Adi Natan
Staff Scientist, SLAC National Accelerator Laboratory
Web page: http://web.stanford.edu/people/natan
Bio
Dr Natan leads the Non-Periodic ultrafast X-ray Imaging group at the Stanford PULSE Institute, where the research focuses on imaging ultrafast atomic motion in systems that interact with complex fields and environments, mostly using ultrafast X-ray FEL pulses. The purpose of this research is to study light-matter interaction in the shortest length and timescales, to uncover the interplay between correlated electronic motion and relaxation, nuclear motion, and photo-absorption processes. The research team develops experimental and computational tools to image quantum dynamics at the atomic scale, with the aim to overcome the limits of current approaches that rely on modeling and simulation. The research also leverages recent advances in ultrafast x-ray lasers, like the LCLS at SLAC National Accelerator Laboratory, and helps develop effective protocols, new modalities, detection schemes, and demonstrates important new capabilities as soon as they become feasible. Previously, Dr Natan was the co-PI of the Strong Field AMO physics task at PULSE, where he studied strong-field light-matter interaction in atoms and molecules, in particular, light-induced conical intersections, imaging strong-field ionization dynamics, and attosecond electronic delays.
Dr Natan received his PhD in Physics from the Weizmann Institute of Science, where he worked with Prof. Yaron Silberberg on coherent control, strong field interaction, nonlinear spectroscopy, and quantum optics. He was later a postdoctoral fellow at PULSE under the supervision of Prof. Phil Bucksbaum working on strong field AMO physics, and ultrafast X-ray science.
Current Role at Stanford
Principal investigator, Stanford PULSE Institute
Education & Certifications
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PhD, Weizmann Institute of Science
All Publications
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Characterization of Deformational Isomerization Potential and Interconversion Dynamics with Ultrafast X-ray Solution Scattering.
Journal of the American Chemical Society
2024
Abstract
Dimeric complexes composed of d8 square planar metal centers and rigid bridging ligands provide model systems to understand the interplay between attractive dispersion forces and steric strain in order to assist the development of reliable methods to model metal dimer complexes more broadly. [Ir2 (dimen)4]2+ (dimen = para-diisocyanomenthane) presents a unique case study for such phenomena, as distortions of the optimal structure of a ligand with limited conformational flexibility counteract the attractive dispersive forces from the metal and ligand to yield a complex with two ground state deformational isomers. Here, we use ultrafast X-ray solution scattering (XSS) and optical transient absorption spectroscopy (OTAS) to reveal the nature of the equilibrium distribution and the exchange rate between the deformational isomers. The two ground state isomers have spectrally distinct electronic excitations that enable the selective excitation of one isomer or the other using a femtosecond duration pulse of visible light. We then track the dynamics of the nonequilibrium depletion of the electronic ground state population─often termed the ground state hole─with ultrafast XSS and OTAS, revealing a restoration of the ground state equilibrium in 2.3 ps. This combined experimental and theoretical study provides a critical test of various density functional approximations in the description of bridged d8-d8 metal complexes. The results show that density functional theory calculations can reproduce the primary experimental observations if dispersion interactions are added, and a hybrid functional, which includes exact exchange, is used.
View details for DOI 10.1021/jacs.4c00817
View details for PubMedID 38727611
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Real-space inversion and super-resolution of ultrafast scattering
PHYSICAL REVIEW A
2023; 107 (2)
View details for DOI 10.1103/PhysRevA.107.023105
View details for Web of Science ID 000933248300002
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Transient vibration and product formation of photoexcited CS2 measured by time-resolved x-ray scattering.
The Journal of chemical physics
2022; 157 (16): 164305
Abstract
We have observed details of the internal motion and dissociation channels in photoexcited carbon disulfide (CS2) using time-resolved x-ray scattering (TRXS). Photoexcitation of gas-phase CS2 with a 200nm laser pulse launches oscillatory bending and stretching motion, leading to dissociation of atomic sulfur in under a picosecond. During the first 300fs following excitation, we observe significant changes in the vibrational frequency as well as some dissociation of the C-S bond, leading to atomic sulfur in the both 1D and 3P states. Beyond 1400fs, the dissociation is consistent with primarily 3P atomic sulfur dissociation. This channel-resolved measurement of the dissociation time is based on our analysis of the time-windowed dissociation radial velocity distribution, which is measured using the temporal Fourier transform of the TRXS data aided by a Hough transform that extracts the slopes of linear features in an image. The relative strength of the two dissociation channels reflects both their branching ratio and differences in the spread of their dissociation times. Measuring the time-resolved dissociation radial velocity distribution aids the resolution of discrepancies between models for dissociation proposed by prior photoelectron spectroscopy work.
View details for DOI 10.1063/5.0113079
View details for PubMedID 36319419
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Attosecond coherent electron motion in Auger-Meitner decay.
Science (New York, N.Y.)
1800: eabj2096
Abstract
[Figure: see text].
View details for DOI 10.1126/science.abj2096
View details for PubMedID 34990213
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Disentangling the subcycle electron momentum spectrum in strong-field ionization
PHYSICAL REVIEW RESEARCH
2021; 3 (2)
View details for DOI 10.1103/PhysRevResearch.3.023065
View details for Web of Science ID 000643687200002
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Resolving multiphoton processes with high-order anisotropy ultrafast X-ray scattering.
Faraday discussions
2021
Abstract
We present the first results on experimentally measured ultrafast X-ray scattering of strongly driven molecular iodine and analysis of high-order anisotropic components of the scattering signal. We discuss the technical details of retrieving high fidelity high-order anisotropy components from the measured scattering data and outline a method to analyze such signals using Legendre decomposition. We describe how anisotropic motions can be extracted from the various Legendre orders using simulated anisotropic scattering signals and Fourier analysis. We implement the method on the measured signal and observe a multitude of dissociation and vibration motions simultaneously arising from various multiphoton transitions occurring in the sample. We use the anisotropic scattering information to disentangle the different processes and assign their dissociation velocities on the Angstrom and femtosecond scales de novo.
View details for DOI 10.1039/d0fd00126k
View details for PubMedID 33565543
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Electronic Population Transfer via Impulsive Stimulated X-Ray Raman Scattering with Attosecond Soft-X-Ray Pulses.
Physical review letters
2020; 125 (7): 073203
Abstract
Free-electron lasers provide a source of x-ray pulses short enough and intense enough to drive nonlinearities in molecular systems. Impulsive interactions driven by these x-ray pulses provide a way to create and probe valence electron motions with high temporal and spatial resolution. Observing these electronic motions is crucial to understand the role of electronic coherence in chemical processes. A simple nonlinear technique for probing electronic motion, impulsive stimulated x-ray Raman scattering (ISXRS), involves a single impulsive interaction to produce a coherent superposition of electronic states. We demonstrate electronic population transfer via ISXRS using broad bandwidth (5.5 eV full width at half maximum) attosecond x-ray pulses produced by the Linac Coherent Light Source. The impulsive excitation is resonantly enhanced by the oxygen 1s→2π^{*} resonance of nitric oxide (NO), and excited state neutral molecules are probed with a time-delayed UV laser pulse.
View details for DOI 10.1103/PhysRevLett.125.073203
View details for PubMedID 32857563
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Electronic Population Transfer via Impulsive Stimulated X-Ray Raman Scattering with Attosecond Soft-X-Ray Pulses
PHYSICAL REVIEW LETTERS
2020; 125 (7)
View details for DOI 10.1103/PhysRevLett.125.073203
View details for Web of Science ID 000558086800003
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Characterizing Multiphoton Excitation Using Time-Resolved X-ray Scattering
PHYSICAL REVIEW X
2020; 10 (1)
View details for DOI 10.1103/PhysRevX.10.011065
View details for Web of Science ID 000519993700001
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X-ray diffractive imaging of controlled gas-phase molecules: Toward imaging of dynamics in the molecular frame.
The Journal of chemical physics
2020; 152 (8): 084307
Abstract
We report experimental results on the diffractive imaging of three-dimensionally aligned 2,5-diiodothiophene molecules. The molecules were aligned by chirped near-infrared laser pulses, and their structure was probed at a photon energy of 9.5 keV (lambda 130 pm) provided by the Linac Coherent Light Source. Diffracted photons were recorded on the Cornell-SLAC pixel array detector, and a two-dimensional diffraction pattern of the equilibrium structure of 2,5-diiodothiophene was recorded. The retrieved distance between the two iodine atoms agrees with the quantum-chemically calculated molecular structure to be within 5%. The experimental approach allows for the imaging of intrinsic molecular dynamics in the molecular frame, albeit this requires more experimental data, which should be readily available at upcoming high-repetition-rate facilities.
View details for DOI 10.1063/1.5133963
View details for PubMedID 32113333
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Tunable isolated attosecond X-ray pulses with gigawatt peak power from a free-electron laser
NATURE PHOTONICS
2020; 14 (1): 30-+
View details for DOI 10.1038/s41566-019-0549-5
View details for Web of Science ID 000504727600007
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Attosecond transient absorption spooktroscopy: a ghost imaging approach to ultrafast absorption spectroscopy.
Physical chemistry chemical physics : PCCP
2019
Abstract
The recent demonstration of isolated attosecond pulses from an X-ray free-electron laser (XFEL) opens the possibility for probing ultrafast electron dynamics at X-ray wavelengths. An established experimental method for probing ultrafast dynamics is X-ray transient absorption spectroscopy, where the X-ray absorption spectrum is measured by scanning the central photon energy and recording the resultant photoproducts. The spectral bandwidth inherent to attosecond pulses is wide compared to the resonant features typically probed, which generally precludes the application of this technique in the attosecond regime. In this paper we propose and demonstrate a new technique to conduct transient absorption spectroscopy with broad bandwidth attosecond pulses with the aid of ghost imaging, recovering sub-bandwidth resolution in photoproduct-based absorption measurements.
View details for DOI 10.1039/c9cp03951a
View details for PubMedID 31793561
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On the limits of observing motion in time-resolved X-ray scattering
PHILOSOPHICAL TRANSACTIONS OF THE ROYAL SOCIETY A-MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES
2019; 377 (2145)
View details for DOI 10.1098/rsta.2017.0477
View details for Web of Science ID 000465499800010
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On the limits of observing motion in time-resolved X-ray scattering.
Philosophical transactions. Series A, Mathematical, physical, and engineering sciences
2019; 377 (2145): 20170477
Abstract
Limits on the ability of time-resolved X-ray scattering (TRXS) to observe harmonic motion of amplitude, A and frequency, omega0, about an equilibrium position, R0, are considered. Experimental results from a TRXS experiment at the LINAC Coherent Light Source are compared to classical and quantum theories that demonstrate a fundamental limitation on the ability to observe the amplitude of motion. These comparisons demonstrate dual limits on the spatial resolution through Qmax and the temporal resolution through omegamax for observing the amplitude of motion. In the limit where omegamax omega0, the smallest observable amplitude of motion is A=2 pi/ Qmax. In the limit where omegamax≥2 omega0, A≤2 pi/ Qmax is observable provided there are sufficient statistics. This article is part of the theme issue 'Measurement of ultrafast electronic and structural dynamics with X-rays'.
View details for PubMedID 30929636
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Generation and Characterization of Attosecond Pulses from an X-ray Free-electron Laser
IEEE. 2019
View details for Web of Science ID 000482226301273
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Characterizing isolated attosecond pulses with angular streaking
OPTICS EXPRESS
2018; 26 (4): 4531–47
Abstract
We present a reconstruction algorithm for isolated attosecond pulses, which exploits the phase dependent energy modulation of a photoelectron ionized in the presence of a strong laser field. The energy modulation due to a circularly polarized laser field is manifest strongly in the angle-resolved photoelectron momentum distribution, allowing for complete reconstruction of the temporal and spectral profile of an attosecond burst. We show that this type of reconstruction algorithm is robust against counting noise and suitable for single-shot experiments. This algorithm holds potential for a variety of applications for attosecond pulse sources.
View details for DOI 10.1364/OE.26.004531
View details for Web of Science ID 000426268500073
View details for PubMedID 29475303
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Fourier-transform inelastic x-ray scattering: A new kind of gas-phase vibrational spectroscopy
IEEE. 2018
View details for Web of Science ID 000526031000400
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Imaging the breakdown of molecular-frame dynamics through rotational uncoupling
PHYSICAL REVIEW A
2017; 95 (6)
View details for DOI 10.1103/PhysRevA.95.061403
View details for Web of Science ID 000404014100001
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Observation of Quantum Interferences via Light-Induced Conical Intersections in Diatomic Molecules
PHYSICAL REVIEW LETTERS
2016; 116 (14)
Abstract
We observe energy-dependent angle-resolved diffraction patterns in protons from strong-field dissociation of the molecular hydrogen ion H_{2}^{+}. The interference is a characteristic of dissociation around a laser-induced conical intersection (LICI), which is a point of contact between two surfaces in the dressed two-dimensional Born-Oppenheimer potential energy landscape of a diatomic molecule in a strong laser field. The interference magnitude and angular period depend strongly on the energy difference between the initial state and the LICI, consistent with coherent diffraction around a cone-shaped potential barrier whose width and thickness depend on the relative energy of the initial state and the cone apex. These findings are supported by numerical solutions of the time-dependent Schrödinger equation for similar experimental conditions.
View details for DOI 10.1103/PhysRevLett.116.143004
View details for Web of Science ID 000373587500007
View details for PubMedID 27104704
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Observing the Uncoupling of Electron Motion from the Molecular Frame in Photoelectron Angular Distributions
IEEE. 2016
View details for Web of Science ID 000391286400498
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Strongly aligned gas-phase molecules at free-electron lasers
JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS
2015; 48 (20)
View details for DOI 10.1088/0953-4075/48/20/204002
View details for Web of Science ID 000362421800004
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Ultrafast isomerization initiated by X-ray core ionization.
Nature communications
2015; 6: 8199-?
Abstract
Rapid proton migration is a key process in hydrocarbon photochemistry. Charge migration and subsequent proton motion can mitigate radiation damage when heavier atoms absorb X-rays. If rapid enough, this can improve the fidelity of diffract-before-destroy measurements of biomolecular structure at X-ray-free electron lasers. Here we study X-ray-initiated isomerization of acetylene, a model for proton dynamics in hydrocarbons. Our time-resolved measurements capture the transient motion of protons following X-ray ionization of carbon K-shell electrons. We Coulomb-explode the molecule with a second precisely delayed X-ray pulse and then record all the fragment momenta. These snapshots at different delays are combined into a 'molecular movie' of the evolving molecule, which shows substantial proton redistribution within the first 12 fs. We conclude that significant proton motion occurs on a timescale comparable to the Auger relaxation that refills the K-shell vacancy.
View details for DOI 10.1038/ncomms9199
View details for PubMedID 26354002
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Experimental Signature of Light Induced Conical Intersections in Diatomics
SPRINGER-VERLAG BERLIN. 2015: 122–25
View details for DOI 10.1007/978-3-319-13242-6_29
View details for Web of Science ID 000357738800029
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Probing electron delays in above-threshold ionization
OPTICA
2014; 1 (6): 361-364
View details for DOI 10.1364/OPTICA.1.000361
View details for Web of Science ID 000354864400001
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Experimental Observation of Light Induced Conical Intersections in a Diatomic Molecule
IEEE. 2014
View details for Web of Science ID 000369908600478
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Quantum control of photodissociation by manipulation of bond softening
PHYSICAL REVIEW A
2012; 86 (4)
View details for DOI 10.1103/PhysRevA.86.043418
View details for Web of Science ID 000309808000014