This work was supported in part by grants-in-aid KAKENHI from the Japan Society for the Promotion of Science (JSPS) and the Ministry of Education, Culture, Sports, Science, and Technology (MEXT) Japan (#26104539, #26620020, #26810011, #15H03766, #15KT0060, #16H00826, and #16K13927); the Konica Minolta Science and Technology Foundation; the "Planting Seeds for Research" program of TokyoTech; the Imaging Science Project of the Center for Novel Science Initiatives (CNSI) at the National Institutes of Natural Sciences (NINS) (#IS261006); the RIKEN-IMS joint program on "Extreme Photonics;" and the Consortium for Photon Science and Technology (CPhoST).

<ol><li>Stapelfeldt, H., Constant, E., Sakai, H., Corkum, P. B. <a target="_blank" href="http://journals.aps.org/pra/abstract/10.1103/PhysRevA.58.426">Time-resolved Coulomb explosion imaging: A method to measure structure and dynamics of molecular nuclear wave packets.</a> Phys. Rev. A. 58, 426-433 (1998).</li>
<li>Hishikawa, A., Matsuda, A., Fushitani, M., Takahashi, E. J. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/pubmed?term=((Visualizing+Recurrently+Migrating+Hydrogen+in+Acetylene+Dication+by+Intense+Ultrashort+Laser+Pulses%5BTitle%5D)+AND+%22Phys.+Rev.+Lett%22%5BJournal%5D)">Visualizing Recurrently Migrating Hydrogen in Acetylene Dication by Intense Ultrashort Laser Pulses.</a> Phys. Rev. Lett. 99, 258302(2007).</li>
<li>Légaré, F., et al. <a target="_blank" href="http://journals.aps.org/pra/abstract/10.1103/PhysRevA.71.013415">Laser Coulomb-explosion imaging of small molecules.</a> Phys. Rev. A. 71, 013415(2005).</li>
<li>Stapelfeldt, H., Seideman, T. <a target="_blank" href="http://journals.aps.org/rmp/abstract/10.1103/RevModPhys.75.543">Colloquium: Aligning molecules with strong laser pulses.</a> Rev. Mod. Phys. 75, 543-557 (2003).</li>
<li>Ohshima, Y., Hasegawa, H. <a target="_blank" href="http://www.tandfonline.com/doi/abs/10.1080/0144235X.2010.511769">Coherent rotational excitation by intense nonresonant laser fields.</a> Int. Rev. Phys. Chem. 29, 619-663 (2010).</li>
<li>Kitano, K., Hasegawa, H., Ohshima, Y. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/pubmed?term=((Ultrafast+Angular+Momentum+Orientation+by+Linearly+Polarized+Laser+Fields%5BTitle%5D)+AND+%22Phys.+Rev.+Lett%22%5BJournal%5D)">Ultrafast Angular Momentum Orientation by Linearly Polarized Laser Fields.</a> Phys. Rev. Lett. 103, 223002(2009).</li>
<li>Fleischer, S., Khodorkovsky, Y., Prior, Y., Averbukh, I. S. <a target="_blank" href="https://arxiv.org/abs/1012.1253">Controlling the sense of molecular rotation.</a> New J. Phys. 11, 105039(2009).</li>
<li>Korobenko, A., Milner, A. A., Milner, V. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/pubmed?term=((Direct+Observation%2C+Study%2C+and+Control+of+Molecular+Superrotors%5BTitle%5D)+AND+%22Phys.+Rev.+Lett%22%5BJournal%5D)">Direct Observation, Study, and Control of Molecular Superrotors.</a> Phys. Rev. Lett. 112, 113004(2014).</li>
<li>Rosca-Pruna, F., Vrakking, M. J. J. <a target="_blank" href="http://aip.scitation.org/doi/abs/10.1063/1.1458537">Revival structures in picosecond laser-induced alignment of I2 molecules. I. Experimental results.</a> J. Chem. Phys. 116, 6567-6578 (2002).</li>
<li>Dooley, P. W., et al. <a target="_blank" href="http://journals.aps.org/pra/abstract/10.1103/PhysRevA.68.023406">Direct imaging of rotational wave-packet dynamics of diatomic molecules.</a> Phys. Rev. A. 68, 023406(2003).</li>
<li>Mizuse, K., Kitano, K., Hasegawa, H., Ohshima, Y. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/pubmed?term=((Quantum+unidirectional+rotation+directly+imaged+with+molecules%5BTitle%5D)+AND+%22Sci.+Adv%22%5BJournal%5D)">Quantum unidirectional rotation directly imaged with molecules.</a> Sci. Adv. 1, 1400185(2015).</li>
<li>Lin, K., et al. <a target="_blank" href="http://journals.aps.org/pra/abstract/10.1103/PhysRevA.92.013410">Visualizing molecular unidirectional rotation.</a> Phys. Rev. A. 92, 013410(2015).</li>
<li>Korobenko, A., Hepburn, J. W., Milner, V. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/pubmed?term=((Observation+of+nondispersing+classical-like+molecular+rotation%5BTitle%5D)+AND+%22Phys.+Chem.+Chem.+Phys%22%5BJournal%5D)">Observation of nondispersing classical-like molecular rotation.</a> Phys. Chem. Chem. Phys. 17, 951-956 (2015).</li>
<li>Whitaker, B. J. <a target="_blank" href="http://scholar.google.com/scholar?hl=en&safe=off&q=author%3aWhitaker%2C+BJ+%22Imaging+in+Molecular+Dynamics%22">Imaging in Molecular Dynamics</a>. , Cambridge University Press. (2003).</li>
<li>Ullrich, J., et al. <a target="_blank" href="http://iopscience.iop.org/article/10.1088/0034-4885/66/9/203/meta">Recoil-ion and electron momentum spectroscopy: reaction-microscopes.</a> Rep. Prog. Phys. 66, 1463(2003).</li>
<li>Lee, S. K., et al. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/pubmed?term=((Coincidence+ion+imaging+with+a+fast+frame+camera%5BTitle%5D)+AND+%22Rev+Sci+Instrum%22%5BJournal%5D)">Coincidence ion imaging with a fast frame camera.</a> Rev Sci Instrum. 85, 123303(2014).</li>
<li>Lee, S. K., et al. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/pubmed?term=((Communication%3A+Time-+and+space-sliced+velocity+map+electron+imaging%5BTitle%5D)+AND+%22J.+Chem.+Phys%22%5BJournal%5D)">Communication: Time- and space-sliced velocity map electron imaging.</a> J. Chem. Phys. 141, 221101(2014).</li>
<li>John, J. J., et al. <a target="_blank" href="http://iopscience.iop.org/article/10.1088/1748-0221/7/08/C08001/meta">PImMS, a fast event-triggered monolithic pixel detector with storage of multiple timestamps.</a> Journal of Instrumentation. 7, 8001(2012).</li>
<li>Nomerotski, A., et al. <a target="_blank" href="http://iopscience.iop.org/article/10.1088/1748-0221/5/07/C07007">Pixel Imaging Mass Spectrometry with fast and intelligent Pixel detectors.</a> Journal of Instrumentation. 5, 07007(2010).</li>
<li>Luria, K., Christen, W., Even, U. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/pubmed?term=((Generation+and+Propagation+of+Intense+Supersonic+Beams%5BTitle%5D)+AND+%22J.+Phys.+Chem.+A%22%5BJournal%5D)">Generation and Propagation of Intense Supersonic Beams.</a> J. Phys. Chem. A. 115, 7362-7367 (2011).</li>
<li>Eppink, A. T. J. B., Parker, D. H. <a target="_blank" href="http://aip.scitation.org/doi/abs/10.1063/1.1148310">Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen.</a> Rev. Sci. Instrum. 68, 3477-3484 (1997).</li>
<li>Gebhardt, C. R., Rakitzis, T. P., Samartzis, P. C., Ladopoulos, V., Kitsopoulos, T. N. <a target="_blank" href="http://aip.scitation.org/doi/abs/10.1063/1.1403010">Slice imaging: A new approach to ion imaging and velocity mapping.</a> Rev. Sci. Instrum. 72, 3848(2001).</li>
<li>Stöhr, J. <a target="_blank" href="http://scholar.google.com/scholar?hl=en&safe=off&q=author%3aSt%C3%B6hr%2C+J+%22NEXAFS+Spectroscopy%22">NEXAFS Spectroscopy</a>. , Springer. 132(1992).</li>
<li>Siders, C. W., Siders, J. L. W., Taylor, A. J., Park, S. -G., Weiner, A. M. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/pubmed?term=((Efficient+High-Energy+Pulse-Train+Generation+Using+a+2+n-Pulse+Michelson+Interferometer%5BTitle%5D)+AND+%22Appl.+Opt%22%5BJournal%5D)">Efficient High-Energy Pulse-Train Generation Using a 2 n-Pulse Michelson Interferometer.</a> Appl. Opt. 37, 5302-5305 (1998).</li>
<li>Pitzer, M., et al. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/pubmed?term=((Direct+Determination+of+Absolute+Molecular+Stereochemistry+in+Gas+Phase+by+Coulomb+Explosion+Imaging%5BTitle%5D)+AND+%22Science%22%5BJournal%5D)">Direct Determination of Absolute Molecular Stereochemistry in Gas Phase by Coulomb Explosion Imaging.</a> Science. 341, 1096-1100 (2013).</li>
<li>Rakitzis, T. P., Samartzis, P. C., Kitsopoulos, T. N. <a target="_blank" href="http://aip.scitation.org/doi/10.1063/1.480396">Observing the symmetry breaking in the angular distributions of oriented photofragments using velocity mapping.</a> J. Chem. Phys. 111, 10415(1999).</li>
<li>Chang, B. -Y., Hoetzlein, R. C., Mueller, J. A., Geiser, J. D., Houston, P. L. <a target="_blank" href="http://aip.scitation.org/doi/10.1063/1.1148824">Improved two-dimensional product imaging: The real-time ion-counting method.</a> Rev. Sci. Instrum. 69, 1665(1998).</li>
<li>Wiley, W. C., McLaren, I. H. <a target="_blank" href="http://aip.scitation.org/doi/abs/10.1063/1.1715212">Time-of-Flight Mass Spectrometer with Improved Resolution.</a> Rev. Sci. Instrum. 26, 1150(1955).</li>
<li>Townsend, D., Minitti, M. P., Suits, A. G. <a target="_blank" href="http://aip.scitation.org/doi/10.1063/1.1544053">Direct current slice imaging.</a> Rev. Sci. Instrum. 74, 2530(2003).</li>
<li>Wu, G., et al. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/pubmed?term=((A+new+crossed+molecular+beam+apparatus+using+time-sliced+ion+velocity+imaging+technique%5BTitle%5D)+AND+%22Rev.+Sci.+Instrum%22%5BJournal%5D)">A new crossed molecular beam apparatus using time-sliced ion velocity imaging technique.</a> Rev. Sci. Instrum. 79, 094104(2008).</li>
<li>Treacy, E. <a target="_blank" href="http://ieeexplore.ieee.org/document/1076303/">Optical pulse compression with diffraction gratings.</a> Quantum Electronics, IEEE Journal of. 5, 454-458 (1969).</li>
<li>Dörner, R., et al. <a target="_blank" href="http://www.sciencedirect.com/science/article/pii/S037015739900109X">Cold Target Recoil Ion Momentum Spectroscopy: a 'momentum microscope' to view atomic collision dynamics.</a> Physics Reports. 330, 95-192 (2000).</li>
<li>Herwig, P., et al. <a target="_blank" href="http://www.ncbi.nlm.nih.gov/pubmed?term=((Imaging+the+Absolute+Configuration+of+a+Chiral+Epoxide+in+the+Gas+Phase%5BTitle%5D)+AND+%22Science%22%5BJournal%5D)">Imaging the Absolute Configuration of a Chiral Epoxide in the Gas Phase.</a> Science. 342, 1084-1086 (2013).</li>
<li>Suzuki, Y. -I., Suzuki, T. <a target="_blank" href="http://journals.aps.org/pra/abstract/10.1103/PhysRevA.91.053413">Linear and circular dichroism in photoelectron angular distributions caused by electron correlation.</a> Phys. Rev. A. 91, 053413(2015).</li>
</ol>

The authors have nothing to disclose.

Das vorliegende Verfahren ermöglicht es uns, eine Echtzeit-Film der molekularen Rotation mit einem Schlitz-basierte 2D-Imaging-Setup zu erfassen. Da die beobachteten Ionen durch den Schlitz passieren, Schritt 1.5 ist einer der entscheidenden Schritte. Die Ränder der Schlitz Messer müssen scharf sein. Wenn es einen kleinen Defekt, wie beispielsweise ein 0,3 mm Loch in dem Schlitz wird ein Kratzer in der Ionenbild (Abbildung 6) beobachtet. In einem solchen Fall sollte die Spaltklinge mit 2.000-Körnung...

Für ein tieferes Verständnis und eine bessere Nutzung der dynamischen Natur von Molekülen, ist es wichtig, klar zu molekularen Bewegungen von Interesse zu visualisieren. Zeitaufgelöste Coulomb Explosion Imaging ist eine der leistungsfähigen Ansätze dieses Ziel 1, 3 2, zu erreichen. In diesem Ansatz werden die Molekulardynamik von Interesse durch eine Pumpe ultrakurzen Laserfeld initiiert und werden dann durch eine zeitverzögerte Abtastimpuls sondiert. Bei der Sonde Bestrahlung werden Moleküle mehrfach ionisiert und in Fragmentionen aufgrund der Coulomb-Abstoßung gebrochen. Die räumliche Verteilung der ausgestoßenen Ionen ist ein Maß für die molekulare Struktur und die räumliche Orientierung an der Sondenbestrahlung. Eine Folge von Mess Abtasten der Pump-Probe-Verzögerungszeit führt zur Schaffung eines molekularen Films. Es ist bemerkenswert, dass für den einfachsten Fall - zweiatomigen Molekülen - die Winkelverteilung der ausgestoßenen Ionendirekt spiegelt die Molekülachse Verteilung (dh die quadriert Drehwellenfunktion). Im Hinblick auf den Pumpvorgang, die jüngsten Fortschritte bei der kohärenten Kontrolle der Molekularbewegung mit ultrakurzen Laserfeldern hat zur Schaffung geführt von stark kontrollierten Drehwellenpakete 4, 5. Weiterhin kann die Drehrichtung aktiv durch die Verwendung eines polarisationsgesteuerten Laserfeld 6, 7, 8 gesteuert werden. Es ist daher zu erwarten, dass ein detailliertes Bild der molekularen Rotation, einschließlich Wellen Naturen, sichtbar gemacht werden konnte , wenn die Coulomb - Explosion Abbildungstechnik mit einer solchen Pumpvorgang 9 kombiniert wird, 10, 11, 12, 13. Allerdings haben wir einigemal begegnen experimentellen Schwierigkeiten mit den bestehenden bildgebenden Verfahren verbunden sind, wie unten erwähnt. Der Zweck dieses Papiers ist es, einen neuen Weg zur Überwindung dieser Schwierigkeiten zu präsentieren und einen qualitativ hochwertigen Film von molekularen Drehwellenpaketen zu schaffen. Die erste experimentelle Film der molekularen Rotation mit dem vorliegenden Verfahren genommen, zusammen mit ihrer physischen Auswirkungen wurden in unseren früheren Papier 11 dargestellt. Der Hintergrund der Entwicklung, die detaillierten theoretischen Aspekt der vorliegenden Bildgebungstechnik, und ein Vergleich mit anderen Techniken wird in einer der nächsten Papier gegeben werden. Hier werden wir in erster Linie konzentrieren sich auf die praktischen und technischen Aspekte des Verfahrens, einschließlich der Kombination der typischen Pump-Probe-optischen Aufbau und die neue Bildgebungsgerät. Wie in der früheren Arbeit wird das Zielsystem unidirektional rotierenden Stickstoffmoleküle 11. Die wichtigsten experimentellen Schwierigkeiten derbestehenden Abbildungseinrichtung, die schematisch in 1 gezeigt ist , hat mit der Position des Detektors oder der Kamerawinkel zu tun. Weil die Drehachse mit der Laserausbreitungseinstimmt Achse 6, 7, 8 in laserfeldinduzierte Molekülrotation ist es nicht praktisch , einen Detektor entlang der Drehachse anzubringen. Wenn der Detektor installiert ist, um die Laserbestrahlung zu vermeiden, entspricht die Kamerawinkel einer Seiten Beobachtung der Rotation. In diesem Fall ist es unmöglich , die ursprüngliche Orientierung von Molekülen aus dem projizierten (2D) Ionenbild 14 zu rekonstruieren. Eine 3D - Bilddetektor 14, 15, 16, 17, 18, 19, mit denen die Ankunftszeit an der oberen Detektor und das Ionen impact Positionen gemessen werden, bot eine einzigartige Möglichkeit, direkt molekularen Rotation beobachten 10 unter Verwendung von Coulomb Explosion Imaging, 12. Jedoch sind die akzeptablen ion counts per Laserschuß niedrig (typisch &lt;10 Ionen) in dem 3D - Detektor, was bedeutet , dass es schwierig ist , einen langen Film der Molekularbewegung mit hoher Bildqualität 14 zu schaffen. Die Totzeit der Detektoren (typischerweise ns) wirkt sich auch auf die Bildauflösung und Bildbearbeitungseffizienz. Es ist auch keine einfache Aufgabe durch Überwachung eines Echtzeit-Ionenbild mit einer Laserwiederholungsrate von &lt;~ 1 kHz eine gute Pumpsondenstrahl überlappen zu lassen. Obwohl mehrere Gruppen Drehwellenpakete die 3D - Technik beobachtet haben, wurde die räumliche Information beschränkt und / oder direkte und eine detaillierte Darstellung der Wellennatur, einschließlich komplizierte Knotenstrukturen, nicht 10 erreicht, 12. Das Wesen derdie neue Imaging - Technik ist die Verwendung des &quot;neuen Kamerawinkel&quot; in Abbildung 1. In dieser Konfiguration Belichtungslaserstrahl zu einem Detektor vermieden wird, während die 2D-Detektor zur Rotationsebene parallel ist, zu der Beobachtung, von der Drehachsenrichtung führt. Der Schlitz erlaubt nur die Ionen in der Rotationsebene (die Polarisationsebene der Laserpulse) zu einem Bild beitragen. Ein 2D-Detektor, die eine höhere Zählrate (typischerweise ~ 100-Ionen) als ein 3D-Detektor bietet, kann verwendet werden. Der Aufbau der Elektronik ist einfacher als im Fall der 3D-Erkennung, während die Messeffizienz höher ist. Zeitaufwendige mathematischen Rekonstruktion, wie Abel Inversion 14 wird auch Winkelinformationen zu extrahieren , nicht benötigt werden . Diese Eigenschaften führen zu der einfachen Optimierung des Messsystems und auf die Herstellung von qualitativ hochwertigen Filmen. Ein Standard-2D / 3D-geladener Teilchen Bildgebungsgerät kann leicht an die vorliegende Einrichtung witho geändert werdenut die Verwendung teurer Ausrüstung.

<table><tbody><tr><td>CMOS camera</td><td>Toshiba TELI</td><td>BU-238M-ES</td><td>equipped with SONY IMX174 sensor</td></tr><tr><td>High voltage switch</td><td>Behlke</td><td>HTS-41-03-GSM</td><td></td></tr><tr><td>High voltage switch</td><td>Behlke</td><td>HTS-80-03</td><td></td></tr><tr><td>Digital delay generator</td><td>Stanford research systems</td><td>DG535</td><td></td></tr><tr><td>Digital delay generator</td><td>Stanford research systems</td><td>DG645</td><td></td></tr><tr><td>Microchannel plate</td><td>Photonis</td><td>3075</td><td></td></tr><tr><td>Pulsed valve</td><td>LAMID LTD</td><td>Even-Lavie valve&amp;nbsp;</td><td>High repetition, room temperature model</td></tr><tr><td>Molecular beam skimmers</td><td>Institute for Molecular Science</td><td>13C11</td><td>3 and 1.5 mm center hole, 25 degrees full inner angle, and ~50 mm length</td></tr><tr><td>Optical Comparator</td><td>Nikon</td><td>V-24B</td><td></td></tr><tr><td>DPSS laser</td><td>Lighthouse Photonics</td><td>Sprout</td><td></td></tr><tr><td>Femtosecond Ti:Sapphire oscillator</td><td>KMLabs</td><td>Halcyon</td><td></td></tr><tr><td>Femtosecond Ti:Sapphire amplifier</td><td>Quantronix</td><td>Odin-II HE</td><td></td></tr><tr><td>Motorized linear stage</td><td>Sigma Koki</td><td>KST(GS)-100X</td><td></td></tr><tr><td>Manual X-stage</td><td>Sigma Koki</td><td>TSD-601S</td><td></td></tr><tr><td>High resolution mirror mount</td><td>Newport</td><td>Suprema SX100-F2KN-254</td><td></td></tr><tr><td>High resolution mirror mount</td><td>LIOP-TEC GmbH</td><td>SR100-100R-2-HS</td><td></td></tr><tr><td>Polarization checker</td><td>Paradigm Devices, Inc.</td><td>O-tool VIS</td><td></td></tr><tr><td>Instrument communication interface</td><td>National Instruments</td><td>NI-MAX</td><td></td></tr><tr><td>Graphical development environment for measurement programs</td><td>National Instruments</td><td>LabVIEW 2014</td><td></td></tr><tr><td>Laser line dielectric mirror</td><td>CVI/LEO</td><td>TLM2-400/800-45UNP</td><td></td></tr><tr><td>Laser line dielectric mirror</td><td>Altechna</td><td>Low GDD Ultrafast mirror</td><td></td></tr><tr><td>Laser line dielectric mirror</td><td>Altechna</td><td>Low GDD Ultrafast mirror</td><td></td></tr><tr><td>Femtosecond polarizer</td><td>Advanced Thin Films</td><td>PBS-GVD</td><td></td></tr></tbody></table>

direct imaging of laser-driven ultrafast molecular rotation

Wir stellen eine Methode zur Visualisierung von laserinduzierten, ultraschnelle molekulare Drehwellenpaketdynamik. Wir haben ein neues 2-dimensionale Coulomb Explosion Imaging-Setup entwickelt, in denen ein bisher nicht praktikabel-Kamerawinkel realisiert wird. In unserer Imaging-Technik, zweiatomigen Moleküle werden mit einem zirkular polarisierten starken Laserpuls bestrahlt. Die ausgestoßenen Atomionen sind senkrecht zu der Laserausbreitungs beschleunigt. Die Ionen in der Laserpolarisationsebene liegen, werden durch die Verwendung eines mechanischen Schlitz ausgewählt, und mit einem Hochdurchsatz abgebildet wird, 2-dimensionalen Detektor installiert parallel zur Polarisationsebene. Weil ein zirkular polarisiertes (isotrop) Coulomb explodierenden Impuls verwendet wird, entspricht die beobachtete Winkelverteilung der ausgestoßenen Ionen direkt auf die quadrierten Rotationswellenfunktion zur Zeit der Pulsbestrahlung. Um eine Echtzeit-Film der molekularen Rotation, die vorliegende Abbildungstechnik schaffen mit einem Femtosekunden-Pump-Probe-o kombiniertptical Einrichtung, in der die Pumpimpulse schaffen rotierenden unidirektional molekularen Ensembles. Aufgrund der hohen Bild Durchsatz unseres Nachweissystems kann die Pump-Probe experimentellen Bedingungen leicht durch Überwachung eines Echtzeit-Momentaufnahme optimiert werden. Als Ergebnis ist die Qualität des beobachteten Film ausreichend hoch, um die detaillierte Wellennatur der Bewegung für die Visualisierung. Wir stellen ferner fest, dass die vorliegende Technik in bestehende Standard-Ionen-Imaging-Setups implementiert werden, eine neue Kamerawinkel oder Blickwinkel für die molekularen Systemen, ohne die Notwendigkeit für umfangreiche Änderungen an.

4A zeigt eine Sonden nur rohes Bild der N 2+ -Ionen ausgeworfen der Sonden Bestrahlung (Coulomb - Explosion), genommen für eine Sonde Laserschuss. Jeder helle Punkt entspricht einem Ion. 4B zeigt eine summierte Bild von 10.000 binarisiert RAW - Kamerabilder. Diese Bilder zeigen, dass unsere Imaging-Setup die Moleküle aller Orientierungswinkel in der Polarisationsebene zu überwachen. 4C zeigt die normierte Polarplot d...

Watch this Scientific Journal Video about Direct Imaging of Laser-driven Ultrafast Molecular Rotation at JoVE.com

Direct Imaging of Laser-driven Ultrafast Molecular Rotation

We present a protocol for creating a real-time movie of a molecular rotational wave packet using a high-resolution Coulomb explosion imaging setup.

Direct Imaging von lasergetriebenen Ultrakurz Molecular Rotation

We present a method for visualizing laser-induced, ultrafast molecular rotational wave packet dynamics. We have developed a new 2-dimensional Coulomb ...

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9.7K Aufrufe.  Tokyo Institute of Technology. We present a protocol for creating a real-time movie of a molecular rotational wave packet using a high-resolution Coulomb explosion imaging setup.

Serie: Direct Imaging of Laser-driven Ultrafast Molecular Rotation

Fluorescence Lifetime Imaging of Molecular Rotors in Living Cells

Diffusion is often an important rate-determining step in chemical reactions or biological processes and plays a role in a wide range of intracellular events. Viscosity is one of the key parameters affecting the diffusion of molecules and proteins, and changes in viscosity have been linked to disease and malfunction at the cellular level.1-3 While methods to measure the bulk viscosity are well developed, imaging microviscosity remains a challenge. Viscosity maps of microscopic objects, such as single cells, have until recently been hard to obtain. Mapping viscosity with fluorescence techniques is advantageous because, similar to other optical techniques, it is minimally invasive, non-destructive and can be applied to living cells and tissues.
Fluorescent molecular rotors exhibit fluorescence lifetimes and quantum yields which are a function of the viscosity of their microenvironment.4,5 Intramolecular twisting or rotation leads to non-radiative decay from the excited state back to the ground state. A viscous environment slows this rotation or twisting, restricting access to this non-radiative decay pathway. This leads to an increase in the fluorescence quantum yield and the fluorescence lifetime. Fluorescence Lifetime Imaging (FLIM) of modified hydrophobic BODIPY dyes that act as fluorescent molecular rotors show that the fluorescence lifetime of these probes is a function of the microviscosity of their environment.6-8 A logarithmic plot of the fluorescence lifetime versus the solvent viscosity yields a straight line that obeys the F&ouml;rster Hoffman equation.9 This plot also serves as a calibration graph to convert fluorescence lifetime into viscosity.
Following incubation of living cells with the modified BODIPY fluorescent molecular rotor, a punctate dye distribution is observed in the fluorescence images. The viscosity value obtained in the puncta in live cells is around 100 times higher than that of water and of cellular cytoplasm.6,7 Time-resolved fluorescence anisotropy measurements yield rotational correlation times in agreement with these large microviscosity values. Mapping the fluorescence lifetime is independent of the fluorescence intensity, and thus allows the separation of probe concentration and viscosity effects. 
In summary, we have developed a practical and versatile approach to map the microviscosity in cells based on FLIM of fluorescent molecular rotors.

Fluorescence Lifetime Imaging (FLIM) has emerged as a key technique to image the environment and interaction of specific proteins and dyes in living cells. FLIM of fluorescent molecular rotors allows mapping of viscosity in living cells.

Fluorescence Lifetime Imaging für molekulare Rotoren in lebenden Zellen

Diffusion is often an important rate-determining step in chemical reactions or biological processes and plays a role in a wide range of intracellular ...

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Biotechnik

Spatial Separation of Molecular Conformers and Clusters

Gas-phase molecular physics and physical chemistry experiments commonly use supersonic expansions through pulsed valves for the production of cold molecular beams. However, these beams often contain multiple conformers and clusters, even at low rotational temperatures. We present an experimental methodology that allows the spatial separation of these constituent parts of a molecular beam expansion. Using an electric deflector the beam is separated by its mass-to-dipole moment ratio, analogous to a bender or an electric sector mass spectrometer spatially dispersing charged molecules on the basis of their mass-to-charge ratio. This deflector exploits the Stark effect in an inhomogeneous electric field and allows the separation of individual species of polar neutral molecules and clusters. It furthermore allows the selection of the coldest part of a molecular beam, as low-energy rotational quantum states generally experience the largest deflection. Different structural isomers (conformers) of a species can be separated due to the different arrangement of functional groups, which leads to distinct dipole moments. These are exploited by the electrostatic deflector for the production of a conformationally pure sample from a molecular beam. Similarly, specific cluster stoichiometries can be selected, as the mass and dipole moment of a given cluster depends on the degree of solvation around the parent molecule. This allows experiments on specific cluster sizes and structures, enabling the systematic study of solvation of neutral molecules.

We present a technique that allows the spatial separation of different conformers or clusters present in a molecular beam. An electrostatic deflector is used to separate species by their mass-to-dipole moment ratio, leading to the production of gas-phase ensembles of a single conformer or cluster stoichiometry.

Räumliche Trennung von molekularen Konformen und Clustern

Gas-phase molecular physics and physical chemistry experiments commonly use supersonic expansions through pulsed valves for the production of cold ...

Ingenieurwesen

Characterizing Far-infrared Laser Emissions and the Measurement of Their Frequencies

The generation and subsequent measurement of far-infrared radiation has found numerous applications in high-resolution spectroscopy, radio astronomy, and Terahertz imaging. For about 45 years, the generation of coherent, far-infrared radiation has been accomplished using the optically pumped molecular laser. Once far-infrared laser radiation is detected, the frequencies of these laser emissions are measured using a three-laser heterodyne technique. With this technique, the unknown frequency from the optically pumped molecular laser is mixed with the difference frequency between two stabilized, infrared reference frequencies. These reference frequencies are generated by independent carbon dioxide lasers, each stabilized using the fluorescence signal from an external, low pressure reference cell. The resulting beat between the known and unknown laser frequencies is monitored by a metal-insulator-metal point contact diode detector whose output is observed on a spectrum analyzer. The beat frequency between these laser emissions is subsequently measured and combined with the known reference frequencies to extrapolate the unknown far-infrared laser frequency. The resulting one-sigma fractional uncertainty for laser frequencies measured with this technique is &#177; 5 parts in 107. Accurately determining the frequency of far-infrared laser emissions is critical as they are often used as a reference for other measurements, as in the high-resolution spectroscopic investigations of free radicals using laser magnetic resonance. As part of this investigation, difluoromethane, CH2F2, was used as the far-infrared laser medium. In all, eight far-infrared laser frequencies were measured for the first time with frequencies ranging from 0.359 to 1.273 THz. Three of these laser emissions were discovered during this investigation and are reported with their optimal operating pressure, polarization with respect to the CO2 pump laser, and strength.

We describe the generation of far-infrared radiation using an optically pumped molecular laser along with the measurement of their frequencies with heterodyne techniques. The experimental system and techniques are demonstrated using difluoromethane (CH2F2) as the laser medium whose results include three new laser emissions and eight measured laser frequencies.

Charakterisierung von Fern-Infrarot-Laseremissionen und die Messung ihrer Frequenzen

The generation and subsequent measurement of far-infrared radiation has found numerous applications in high-resolution spectroscopy, radio astronomy, and ...

Coulomb Explosion Imaging as a Tool to Distinguish Between Stereoisomers

This article shows how the COLTRIMS (Cold Target Recoil Ion Momentum Spectroscopy) or the "reaction microscope" technique can be used to distinguish between enantiomers (stereoisomers) of simple chiral species on the level of individual molecules. In this approach, a gaseous molecular jet of the sample expands into a vacuum chamber and intersects with femtosecond (fs) laser pulses. The high intensity of the pulses leads to fast multiple ionization, igniting a so-called Coulomb Explosion that produces several cationic (positively charged) fragments. An electrostatic field guides these cations onto time- and position-sensitive detectors. Similar to a time-of-flight mass spectrometer, the arrival time of each ion yields information on its mass. As a surplus, the electrostatic field is adjusted in a way that the emission direction and the kinetic energy after fragmentation lead to variations in the time-of-flight and in the impact position on the detector.
Each ion impact creates an electronic signal in the detector; this signal is treated by high-frequency electronics and recorded event by event by a computer. The registered data correspond to the impact times and positions. With these data, the energy and the emission direction of each fragment can be calculated. These values are related to structural properties of the molecule under investigation, i.e. to the bond lengths and relative positions of the atoms, allowing to determine molecule by molecule the handedness of simple chiral species and other isomeric features.

For small chiral species, Coulomb Explosion Imaging provides a new approach to determine the handedness of individual molecules.

Coulomb Explosion Imaging als Instrument zur Unterscheidung zwischen Stereoisomere

This article shows how the COLTRIMS (Cold Target Recoil Ion Momentum Spectroscopy) or the "reaction microscope" technique can be used to distinguish ...

Chemie

Cooling an Optically Trapped Ultracold Fermi Gas by Periodical Driving

We present a cooling method for a cold Fermi gas by parametrically driving atomic motions in a crossed-beam optical dipole trap (ODT). Our method employs the anharmonicity of the ODT, in which the hotter atoms at the edge of the trap feel the anharmonic components of the trapping potential, while the colder atoms in the center of the trap feel the harmonic one. By modulating the trap depth with frequencies that are resonant with the anharmonic components, we selectively excite the hotter atoms out of the trap while keeping the colder atoms in the trap, generating parametric cooling. This experimental protocol starts with a magneto-optical trap (MOT) that is loaded by a Zeeman slower. The precooled atoms in the MOT are then transferred to an ODT, and a bias magnetic field is applied to create an interacting Fermi gas. We then lower the trapping potential to prepare a cold Fermi gas near the degenerate temperature. After that, we sweep the magnetic field to the noninteracting regime of the Fermi gas, in which the parametric cooling can be manifested by modulating the intensity of the optical trapping beams. We find that the parametric cooling effect strongly depends on the modulation frequencies and amplitudes. With the optimized frequency and amplitude, we measure the dependence of the cloud energy on the modulation time. We observe that the cloud energy is changed in an anisotropic way, where the energy of the axial direction is significantly reduced by parametric driving. The cooling effect is limited to the axial direction because the dominant anharmonicity of the crossed-beam ODT is along the axial direction. Finally, we propose to extend this protocol for the trapping potentials of large anharmonicity in all directions, which provides a promising scheme for cooling quantum gases using external driving.

We present a parametric driving method to cool an ultracold Fermi gas in a crossed-beam optical dipole trap. This method selectively removes high-energy atoms from the trap by periodically modulating the trap depth with frequencies that are resonant with the anharmonic components of the trapping potential.

Kühlen eines Optisch Trapped Ultrakalte Fermi Gas von Zeitfahr

We present a cooling method for a cold Fermi gas by parametrically driving atomic motions in a crossed-beam optical dipole trap (ODT). Our method employs ...

Novel Techniques for Observing Structural Dynamics of Photoresponsive Liquid Crystals

We discuss in this article the experimental measurements of the molecules in liquid crystal (LC) phase using the time-resolved infrared (IR) vibrational spectroscopy and time-resolved electron diffraction. Liquid crystal phase is an important state of matter that exists between the solid and liquid phases and it is common in natural systems as well as in organic electronics. Liquid crystals are orientationally ordered but loosely packed, and therefore, the internal conformations and alignments of the molecular components of LCs can be modified by external stimuli. Although advanced time-resolved diffraction techniques have revealed picosecond-scale molecular dynamics of single crystals and polycrystals, direct observations of packing structures and ultrafast dynamics of soft materials have been hampered by blurry diffraction patterns. Here, we report time-resolved IR vibrational spectroscopy and electron diffractometry to acquire ultrafast snapshots of a columnar LC material bearing a photoactive core moiety. Differential-detection analyses of the combination of time-resolved IR vibrational spectroscopy and electron diffraction are powerful tools for characterizing structures and photoinduced dynamics of soft materials.

Here, we present the protocols of differential-detection analyses of time-resolved infrared vibrational spectroscopy and electron diffraction which enable observations of the deformations of local structures around photoexcited molecules in a columnar liquid crystal, giving an atomic perspective on the relationship between the structure and the dynamics of this photoactive material.

Neuartige Techniken zur Beobachtung von Strukturdynamik von Photoresponsive Flüssigkristallen

We discuss in this article the experimental measurements of the molecules in liquid crystal (LC) phase using the time-resolved infrared (IR) vibrational ...

Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization

We present a pump-probe method for preparing vibrational coherences in polyatomic radical cations and probing their ultrafast dynamics. By shifting the wavelength of the strong-field ionizing pump pulse from the commonly used 800 nm into the near-infrared (1200-1600 nm), the contribution of adiabatic electron tunneling to the ionization process increases relative to multiphoton absorption. Adiabatic ionization results in predominant population of the ground electronic state of the ion upon electron removal, which effectively prepares a coherent vibrational state (&#34;wave packet&#34;) amenable to subsequent excitation. In our experiments, the coherent vibrational dynamics are probed with a weak-field 800 nm pulse and the time-dependent yields of dissociation products measured in a time-of-flight mass spectrometer. We present the measurements on the molecule dimethyl methylphosphonate (DMMP) to illustrate how using 1500 nm pulses for excitation enhances the amplitude of coherent oscillations in ion yields by a factor of 10 as compared to 800 nm pulses. This protocol may be implemented in existing pump-probe setups through the incorporation of an optical parametric amplifier (OPA) for wavelength conversion.

We present a protocol for probing ultrafast vibrational coherences in polyatomic radical cations that result in molecular dissociation.

Messung der ultraschnellen Schwingungs Zusammenhänge in polyatomaren radikale kationen mit Strong-Feld adiabatische Ionisation

We present a pump-probe method for preparing vibrational coherences in polyatomic radical cations and probing their ultrafast dynamics. By shifting the ...

Construction and Operation of a Light-driven Gold Nanorod Rotary Motor System

The possibility to generate and measure rotation and torque at the nanoscale is of fundamental interest to the study and application of biological and artificial nanomotors and may provide new routes towards single cell analysis, studies of non-equilibrium thermodynamics, and mechanical actuation of nanoscale systems. A facile way to drive rotation is to use focused circularly polarized laser light in optical tweezers. Using this approach, metallic nanoparticles can be operated as highly efficient scattering-driven rotary motors spinning at unprecedented rotation frequencies in water.
In this protocol, we outline the construction and operation of circularly-polarized optical tweezers for nanoparticle rotation and describe the instrumentation needed for recording the Brownian dynamics and Rayleigh scattering of the trapped particle. The rotational motion and the scattering spectra provides independent information on the properties of the nanoparticle and its immediate environment. The experimental platform has proven useful as a nanoscopic gauge of viscosity and local temperature, for tracking morphological changes of nanorods and molecular coatings, and as a transducer and probe of photothermal and thermodynamic processes.

Plasmonic gold nanorods can be trapped in liquids and rotated at kHz frequencies using circularly-polarized optical tweezers. Introducing tools for Brownian dynamics analysis and light scatteringspectroscopy leads to a powerful system for research and application in numerous fields of science.

Bau und Betrieb eines lichtgetriebenen Gold Nanorod Rotary Motor Systems

The possibility to generate and measure rotation and torque at the nanoscale is of fundamental interest to the study and application of biological and ...

Light-driven Molecular Motors on Surfaces for Single Molecular Imaging

The design and synthesis of a synthetic system that aims for the direct visualization of a synthetic rotary motor at the single molecule level on surfaces are demonstrated. This work requires careful design, considerable synthetic effort, and proper analysis. The rotary motion of the molecular motor in solution is shown by 1H NMR and UV-vis absorption spectroscopy techniques. In addition, the method to graft the motor onto an amine-coated quartz is described. This method helps to gain more insight into molecular machines.

The manuscript describes how to synthesize and graft a molecular motor on surfaces for single molecular imaging.

Lichtgetriebenen molekularen Motoren auf Oberflächen für einzelne molekulare Bildgebung

The design and synthesis of a synthetic system that aims for the direct visualization of a synthetic rotary motor at the single molecule level on surfaces ...

Infrared Degenerate Four-wave Mixing with Upconversion Detection for Quantitative Gas Sensing

We present a protocol for performing gas spectroscopy using infrared degenerated four-wave mixing (IR-DFWM), for the quantitative detection of gas species in the ppm-to-single-percent range. The main purpose of the method is the spatially resolved detection of low-concentration species, which have no transitions in the visible or near-IR spectral range that could be used for detection. IR-DFWM is a nonintrusive method, which is a great advantage in combustion research, as inserting a probe into a flame can change it drastically. The IR-DFWM is combined with upconversion detection. This detection scheme uses sum-frequency generation to move the IR-DFWM signal from the mid-IR to the near-IR region, to take advantage of the superior noise characteristics of silicon-based detectors. This process also rejects most of the thermal background radiation. The focus of the protocol presented here is on the proper alignment of the IR-DFWM optics and on how to align an intracavity upconversion detection system.

Here, we present a protocol to perform sensitive, spatially resolved gas spectroscopy in the mid-infrared region, using degenerate four-wave mixing combined with upconversion detection.

Infrarot-entartete vier-Welle mischen mit Großbildschirmen Erkennung für Quantitative Gassensorik

We present a protocol for performing gas spectroscopy using infrared degenerated four-wave mixing (IR-DFWM), for the quantitative detection of gas species ...