Three-dimensional (3D) moment imaging with a USB3 oscilloscope.

We report a new implementation of a recently developed 3D momentum imaging technique [Lee et al. J. Chem. Phys. 141, 221101 (2014)]. The previously employed high-speed digitizer in the setup is replaced by a portable USB3 oscilloscope. A new triggering scheme was developed to suppress trigger jitters and to synchronize the signals from a camera and the oscilloscope. The performance of the setup was characterized in the study of laser desorption/ionization of 2,5-dihydroxybenzoic acid on a velocity map imaging apparatus. A ∼60 picosecond time resolution in measuring time-of-flight is achieved with a count rate of ∼1 kHz, which is comparable to the system using high-speed digitizers. The new setup affords great portability and wider accessibility to the high-performing 3D momentum imaging technique.

Slicing Newton spheres with a two-camera 3D imaging system.

We demonstrate a simple approach to achieve three-dimensional ion momentum imaging. The method employs two complementary metal-oxide-semiconductor cameras in addition to a standard microchannel plates/phosphor screen imaging detector. The two cameras are timed to measure the decay of luminescence excited by ion hits to extract the time of flight. The achieved time resolution is better than 10 ns, which is mainly limited by camera jitters. A better than 5 ns resolution can be achieved when the jitter is suppressed.

Attosecond Imaging of Electronic Wave Packets.

An electronic wave packet has significant spatial evolution besides its temporal evolution, due to the delocalized nature of composing electronic states. The spatial evolution was not previously accessible to experimental investigations at the attosecond timescale. A phase-resolved two-electron-angular-streaking method is developed to image the shape of the hole density of an ultrafast spin-orbit wave packet in the krypton cation. Furthermore, the motion of an even faster wave packet in the xenon cation is captured for the first time: An electronic hole is refilled 1.2 fs after it is produced, and the hole filling is observed on the opposite side where the hole is born.

Carrier-Envelope Phase Controlling of Ion Momentum Distributions in Strong Field Double Ionization of Methyl Iodide.

In strong field ionization of methyl iodide initiated by elliptically polarized few-cycle pulses, a significant correlation was observed between the carrier-envelope phases (CEPs) of the laser and the preferred ejection direction of methyl cation arising from dissociative double ionization. This was attributed to the carrier-envelope phase dependent double ionization yields of methyl iodide. This observation provides a new way for monitoring the absolute CEPs of few-cycle pulses by observing the ion momentum distributions.

Ellipticity controlled dissociative double ionization of ethane by strong fields.

The yields of all dissociation channels of ethane dications produced by strong field double ionization were measured. It was found that the branching ratios can be controlled by varying the ellipticity of laser pulses. The CH3+ formation and H+ formation channels show a clear competition, producing the highest and lowest branching ratios at ellipticity of ∼0.6, respectively. With the help of theoretical calculations, such a control was attributed to the ellipticity dependent yields of different sequential ionization pathways.

Coulomb Explosion Dynamics of Chlorocarbonylsulfenyl Chloride.

The Coulomb explosion dynamics following strong field ionization of chlorocarbonylsulfenyl chloride was studied using multimass coincidence detection and covariance imaging analysis, supported by density functional theory calculations. These results show evidence of multiple dissociation channels from various charge states. Double ionization to low-lying electronic states leads to a dominant C-S cleavage channel, while higher states can alternatively correlate to the loss of Cl+. Triple ionization leads to a double dissociation channel, the observation of which is confirmed via three-body covariance analysis, while further ionization leads primarily to atomic or diatomic fragments whose relative momenta depend strongly on the starting structure of the molecule.

All-Optical Three-Dimensional Electron Momentum Imaging.

We report a new implementation of three-dimensional (3D) momentum imaging for electrons, employing a two-dimensional (2D) imaging detector and a silicon photomultiplier tube (siPMT). To achieve the necessary time resolution for 3D electron imaging, a poly(p-phenylene)-dye-based fast scintillator (Exalite 404) was used in the imaging detector instead of conventional phosphors. The system demonstrated an electron time-of-flight resolution comparable with that of electrical MCP pick-off (tens of picoseconds), while achieving an unprecedented dead time reduction (∼0.48 ns) when detecting two electrons.

Developing a camera-based 3D momentum imaging system capable of 1 Mhits/s.

A camera-based three-dimensional (3D) imaging system with a superb time-of-flight (TOF) resolution and multi-hit capability was recently developed for electron/ion imaging [Lee et al. J. Chem. Phys. 141, 221101 (2014)]. In this work, we report further improvement of the event rate of the system by adopting an event-driven camera, Tpx3Cam, for detecting the 2D positions of electrons, while a high-speed digitizer provides highly accurate (∼30 ps) TOF information for each event at a rate approaching 1 Mhits/sec.

Direct in-situ single-shot measurements of the absolute carrier-envelope phases of ultrashort pulses.

Many important physical processes such as nonlinear optics and coherent control are highly sensitive to the absolute carrier-envelope phase (CEP) of driving ultrashort laser pulses. This makes the measurement of CEP immensely important in relevant fields. Even though relative CEPs can be measured with a few existing technologies, the estimate of the absolute CEP is not straightforward and always requires theoretical inputs. Here, we demonstrate a novel in-situ technique based on angular streaking that can achieve such a goal without complicated calibration procedures. Single-shot measurements of the absolute CEP have been achieved with an estimated precision of 0.19 radians.

Demonstration of multi-hit and multi-mass capability of 3D imaging in a conventional velocity map imaging experiment.

Coincidence and three-dimensional (3D) imaging offer unique capability in photodissociation and scattering experiments, and a variety of methods have been developed. The basic concept behind all these approaches is to register both the position (x, y) at which the particle hits the detector and the arrival time (t). A novel advance to the time and position sensitive detection was introduced recently by Li and co-workers [Rev. Sci. Instrum. 85(12), 123303 (2014)]. This method utilizes a high-speed digitizer and a computer algorithm along with the camera and detector usually employed in a conventional velocity map imaging apparatus. Due to the normal intensity variations of the ion spots, a correlation can be made between ion intensity recorded by the camera and peak intensity in the digitizer. This makes it possible to associate each ion spot's position with its respective arrival time, thereby constructing a 3D distribution. The technique was primarily introduced for ultrafast ion and electron imaging experiments at high repetition rate with single or few events per image frame. We have recently succeeded in adapting this approach at low repetition rate. Modifications were done to the initial setup to enhance the acquisition efficiency to obtain and correlate multiple hits per laser shot rather than single-hit events. The results are demonstrated in two experiments, dimethyl amine dissociative ionization at 205 nm and carbonyl sulfide photodissociation at 217 nm, with up to 27 events correlated in a single frame. Temporal and spatial slicing capabilities were achieved with good resolution, giving the photofragment velocity and angular distribution for multiple masses simultaneously.

Disentangling Strong-Field Multielectron Dynamics with Angular Streaking.

The study into the interaction between a strong laser field and atoms/molecules has led to significant advances in developing spectroscopic tools in the attosecond time-domain and methods for controlling chemical reactions. There has been great interest in understanding the complex electronic and nuclear dynamics of molecules in strong laser fields. However, it is still a formidable challenge to fully model such dynamics. Conventional experimental tools such as photoelectron spectroscopy encounter difficulties in revealing the involved states because the electron spectra are largely dictated by the property of the laser field. Here, with strong field angular streaking technique, we measure the angle-dependent ionization yields that directly reflect the symmetry of the ionizing orbitals of methyl iodide and thus reveal the ionization/dissociation dynamics. Moreover, kinematically complete measurements of momentum vectors of all fragments in dissociative double ionization processes allow access to electron-momentum correlations that reveal correlated multielectron dynamics.

Observation of Nanosecond Hot Carrier Decay in Graphene.

An extremely long decay time of hot carriers in graphene at room temperature was observed for the first time by monitoring the photoinduced thermionic emission using a highly sensitive time-of-flight angle-resolved photoemission spectroscopy method. The emission persisted beyond 1 ns, two orders of magnitude longer than previously reported carrier decay. The long lifetime was attributed to the excitation of image potential states at very low laser fluencies.

A new electron-ion coincidence 3D momentum-imaging method and its application in probing strong field dynamics of 2-phenylethyl-N, N-dimethylamine.

We report the development of a new three-dimensional (3D) momentum-imaging setup based on conventional velocity map imaging to achieve the coincidence measurement of photoelectrons and photo-ions. This setup uses only one imaging detector (microchannel plates (MCP)/phosphor screen) but the voltages on electrodes are pulsed to push both electrons and ions toward the same detector. The ion-electron coincidence is achieved using two cameras to capture images of ions and electrons separately. The time-of-flight of ions and electrons are read out from MCP using a digitizer. We demonstrate this new system by studying the dissociative single and double ionization of PENNA (2-phenylethyl-N,N-dimethylamine). We further show that the camera-based 3D imaging system can operate at 10 kHz repetition rate.

Attosecond Electron Correlation Dynamics in Double Ionization of Benzene Probed with Two-Electron Angular Streaking.

With a novel three-dimensional electron-electron coincidence imaging technique and two-electron angular streaking method, we show that the emission time delay between two electrons can be measured from tens of attoseconds to more than 1 fs. Surprisingly, in benzene, the double ionization rate decays as the time delay between the first and second electron emission increases during the first 500 as. This is further supported by the decay of the Coulomb repulsion in the direction perpendicular to the laser polarization. This result reveals that laser-induced electron correlation plays a major role in strong field double ionization of benzene driven by a nearly circularly polarized field.

Note: An improved 3D imaging system for electron-electron coincidence measurements.

We demonstrate an improved imaging system that can achieve highly efficient 3D detection of two electrons in coincidence. The imaging system is based on a fast frame complementary metal-oxide semiconductor camera and a high-speed waveform digitizer. We have shown previously that this detection system is capable of 3D detection of ions and electrons with good temporal and spatial resolution. Here, we show that with a new timing analysis algorithm, this system can achieve an unprecedented dead-time (<0.7 ns) and dead-space (<1 mm) when detecting two electrons. A true zero dead-time detection is also demonstrated.

Communication: time- and space-sliced velocity map electron imaging.

We develop a new method to achieve slice electron imaging using a conventional velocity map imaging apparatus with two additional components: a fast frame complementary metal-oxide semiconductor camera and a high-speed digitizer. The setup was previously shown to be capable of 3D detection and coincidence measurements of ions. Here, we show that when this method is applied to electron imaging, a time slice of 32 ps and a spatial slice of less than 1 mm thick can be achieved. Each slice directly extracts 3D velocity distributions of electrons and provides electron velocity distributions that are impossible or difficult to obtain with a standard 2D imaging electron detector.

Coincidence ion imaging with a fast frame camera.

A new time- and position-sensitive particle detection system based on a fast frame CMOS (complementary metal-oxide semiconductors) camera is developed for coincidence ion imaging. The system is composed of four major components: a conventional microchannel plate/phosphor screen ion imager, a fast frame CMOS camera, a single anode photomultiplier tube (PMT), and a high-speed digitizer. The system collects the positional information of ions from a fast frame camera through real-time centroiding while the arrival times are obtained from the timing signal of a PMT processed by a high-speed digitizer. Multi-hit capability is achieved by correlating the intensity of ion spots on each camera frame with the peak heights on the corresponding time-of-flight spectrum of a PMT. Efficient computer algorithms are developed to process camera frames and digitizer traces in real-time at 1 kHz laser repetition rate. We demonstrate the capability of this system by detecting a momentum-matched co-fragments pair (methyl and iodine cations) produced from strong field dissociative double ionization of methyl iodide.

Bond-selective dissociation of polyatomic cations in mid-infrared strong fields.

Strong field-induced dissociation by intense mid-infrared pulses was investigated in bromofluoroform monocation (CF3Br(+)) and iodobenzene dication (C6H5I(2+)) using ab initio molecular dynamics calculations. In both systems, bond -selective dissociation was achieved using appropriate laser polarizations and wavelengths. For CF3Br(+), energetically disfavored fluorine elimination was strongly enhanced at wavelengths of 7 to 8 µm with polarization along a C-F bond. This is the result of two effects: the deposition of high enough kinetic energy into the molecule by the laser field and the near-resonant excitation of the C-F stretching mode. At shorter and off-resonant wavelengths, bromine elimination becomes significant due to rapid intramolecular vibrational energy redistribution (IVR). For C6H5I(2+), the branching ratios for the dissociation of the ortho-, meta-, and para-hydrogens can be controlled simply by changing the laser polarization. These results show the general applicability of bond selective dissociation of cations by intense mid-infrared laser fields.

Strong-field ionization rate depends on the sign of the magnetic quantum number.

We report the first experimental observation of the dependence of strong-field ionization rate on the sign of the magnetic quantum number. We measure the strong-field sequential double ionization yield of argon by two time-delayed near-circularly polarized laser pulses. It is found that double-ionization yield is enhanced more than 3 times if two lasers have the opposite helicities. Analysis shows that the single ionization of both the neutral and ion prefer the same sign of the magnetic quantum number. A qualitative and intuitive model is proposed to help understand this phenomenon.

Laser-induced low energy electron diffraction in aligned molecules.

We measured the photoelectron spectra and angular distributions of partially aligned N(2), O(2), and CO(2) in the rescattering plateau of above threshold ionization (ATI). The measured ATI electrons have relatively low collision energies (<15 eV). The photoelectron angular distributions (PAD) show clearly species and energy dependence. A simple two-center interference model was not able to consistently retrieve structural properties. We conclude that due to the interplay between the electrons and rescattering potential, the molecular structural information is obscured and cannot be extracted conveniently. However, the sensitivity of the PAD to the scattering potential in laser-induced electron diffraction promises a practical tool for studying electron-ion scattering dynamics.