この作品は、米国陸軍研究局を通じて契約 W911NF-18-1-0051 によって支えられました。

<ol>
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このプロトコルでは、電子基底状態におけるイオンの選択的な調製をラジカル陽イオン多原子の超高速振動ダイナミクスを解決することが出来ます。中に標準的な強い電場電離法 800 nm は最初の行 diatomics10、11,12,13と CO の地上電子状態ラジカル陽イオンの振動コヒーレンスを準備することが2</...

1960 年代にレーザーの発明、分子の化学結合を選択的に破壊の目的以来の化学者および物理学者の長年の夢。両方を調整する能力レーザー周波数と強度は、関連付けられている振動数1,2,3,4 選択的エネルギー吸光度を通してターゲット結合の直接胸の谷間を有効にすると信じられていた.しかし、初期の実験は、分子内振動再配布分子全体で吸収されたエネルギーの多くの場合が最も弱い結合4、5の非選択的胸の谷間の結果を発見します。フェムト秒のパルス レーザー、後半ポンプ-プローブ法6コヒーレント振動状態、または「波パケット」の直接操作の 1980 年有効に成功した裂その他制御まではありませんでした。目標6,7,8。前記「ポンプ」パルス励起状態またはその後遅れ「プローブ」パルスによって励起イオンを準備、ポンプ ・ プローブ測定分子9、超高速のプロセスを研究するための最も広く使用されている技術の 1 つのまま 10、11,12,13,14,15,16,17,18、 19,20。
超高速解離イオン ポンプによって標的分子の非選択的断片化に起因して質量分析検出に結合されたポンプ-プローブ励起を用いた多原子のラジカル イオンのダイナミクスを研究する重要な制限チタンサファイアレーザー波長 800 nm21,22,23パルスします。この過剰な断片化に起因する非断熱の多光子イオン化と近赤外光に励起波長をシフトすることによって軽減することができます (例えば.、1200-1500 nm)22,23,24、 25。これらのより長い波長では、イオン化における多光子励起に対する断熱電子トンネリングの増加の貢献は22,23を処理します。断熱トンネリング分子と形態主に「冷たい」基底状態分子イオン19,22,23に少し余分なエネルギーを与えます。らは、近赤外励起の使用がコヒーレント振動励起または「波パケット」、と比較すると 800 nm 励起19、ラジカル陽イオン多原子準備大幅向上を示しています。 20。この作品は、化学兵器エージェント持ち帰りジメチル methylphosphonate (DMMP) 1500 nm と 800 を使用してのポンプ ・ プローブ測定と多光子・ トンネルへの取り組みによって支配される強い電界イオン化の違いを示す、nmポンプ波長です。
ポンプ ・ プローブ実験では、超短パルス レーザーのペアは遅れられたと飛行時間質量分析計に焦点を当てた私たちセットアップ図1 に示すように。これらの実験が必要チタンサファイアレーザー再生増幅器生産 > 2 mJ、800 nm、30 fs パルス。アンプ出力は、エネルギーのほとんどが発電用の 1200-1600 nm、100-300 μ J、20-30 fs パルス光パラメトリック増幅器 (OPA) をポンプに使用され、90: 10 (%r: %t) ビーム ・ スプリッターで分割されます。IR ポンプ光の直径は 22 mm と 5.5 mm とアイリスを使用してコアにダウン平行 800 nm プローブ ビームの直径に拡張されます。これらの collimations は大幅に小さいビーム腰に (9 μ m) プローブ ビーム (30 μ m) より確保電離ポンプ パルスの間に形成されるすべてのイオンが遅れプローブのパルスによって興奮しているポンプ集光で結果します。この構成を使用するは、我々 の実験の目標は集光ビームの端に近い低強度でも形成されることがあります親分子イオンのダイナミクスをプローブするので。我々 は詳細高励起イオンのダイナミクスが重要場合、プローブ径を行うことをポンプよりも注意してください。
ポンプ ・ プローブのパルス伝播線上とワイリー マクラーレン飛行時間質量分析計 (TOF-MS)26 (図 2) の抽出領域に焦点を当てています。バイアルは、分子サンプルを入口に接続し、真空に開いた。このセットアップする必要があります調査中分子以外の蒸気圧力;低蒸気圧で分子、バイアルを温められます。商工会議所への試料気体の流れは、2 つの変数のリーク バルブによって制御されます。サンプル抽出地域27ターゲット分子のローカル高濃度を提供するためにレーザーの焦点 (図 2) から 1/16"ステンレス チューブ約 1 cm を通ってチャンバを入力します。抽出プレートが指向 0.5 mm スリット レーザーの伝搬とイオンのパスに直交します。ポンプ光のレイリーの範囲は約 2 mm、このスリットは強度が高い抽出プレート28を通過する中央焦点ボリュームから生成したイオンのみを許可するフィルターとして機能します。イオンは、Z ギャップ マイクロ チャネル プレート (MCP) 検出器29、彼らが検出され、典型的な商業チタンサファイアレーザの 1 khz の繰り返しで 1 GHz デジタル ・ オシロ スコープで記録に到達する 1 m フィールド無料ドリフト チューブを入力します。

<table><tbody><tr><td>&lt;strong&gt;Mass spectrometer components&lt;/strong&gt;</td><td></td><td></td><td></td></tr><tr><td>TOF lens stack and flight tube assembly</td><td>Jordan TOF Products, Inc.</td><td>C-677</td><td></td></tr><tr><td>18 mm Z-gap detector assembly</td><td>Jordan TOF Products, Inc.</td><td>C-701Z</td><td></td></tr><tr><td>TOF high voltage power supply</td><td>Jordan TOF Products, Inc.</td><td>D-603</td><td></td></tr><tr><td>&lt;strong&gt;Vacuum system components&lt;/strong&gt;</td><td></td><td></td><td></td></tr><tr><td>Rotary vane backing pump</td><td>Edwards Vacuum LLC</td><td>RV12</td><td></td></tr><tr><td>Turbomolecular pumps (2)</td><td>Edwards Vacuum LLC</td><td>EXT255H</td><td></td></tr><tr><td>Turbomolecular pump controllers (2)</td><td>Edwards Vacuum LLC</td><td>EXC300</td><td></td></tr><tr><td>Pressure gauge</td><td>Edwards Vacuum LLC</td><td>AIGX-S-DN40CF</td><td></td></tr><tr><td>Chiller for water cooling</td><td>Neslab</td><td>CFT-25</td><td></td></tr><tr><td>&lt;strong&gt;Femtosecond laser system&lt;/strong&gt;</td><td></td><td></td><td></td></tr><tr><td>Ti:Sapphire regenerative amplifier</td><td>Coherent, Inc.</td><td>Astrella</td><td>oscillator and amplifier in a single integrated system</td></tr><tr><td>Optical Parametric Amplifer (OPA)</td><td>Light Conversion</td><td>TOPAS Prime</td><td></td></tr><tr><td>&lt;strong&gt;Motion control&lt;/strong&gt;</td><td></td><td></td><td></td></tr><tr><td>Motorized linear translation stage 1&quot; travel</td><td>Thorlabs</td><td>Z825B</td><td></td></tr><tr><td>controller for linear translation stage</td><td>Thorlabs</td><td>KDC 101</td><td></td></tr><tr><td>USB controller hub and power supply</td><td>Thorlabs</td><td>KCH 601</td><td></td></tr><tr><td>Manual linear translation stage 1&quot; travel</td><td>Thorlabs</td><td>PT1</td><td></td></tr><tr><td>&lt;strong&gt;Detectors&lt;/strong&gt;</td><td></td><td></td><td></td></tr><tr><td>Pyroelectric laser energy meter</td><td>Coherent, Inc.</td><td>1168337</td><td></td></tr><tr><td>Thermal laser power meter</td><td>Coherent, Inc.</td><td>5356E16R</td><td></td></tr><tr><td>Si-biased detector 200-1100 nm</td><td>Thorlabs</td><td>DET10A</td><td></td></tr><tr><td>Compact USB CMOS Camera</td><td>Thorlabs</td><td>DCC1545M</td><td></td></tr><tr><td>USB spectrometer</td><td>Ocean Optics</td><td>HR4000</td><td></td></tr><tr><td>1 GHz digital oscilloscope&amp;nbsp;</td><td>LeCroy</td><td>WaveRunner 610Zi</td><td></td></tr><tr><td>&lt;strong&gt;Optics&lt;/strong&gt;</td><td></td><td></td><td></td></tr><tr><td>Type 1 BBO crystal</td><td>Crylight Photonics</td><td>BBO007</td><td>aperture and thickness may be customized</td></tr><tr><td>Achromatic half wave plate, 1100-2000 nm</td><td>Thorlabs</td><td>AHWP05M-1600</td><td></td></tr><tr><td>Wollaston prism polarizer</td><td>Thorlabs</td><td>WPM10</td><td></td></tr><tr><td>Hollow retro-reflector</td><td>PLX, Inc.</td><td>OW-20-1C</td><td></td></tr><tr><td>Variable neutral density filter</td><td>Thorlabs</td><td>NDC-100C-2</td><td></td></tr><tr><td>Longpass dichroic mirror 2&quot; diameter</td><td>Thorlabs</td><td>DMLP950L</td><td></td></tr><tr><td>&lt;strong&gt;Software&lt;/strong&gt;</td><td></td><td></td><td></td></tr><tr><td>Digital Camera image software</td><td>Thorlabs</td><td>ThorCam</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</td><td></td></tr><tr><td>Data processing software</td><td>Mathworks</td><td>MATLAB</td><td></td></tr></tbody></table>

measurement of ultrafast vibrational coherences in polyatomic radical cations with strong-field adiabatic ionization

多原子ラジカル陽イオンの振動コヒーレンスを準備し、その超高速ダイナミクスを探るのためのポンプ-プローブ法を提案します。一般的に使用される 800 から強い電界電離ポンプ パルスの波長をシフトすることによって nm 赤外 (1200-1600 nm) に、多光子吸収に対して断熱電子イオン化プロセスへの貢献の増加します。断熱イオン化電子除去を効果的にコヒーレント振動状態 (「波パケット」) 以降の励起に従うを準備する時にイオンの電子基底状態の優勢な人口で起因します。実験では、弱いフィールド 800 nm パルスでコヒーレントな振動ダイナミクスがプローブされ、解離製品の時間依存の利回りは飛行時間質量分析計で測定します。800 nm パルスと比較して 10 の要因によってイオン収率の分子ジメチル methylphosphonate 励起用 1500 nm パルスを使用するコヒーレント振動の振幅と強化方法を説明するために (DMMP) の測定を提案します。波長変換のための光パラメトリック増幅 (OPA) を組み込むことによって既存のポンプ ・ プローブのセットアップでは、このプロトコルを実装できます。

分子 DMMP21の結果が掲載されています。図 3は、それぞれ12 W cm-2、0 1500 nm ポンプと 8 x 1013をされている 800 nm プローブ パルスのピーク強度と遅延時間と 8 x 10 で撮影 DMMP 質量スペクトルを示しています。参考までに、またポンプ パルスのみで撮影した質量スペクトルが表示されます。スペクトルは、平均...

Watch this Scientific Journal Video about Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization at JoVE.com

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

分子解離は、多原子のラジカル陽イオンに超高速の振動コヒーレンスをプロービングのためのプロトコルを提案します。

強いフィールド断熱イオンとラジカル陽イオン多原子の超高速振動コヒーレンスの測定

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

measurement-ultrafast-vibrational-coherences-polyatomic-radical

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Chemistry

Chemical Bonding: Basic Concepts

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6.8K ビュー.  Virginia Commonwealth University. 分子解離は、多原子のラジカル陽イオンに超高速の振動コヒーレンスをプロービングのためのプロトコルを提案します。

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

Molecular Beam Mass Spectrometry With Tunable Vacuum Ultraviolet (VUV) Synchrotron Radiation

Tunable soft ionization coupled to mass spectroscopy is a powerful method to investigate isolated molecules, complexes and clusters and their spectroscopy and dynamics1-4. Fundamental studies of photoionization processes of biomolecules provide information about the electronic structure of these systems. Furthermore determinations of ionization energies and other properties of biomolecules in the gas phase are not trivial, and these experiments provide a platform to generate these data. We have developed a thermal vaporization technique coupled with supersonic molecular beams that provides a gentle way to transport these species into the gas phase. Judicious combination of source gas and temperature allows for formation of dimers and higher clusters of the DNA bases. The focus of this particular work is on the effects of non-covalent interactions, i.e., hydrogen bonding, stacking, and electrostatic interactions, on the ionization energies and proton transfer of individual biomolecules, their complexes and upon micro-hydration by water1, 5-9.
We have performed experimental and theoretical characterization of the photoionization dynamics of gas-phase uracil and 1,3-dimethyluracil dimers using molecular beams coupled with synchrotron radiation at the Chemical Dynamics Beamline10 located at the Advanced Light Source and the experimental details are visualized here. This allowed us to observe the proton transfer in 1,3-dimethyluracil dimers, a system with pi stacking geometry and with no hydrogen bonds1. Molecular beams provide a very convenient and efficient way to isolate the sample of interest from environmental perturbations which in return allows accurate comparison with electronic structure calculations11, 12. By tuning the photon energy from the synchrotron, a photoionization efficiency (PIE) curve can be plotted which informs us about the cationic electronic states. These values can then be compared to theoretical models and calculations and in turn, explain in detail the electronic structure and dynamics of the investigated species 1, 3.

Molecular Beam Mass Spectrometry With Tunable Vacuum Ultraviolet VUV Synchrotron Radiation

A molecular beam coupled to tunable vacuum ultraviolet photoionization mass spectrometer at a synchrotron provides a convenient tool to explore the electronic structure of isolated gas phase molecules and clusters. Proton transfer mechanisms in DNA base dimers were elucidated with this technique.

波長可変真空紫外（VUV）放射光を用いた分子線質量分析

Tunable soft ionization coupled to mass spectroscopy is a powerful method to investigate isolated molecules, complexes and clusters and their spectroscopy ...

工学

Measurement and Analysis of Atomic Hydrogen and Diatomic Molecular AlO, C2, CN, and TiO Spectra Following Laser-induced Optical Breakdown

In this work, we present time-resolved measurements of atomic and diatomic spectra following laser-induced optical breakdown. A typical LIBS arrangement is used. Here we operate a Nd:YAG laser at a frequency of 10 Hz at the fundamental wavelength of 1,064 nm. The 14 nsec pulses with anenergy of 190 mJ/pulse are focused to a 50 &#181;m spot size to generate a plasma from optical breakdown or laser ablation in air. The microplasma is imaged onto the entrance slit of a 0.6 m spectrometer, and spectra are recorded using an 1,800 grooves/mm grating an intensified linear diode array and optical multichannel analyzer (OMA) or an ICCD. Of interest are Stark-broadened atomic lines of the hydrogen Balmer series to infer electron density. We also elaborate on temperature measurements from diatomic emission spectra of aluminum monoxide (AlO), carbon (C2), cyanogen (CN), and titanium monoxide (TiO).
The experimental procedures include wavelength and sensitivity calibrations. Analysis of the recorded molecular spectra is accomplished by the fitting of data with tabulated line strengths. Furthermore, Monte-Carlo type simulations are performed to estimate the error margins. Time-resolved measurements are essential for the transient plasma commonly encountered in LIBS.

Measurement and Analysis of Atomic Hydrogen and Diatomic Molecular AlO, C2, CN, and TiO Spectra Following Laser-induced Optical Breakdown

Time-resolved atomic and diatomic molecular species are measured using LIBS. The spectra are collected at various time delays following the generation of optical breakdown plasma with Nd:YAG laser radiation&#160;and are analyzed to infer electron density and temperature.

測定と原子状水素と二原子分子のAlO、Cの分析<sub&gt; 2</sub&gt;、CN、およびTiOスペクトラ[次のレーザー誘起光学破壊

In this work, we present time-resolved measurements of atomic and diatomic spectra following laser-induced optical breakdown. A typical LIBS arrangement ...

Proton Transfer and Protein Conformation Dynamics in Photosensitive Proteins by Time-resolved Step-scan Fourier-transform Infrared Spectroscopy

Monitoring the dynamics of protonation and protein backbone conformation changes during the function of a protein is an essential step towards understanding its mechanism. Protonation and conformational changes affect the vibration pattern of amino acid side chains and of the peptide bond, respectively, both of which can be probed by infrared (IR) difference spectroscopy. For proteins whose function can be repetitively and reproducibly triggered by light, it is possible to obtain infrared difference spectra with (sub)microsecond resolution over a broad spectral range using the step-scan Fourier transform infrared technique. With ~102-103 repetitions of the photoreaction, the minimum number to complete a scan at reasonable spectral resolution and bandwidth, the noise level in the absorption difference spectra can be as low as ~10-4, sufficient to follow the kinetics of protonation changes from a single amino acid. Lower noise levels can be accomplished by more data averaging and/or mathematical processing. The amount of protein required for optimal results is between 5-100 &#181;g, depending on the sampling technique used. Regarding additional requirements, the protein needs to be first concentrated in a low ionic strength buffer and then dried to form a film. The protein film is hydrated prior to the experiment, either with little droplets of water or under controlled atmospheric humidity. The attained hydration level (g of water / g of protein) is gauged from an IR absorption spectrum. To showcase the technique, we studied the photocycle of the light-driven proton-pump bacteriorhodopsin in its native purple membrane environment, and of the light-gated ion channel channelrhodopsin-2 solubilized in detergent.

Key steps of protein function, in particular backbone conformational changes and proton transfer reactions, often take place in the microsecond to millisecond time scale. These dynamical processes can be studied by time-resolved step-scan Fourier-transform infrared spectroscopy, in particular for proteins whose function is triggered by light.

感光性タンパク質中のプロトン移動とプロテイン立体配座ダイナミクスの時間分解ステップスキャンフーリエ変換赤外分光法により

Monitoring the dynamics of protonation and protein backbone conformation changes during the function of a protein is an essential step towards ...

Direct Imaging of Laser-driven Ultrafast Molecular Rotation

We present a method for visualizing laser-induced, ultrafast molecular rotational wave packet dynamics. We have developed a new 2-dimensional Coulomb explosion imaging setup in which a hitherto-impractical camera angle is realized. In our imaging technique, diatomic molecules are irradiated with a circularly polarized strong laser pulse. The ejected atomic ions are accelerated perpendicularly to the laser propagation. The ions lying in the laser polarization plane are selected through the use of a mechanical slit and imaged with a high-throughput, 2-dimensional detector installed parallel to the polarization plane. Because a circularly polarized (isotropic) Coulomb exploding pulse is used, the observed angular distribution of the ejected ions directly corresponds to the squared rotational wave function at the time of the pulse irradiation. To create a real-time movie of molecular rotation, the present imaging technique is combined with a femtosecond pump-probe optical setup in which the pump pulses create unidirectionally rotating molecular ensembles. Due to the high image throughput of our detection system, the pump-probe experimental condition can be easily optimized by monitoring a real-time snapshot. As a result, the quality of the observed movie is sufficiently high for visualizing the detailed wave nature of motion. We also note that the present technique can be implemented in existing standard ion imaging setups, offering a new camera angle or viewpoint for the molecular systems without the need for extensive modification.

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

レーザー駆動の超高速分子回転のダイレクトイメージング

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

化学

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.

立体異性体を区別するためのツールとしてクーロン爆発イメージング

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

Measurements of Long-range Electronic Correlations During Femtosecond Diffraction Experiments Performed on Nanocrystals of Buckminsterfullerene

The precise details of the interaction of intense X-ray pulses with matter are a topic of intense interest to researchers attempting to interpret the results of femtosecond X-ray free electron laser (XFEL) experiments. An increasing number of experimental observations have shown that although nuclear motion can be negligible, given a short enough incident pulse duration, electronic motion cannot be ignored. The current and widely accepted models assume that although electrons undergo dynamics driven by interaction with the pulse, their motion could largely be considered &#39;random&#39;. This would then allow the supposedly incoherent contribution from the electronic motion to be treated as a continuous background signal and thus ignored. The original aim of our experiment was to precisely measure the change in intensity of individual Bragg peaks, due to X-ray induced electronic damage in a model system, crystalline C60. Contrary to this expectation, we observed that at the highest X-ray intensities, the electron dynamics in C60 were in fact highly correlated, and over sufficiently long distances that the positions of the Bragg reflections are significantly altered. This paper describes in detail the methods and protocols used for these experiments, which were conducted both at the Linac Coherent Light Source (LCLS) and the Australian Synchrotron (AS) as well as the crystallographic approaches used to analyse the data.

We describe an experiment designed to probe the electronic damage induced in nanocrystals of Buckminsterfullerene (C60) by intense, femtosecond pulses of X-rays. The experiment found that, surprisingly, rather than being stochastic, the X-ray induced electron dynamics in C60 are highly correlated, extending over hundreds of unit cells within the crystals1.

バックミンスターフラーレンのナノ結晶のフェムト秒回折実験中長距離電子相関の測定

The precise details of the interaction of intense X-ray pulses with matter are a topic of intense interest to researchers attempting to interpret the ...

An Experimental Protocol for Femtosecond NIR/UV - XUV Pump-Probe Experiments with Free-Electron Lasers

This protocol describes key steps in performing and analyzing femtosecond pump-probe experiments that combine a femtosecond optical laser with a free-electron laser. This includes methods to establish the spatial and temporal overlap between the optical and free-electron laser pulses during the experiment, as well as important aspects of the data analysis, such as corrections for arrival time jitter, which are necessary to obtain high-quality pump-probe data sets with the best possible temporal resolution. These methods are demonstrated for an exemplary experiment performed at the FLASH (Free-electron LASer Hamburg) free-electron laser in order to study ultrafast photochemistry in gas-phase molecules by means of velocity map ion imaging. However, most of the strategies are also applicable to similar pump-probe experiments using other targets or other experimental techniques.

This protocol describes the key steps for performing and analyzing pump-probe experiments combining a femtosecond optical laser with a free-electron laser in order to study ultrafast photochemical reactions in gas-phase molecules.

実験的プロトコル フェムト秒近赤外/紫外-自由電子レーザーによる XUV ポンプ ・ プローブ実験

This protocol describes key steps in performing and analyzing femtosecond pump-probe experiments that combine a femtosecond optical laser with a ...

Photoelectron Imaging of Anions Illustrated by 310 Nm Detachment of F&#8722;

Anion photoelectron imaging is a very efficient method for the study of energy states of bound negative ions, neutral species and interactions of unbound electrons with neutral molecules/atoms. State-of-the-art in vacuo anion generation techniques allow application to a broad range of atomic, molecular, and cluster anion systems. These are separated and selected using time-of-flight mass spectrometry. Electrons are removed by linearly polarized photons (photo detachment) using table-top laser sources which provide ready access to excitation energies from the infra-red to the near ultraviolet. Detecting the photoelectrons with a velocity mapped imaging lens and position sensitive detector means that, in principle, every photoelectron reaches the detector and the detection efficiency is uniform for all kinetic energies. Photoelectron spectra extracted from the images via mathematical reconstruction using an inverse Abel transformation reveal details of the anion internal energy state distribution and the resultant neutral energy states. At low electron kinetic energy, typical resolution is sufficient to reveal energy level differences on the order of a few millielectron-volts, i.e., different vibrational levels for molecular species or spin-orbit splitting in atoms. Photoelectron angular distributions extracted from the inverse Abel transformation represent the signatures of the bound electron orbital, allowing more detailed probing of electronic structure. The spectra and angular distributions also encode details of the interactions between the outgoing electron and the residual neutral species subsequent to excitation. The technique is illustrated by the application to an atomic anion (F&#8722;), but it can also be applied to the measurement of molecular anion spectroscopy, the study of low lying anion resonances (as an alternative to scattering experiments) and femtosecond (fs) time resolved studies of the dynamic evolution of anions.

Here, we present a protocol for photoelectron imaging of anionic species. Anions generated in vacuo and separated by mass spectrometry are probed using velocity mapped photoelectron imaging, providing details of anion and neutral energy levels, anion and neutral structure and the nature of the anion electronic state.

F− 310 Nm 剥離によって示されている陰イオンの光電子イメージング

Anion photoelectron imaging is a very efficient method for the study of energy states of bound negative ions, neutral species and interactions of unbound ...

Ultrafast Time-resolved Near-IR Stimulated Raman Measurements of Functional &#960;-conjugate Systems

Femtosecond time-resolved stimulated Raman spectroscopy is a promising method of observing the structural dynamics of short-lived transients with near infrared (near-IR) transitions, because it can overcome the low sensitivity of spontaneous Raman spectrometers in the near-IR region. Here, we describe technical details of a femtosecond time-resolved near-IR multiplex stimulated Raman spectrometer that we have recently developed. A description of signal generation and optimization, measurement, data acquisition, and calibration and correction of recorded data is provided as well. We present an application of our spectrometer to analyze the excited-state dynamics of &#946;-carotene in toluene solution. A C=C stretch band of &#946;-carotene in the second lowest excited singlet (S2) state and the lowest excited singlet (S1) state is clearly observed in the recorded time-resolved stimulated Raman spectra. The femtosecond time-resolved near-IR stimulated Raman spectrometer is applicable to the structural dynamics of &#960;-conjugate systems from simple molecules to complex materials.

Details of signal generation and optimization, measurement, data acquisition, and data handling for a femtosecond time-resolved near-IR stimulated Raman spectrometer are described. A near infrared stimulated Raman study on the excited-state dynamics of &#946;-carotene in toluene is shown as a representative application.

超高速時間分解型近IR刺激型機能π共役システムのラマン測定

Femtosecond time-resolved stimulated Raman spectroscopy is a promising method of observing the structural dynamics of short-lived transients with near ...

Vibrational Spectra of a N719-Chromophore/Titania Interface from Empirical-Potential Molecular-Dynamics Simulation, Solvated by a Room Temperature Ionic Liquid

The accurate molecular simulation prediction of vibrational spectra, and other structural, energetic and spectral characteristics, of photo-active metal-oxide surfaces in contact with light-absorbing dyes is an ongoing thorny and elusive challenge in physical chemistry. With this in mind, a molecular-dynamics (MD) simulation were performed by using optimized empirical potentials for a well-representative and prototypical dye-sensitized solar cell (DSC) solvated by a widely-studied room temperature ionic liquid (RTIL), in the guise of a [bmim]+[NTf2]- RTIL solvating an N719-sensitizing dye adsorbed onto 101 anatase-titania. In doing so, important insights were gleaned into how using a RTIL as the electrolytic hole acceptor modulates the dynamical and vibrational properties of a N719 dye, estimating the spectra for the DSC photo-active interface via Fourier transformation of mass-weighted velocity autocorrelation functions from MD. The acquired vibrational spectra were compared with the experiment spectra and those sampled from ab initio molecular dynamics (AIMD); in particular, various empirical-potential spectra generated from MD provide insight into how partial-charge charge parameterization of the ionic liquid affects vibrational spectra prediction. In any event, careful fitting of empirical force-field models has been shown to be an effective tool in handling DSC vibrational properties, when validated by AIMD and an experiment.

A dye-sensitized solar cell was solvated by RTILs; using optimized empirical potentials, a molecular dynamics simulation was applied to compute vibrational properties. The obtained vibrational spectra were compared with experiment and ab initio molecular dynamics; various empirical potential spectra show how partial-charge charge parameterization of the ionic liquid affects vibrational spectra prediction.

強いフィールド断熱イオンとラジカル陽イオン多原子の超高速振動コヒーレンスの測定

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波長可変真空紫外（VUV）放射光を用いた分子線質量分析

測定と原子状水素と二原子分子のAlO、Cの分析

感光性タンパク質中のプロトン移動とプロテイン立体配座ダイナミクスの時間分解ステップスキャンフーリエ変換赤外分光法により

レーザー駆動の超高速分子回転のダイレクトイメージング

立体異性体を区別するためのツールとしてクーロン爆発イメージング

バックミンスターフラーレンのナノ結晶のフェムト秒回折実験中長距離電子相関の測定

実験的プロトコルフェムト秒近赤外/紫外-自由電子レーザーによる XUV ポンプ・プローブ実験

F⁻ 310 Nm 剥離によって示されている陰イオンの光電子イメージング

超高速時間分解型近IR刺激型機能π共役システムのラマン測定

経験電位分子動力学シミュレーションによるN719-クロモフォア/チタニア界面の振動スペクトル、室温イオン液体による溶媒和

強いフィールド断熱イオンとラジカル陽イオン多原子の超高速振動コヒーレンスの測定

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波長可変真空紫外（VUV）放射光を用いた分子線質量分析

測定と原子状水素と二原子分子のAlO、Cの分析

感光性タンパク質中のプロトン移動とプロテイン立体配座ダイナミクスの時間分解ステップスキャンフーリエ変換赤外分光法により

レーザー駆動の超高速分子回転のダイレクトイメージング

立体異性体を区別するためのツールとしてクーロン爆発イメージング

バックミンスターフラーレンのナノ結晶のフェムト秒回折実験中長距離電子相関の測定

実験的プロトコル フェムト秒近赤外/紫外-自由電子レーザーによる XUV ポンプ ・ プローブ実験

F− 310 Nm 剥離によって示されている陰イオンの光電子イメージング

超高速時間分解型近IR刺激型機能π共役システムのラマン測定

経験電位分子動力学シミュレーションによるN719-クロモフォア/チタニア界面の振動スペクトル、室温イオン液体による溶媒和

実験的プロトコルフェムト秒近赤外/紫外-自由電子レーザーによる XUV ポンプ・プローブ実験

F⁻ 310 Nm 剥離によって示されている陰イオンの光電子イメージング