Tokyo, Japan
	Since 2001, the Laboratory for Electron Beam Research and Application (LEBRA) has been providing tunable free-electron lasers (FELs) encompassing the near-IR region and some of the mid-IR region (0.9-6 microns), and generating visible wavelengths up to 400 nm by means of nonlinear optical crystals. We are investigating the efficiency of LEBRA-FELs for triggering photoreactions in living organisms. Last year we described the effects of LEBRA-FELs in controlling the photoreaction of lettuce seeds; red FEL (660 nm) and far-red FEL (740 nm) activate and inhibit germination, respectively. Here we used LEBRA-FEL to illuminate the retina of slugs (Limax valentianus), and determined which FEL wavelengths generate electrical spikes from the retina-optic nerve. Blue FEL light (wavelength: 470 nm) efficiently produced electrical spikes from the retina. The results are consistent with a previous study, where a xenon arc lamp with interference filters was used to produce monochromatic visible light. We plan to extend the wavelengths to the near- and mid-IR regions of LEBRA-FEL. We summarize our current results for the use of FEL in investigating the electrophysiology of the retina of slugs. We thank Mr. T. Kuwabara (a graduate of Departments of Physics, College of Science and Technolgy, Nihon University) for helpful assistance.
Export •	reference for this paper to ※ LaTeX, ※ Text, ※ IS/RefMan, ※ EndNote (xml)

WEP010	Development of Phonon Dynamics Measurement System by MIR-FEL and Pico-second Laser	615
	T. Murata, T. Katsurayama, T. Kii, T. Konstantin, K. Masuda, T. Nogi, H. Ohgaki, S. Suphakul, K. Torgasin, H. Zen Kyoto University, Kyoto, Japan K. Hachiya Kyoto University Graduate School of Energy Science, Kyoto, Japan K. Yoshida Kumamoto University, Department of Applied Chemistry and Biochemistry, Kumamoto, Japan
	Coherent control of a lattice vibration in bulk solid (mode-selective phonon excitation: MSPE) is one of the attractive methods in the solid state physics because it becomes a powerful tool for the study of ultrafast lattice dynamics (e.g. electron-phonon interaction and phonon-phonon interaction). Not only for that, MSPE can control electronic, magnetic, and structural phases of materials. In 2013, we have directly demonstrated MSPE of a bulk material with MIR-FEL (KU-FEL) by anti-Stokes Raman scattering spectroscopy. For the next step, we are starting a phonon dynamics measurement to investigate the difference of physical property between thermally excited phonon (phonon of equilibrium state) and optically excited phonon (phonon of non-equilibrium state) by time-resolved method in combination with a pico-second VIS laser. By using pico-second laser, we also expect to perform the anti-Stokes hyper-Raman scattering spectroscopy to extend MSPE method to the phonon mode which has Raman inactive . As the first step, we have commissioned the time-resolved phonon measurement system and started measurement on 6H-SiC. In this conference, we will present the outline of measurement system, and experimental results.
Export •	reference for this paper to ※ LaTeX, ※ Text, ※ IS/RefMan, ※ EndNote (xml)

FRA01	Radiation Damage Free Structure of Photosystem II at 1.95A Resolution
	M. Suga, F. Akita, Y. Nakajima, J.R. Shen, T. Shimizu Okayama University, Okayama, Japan H. Ago, K. Hirata, H. Murakami, G. Ueno, M. Yamamoto, K. Yamashita JASRI/RIKEN, Hyogo, Japan
	The initial reaction of photosynthesis takes place in Photosystem II (PSII), a 700kD membrane protein complex which catalyses photo-oxidation of water into dioxygen through an S-state cycle of the oxygen evolving complex (OEC). The structure of PSII has been solved by XRD at 1.9Å resolution, which revealed the OEC is a Mn4CaO5-cluster. However, EXAFS studies showed that the manganese atoms in the OEC are easily reduced by X-ray irradiation, and slight differences were found in the Mn-Mn distances between the results of XRD, EXAFS and theoretical studies. We present a radiation-damage-free structure of PSII from Thermosynechococcus vulcanus in the S1 state at 1.95Å resolution using femtosecond X-ray pulses of SACLA. Compared with the structure from XRD, the OEC in the XFEL structure has Mn-Mn distances that are shorter by 0.1-0.2Å. The valences of each manganese atom were assigned as Mn1D(III), Mn2C(IV), Mn3B(IV) and Mn4A(III). One of the oxo-bridged oxygens, O5, has significantly longer Mn-O distances in contrast to the other oxo-oxygen atoms, suggesting that it is a hydroxide ion instead of a normal oxygen dianion and therefore may serve as one of the substrate oxygen atoms. Y. Umena et al., Nature, 473(7545): 55-60 (2011). ** M. Suga et al., Nature, 517(7532): 99-103 (2015).
	Slides FRA01 [135.184 MB]
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FRA02	Direct Observation of Bond Formation in Solution with Femtosecond X-Ray Scattering
	K.H. Kim IBS, Daejeon, Republic of Korea H. Ihee, J.G. Kim KAIST, Daejeon, Republic of Korea
	Funding: This work was supported by IBS-R004-G2. Bond breaking and bond making are essential processes in chemical reactions. While ultrafast dynamics of bond breaking have been studied intensively using time time-resolved techniques, it is challenging to keep track of structural dynamics of bond making due to its bimolecular nature. Time-resolved X-ray liquidography (TRXL) has been developed by using the X-ray pulse, instead of optical pulse, as a probe and gives the time-resolved scattering response sensitive to global molecular structure.(, ) The time resolution of 3rd generation source is 100 ps and due to this limited time resolution, ultrafast structural dynamics involved in ultrafast excited-state dynamics and direct observation of bond-breaking and -making processes cannot yet be accomplished with TRXL. This limit is improved with X-ray free electron lasers (XFELs), which deliver 100 fs long X-ray pulses with ~10¹³ photons per pulse. With the advent of X-ray free electron laser (XFEL) generating ultrashort X-ray pulses, the exploration of chemical processes occurring on femtosecond time scale with pump-probe X-ray solution scattering is possible. With the aid of 4th generation X-ray sources (SACLA, Japan), ultrafast tight Au-Au bond formation process of [Au(CN)2-]3 oligomer upon 267 nm laser excitation was directly observed using TRXL. K.H. Kim et al., Nature, 2015, 518, 385-389. ** H. Ihee et al., Science, 2005, 309, 1223-1227.
	Slides FRA02 [29.203 MB]
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FRA03	Where are the Electrons? New Opportunities for Mapping Local Chemical Interaction Dynamics with Time-resolved Soft X-ray Spectroscopy at FELs
	Ph. Wernet HZB, Berlin, Germany
	Photochemically activated molecules catalyze chemical reactions, but a molecular-level understanding of how these short-lived and reactive intermediates catalyze reactions has remained elusive. I will discuss how time-resolved soft x-ray spectroscopy at free-electron lasers enables a fundamental understanding of local atomic and intermolecular interactions and their dynamics b on atomic length and time scales of Ångströms and femtoseconds[1]. In a recent application[2], we used femtosecond resonant inelastic x-ray scattering (RIXS) at the LINAC Coherent Light Source (LCLS, Stanford, USA)[3] to probe the reaction dynamics of the benchmark transition-metal complex Fe(CO)5 in solution. This highlights the ability of femtosecond soft x-ray spectroscopy at free-electron lasers to probe frontier-orbital interactions with atom specificity. I will end by discussing how the currently available methodology can be extended towards probing complex biomolecules in physiological conditions[4]. I will show how in particular high-repetition rate x-ray free-electron laser sources such as the planned LCLS-II will enable probing the local chemistry and it dynamical evolution in metalloproteins. [1] Ph. Wernet. Phys. Chem. Chem. Phys. 13, 16941 (2011). [2] Ph. Wernet et al., Nature, 520, 78-81 (2015). [3] K. Kunnus et al., Rev. Sci. Instrum. 83, 123109 (2012). [4] R. Mitzner et al., J. Phys. Chem. Lett. 4, 3641 (2013).
	Slides FRA03 [61.138 MB]
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FRA04	Measurements and Future Prospects for Coherent Control with FEL Radiation
	K.C. Prince Elettra-Sincrotrone Trieste S.C.p.A., Basovizza, Italy
	FELs produce ultrafast, intense, polarised and coherent pulses of light, similar to optical lasers, and these properties have been exploited in FEL experiments, with one exception, namely longitudinal coherence. There have been few if any FEL applications of this property. The FERMI FEL is longitudinally coherent, and can be configured to produce simultaneous, different wavelengths which are mutually coherent, with a well-defined phase relationship. We have exploited this in recent experiments to produce overlapping pulses of first and second harmonic light with a tunable phase delay, and perform an experiment on neon atoms. The first harmonic was set to about 63 nm and high intensity, and the second harmonic to lower intensity and half of this wavelength. The first harmonic gave rise to two-photon photoemission, while the second harmonic caused single photon emission. At appropriate relative intensities of the two beams, the emitted photoelectrons interfered to give asymmetric angular distributions (Brumer-Shapiro type experiment.) The asymmetry depended on the value of the phase difference between the two wavelengths, thus demonstrating their correlation in phase. The relative phase was controlled with a precision of 3 attoseconds. This result opens the way to coherent control experiments in the short wavelength region, and some planned applications will be illustrated.
	Slides FRA04 [4.216 MB]
Export •	reference for this paper to ※ LaTeX, ※ Text, ※ IS/RefMan, ※ EndNote (xml)