scholarly journals Improved insights in time-resolved photoelectron imaging

2021 ◽  
Author(s):  
Nikoleta Kotsina ◽  
Dave Townsend
Keyword(s):  
Molecular Dynamics ◽  
Excited State ◽  
Data Analysis ◽  
Case Studies ◽  
Light Source ◽  
Imaging Technique ◽  
Photoelectron Imaging ◽  
Time Resolved

We review new light source developments and data analysis considerations relevant to the time-resolved photoelectron imaging technique. Case studies illustrate how these themes may enhance understanding in studies of excited state molecular dynamics.

Visualization and Manipulation of Molecular Motion in Solid State through Photo-Induced Clusteroluminescence

2019 ◽  
Author(s):  
Haoke Zhang ◽  
Lili Du ◽  
Lin Wang ◽  
Junkai Liu ◽  
Qing Wan ◽  
...  
Keyword(s):  
Quantum Mechanics ◽  
Excited State ◽  
Solid State ◽  
Light Source ◽  
Molecular Motion ◽  
Molecular Machine ◽  
Conjugated Molecules ◽  
Time Resolved ◽  
Packing Structure ◽  
New Strategy

<p>Building molecular machine has long been a dream of scientists as it is expected to revolutionize many aspects of technology and medicine. Implementing the solid-state molecular motion is the prerequisite for a practical molecular machine. However, few works on solid-state molecular motion have been reported and it is almost impossible to “see” the motion even if it happens. Here the light-driven molecular motion in solid state is discovered in two non-conjugated molecules <i>s</i>-DPE and <i>s</i>-DPE-TM, resulting in the formation of excited-state though-space complex (ESTSC). Meanwhile, the newly formed ESTSC generates an abnormal visible emission which is termed as clusteroluminescence. Notably, the original packing structure can recover from ESTSC when the light source is removed. These processes have been confirmed by time-resolved spectroscopy and quantum mechanics calculation. This work provides a new strategy to manipulate and “see” solid-state molecular motion and gains new insights into the mechanistic picture of clusteroluminescence.<br></p>

Observation of multi-channel non-adiabatic dynamics in aniline derivatives using time-resolved photoelectron imaging

2016 ◽  
Vol 194 ◽  
pp. 185-208 ◽  
Author(s):  
Magdalena M. Zawadzki ◽  
Marco Candelaresi ◽  
Lisa Saalbach ◽  
Stuart W. Crane ◽  
Martin J. Paterson ◽  
...  
Keyword(s):  
Excited State ◽  
Angular Distributions ◽  
Relaxation Dynamics ◽  
Photoelectron Imaging ◽  
Time Resolved ◽  
Valence States ◽  
Ultimate Fate ◽  
Site Selective ◽  
Photoelectron Angular Distributions ◽  
Electronic Character

We present results from a recent time-resolved photoelectron imaging (TRPEI) study investigating the non-adiabatic relaxation dynamics of N,N-dimethylaniline (N,N-DMA) and 3,5-dimethylaniline (3,5-DMA) following excitation at 240 nm. Analysis of the experimental data is supported by ab initio coupled-cluster calculations evaluating excited state energies and the evolution of several excited state physical properties as a function of N–H/N–CH3 bond extension – a critical reaction coordinate. The use of site-selective methylation brings considerable new insight to the existing body of literature concerning photochemical dynamics in the related system aniline at similar excitation wavelengths. The present work also builds on our own previous investigations in the same species at 250 nm. The TRPEI method provides highly differential energy- and angle-resolved data and, in particular, the temporal evolution of the photoelectron angular distributions afforded by the imaging approach offers much of the new dynamical information. In particular, we see no clear evidence of the second excited 2ππ* state non-adiabatically coupling to the lower-lying S1(ππ*) state or the mixed Rydberg/valence S2(3s/πσ*) state. This, in turn, potentially raises some unresolved questions about the overall nature of the dynamics operating in these systems, especially in regard to the 2ππ* state's ultimate fate. More generally, the findings for the aromatic systems N,N-DMA and 3,5-DMA, taken along with our recent TRPEI results for several aliphatic amine species, highlight interesting questions about the nature of electronic character evolution in mixed Rydberg-valence states as a function of certain key bond extensions and the extent of system conjugation. We begin exploring these ideas computationally for a systematically varied series of tertiary amines.

scholarly journals Time-resolved photoelectron imaging spectra from non-adiabatic molecular dynamics simulations

2013 ◽  
Vol 139 (13) ◽  
pp. 134104 ◽  
Author(s):  
Alexander Humeniuk ◽  
Matthias Wohlgemuth ◽  
Toshinori Suzuki ◽  
Roland Mitrić
Keyword(s):  
Molecular Dynamics ◽  
Molecular Dynamics Simulations ◽  
Photoelectron Imaging ◽  
Time Resolved ◽  
Dynamics Simulations

Visualization and Manipulation of Molecular Motion in Solid State through Photo-Induced Clusteroluminescence

2019 ◽  
Author(s):  
Haoke Zhang ◽  
Lili Du ◽  
Lin Wang ◽  
Junkai Liu ◽  
Qing Wan ◽  
...  
Keyword(s):  
Quantum Mechanics ◽  
Excited State ◽  
Solid State ◽  
Light Source ◽  
Molecular Motion ◽  
Molecular Machine ◽  
Conjugated Molecules ◽  
Time Resolved ◽  
Packing Structure ◽  
New Strategy

<p>Building molecular machine has long been a dream of scientists as it is expected to revolutionize many aspects of technology and medicine. Implementing the solid-state molecular motion is the prerequisite for a practical molecular machine. However, few works on solid-state molecular motion have been reported and it is almost impossible to “see” the motion even if it happens. Here the light-driven molecular motion in solid state is discovered in two non-conjugated molecules <i>s</i>-DPE and <i>s</i>-DPE-TM, resulting in the formation of excited-state though-space complex (ESTSC). Meanwhile, the newly formed ESTSC generates an abnormal visible emission which is termed as clusteroluminescence. Notably, the original packing structure can recover from ESTSC when the light source is removed. These processes have been confirmed by time-resolved spectroscopy and quantum mechanics calculation. This work provides a new strategy to manipulate and “see” solid-state molecular motion and gains new insights into the mechanistic picture of clusteroluminescence.<br></p>

Ultrafast decay dynamics of electronically excited 2-ethylpyrrole

2021 ◽  
Author(s):  
Wenpeng Yuan ◽  
Dongyuan Yang ◽  
Baihui Feng ◽  
Yanjun Min ◽  
Zhichao Chen ◽  
...  
Keyword(s):  
Excited State ◽  
Wavelength Range ◽  
Photoelectron Spectra ◽  
Imaging Method ◽  
Photoelectron Imaging ◽  
Time Resolved ◽  
State Decay ◽  
Electronically Excited ◽  
Uv Excitation

The excited-state decay dynamics of 2-ethylpyrrole following UV excitation at a wavelength range of 254.8-218.0 nm is investigated in detail using femtosecond time-resolved photoelectron imaging method. The time-resolved photoelectron spectra...

scholarly journals Ultrafast photoisomerisation of an isolated retinoid

2019 ◽  
Vol 21 (20) ◽  
pp. 10567-10579 ◽  
Author(s):  
James N. Bull ◽  
Christopher W. West ◽  
Cate S. Anstöter ◽  
Gabriel da Silva ◽  
Evan J. Bieske ◽  
...  
Keyword(s):  
Retinoic Acid ◽  
Excited State ◽  
Gas Phase ◽  
Laser Spectroscopy ◽  
Ion Mobility Spectrometry ◽  
Ion Mobility ◽  
Photoelectron Imaging ◽  
Time Resolved ◽  
Excited State Dynamics

The photoinduced excited state dynamics of gas-phase trans-retinoate (deprotonated trans-retinoic acid, trans-RA−) are studied using tandem ion mobility spectrometry coupled with laser spectroscopy, and frequency-, angle- and time-resolved photoelectron imaging.

scholarly journals Ultrafast valence to non-valence excited state dynamics in a common anionic chromophore

2019 ◽  
Vol 10 (1) ◽  
Author(s):  
James N. Bull ◽  
Cate S. Anstöter ◽  
Jan R. R. Verlet
Keyword(s):  
Excited State ◽  
Internal Conversion ◽  
Rydberg States ◽  
Bound State ◽  
Photoactive Yellow Protein ◽  
Coumaric Acid ◽  
Photoelectron Imaging ◽  
Time Resolved ◽  
Valence States

AbstractNon-valence states in neutral molecules (Rydberg states) have well-established roles and importance in photochemistry, however, considerably less is known about the role of non-valence states in photo-induced processes in anions. Here, femtosecond time-resolved photoelectron imaging is used to show that photoexcitation of the S1(ππ*) state of the methyl ester of deprotonated para-coumaric acid – a model chromophore for photoactive yellow protein (PYP) – leads to a bifurcation of the excited state wavepacket. One part remains on the S1(ππ*) state forming a twisted intermediate, whilst a second part leads to the formation of a non-valence (dipole-bound) state. Both populations eventually decay independently by vibrational autodetachment. Valence-to-non-valence internal conversion has hitherto not been observed in the intramolecular photophysics of an isolated anion, raising questions into how common such processes might be, given that many anionic chromophores have bright valence states near the detachment threshold.

Excited state dynamics and conformations of a Cu(ii)-phthalocyanine-perylenebisimide dyad

2017 ◽  
Vol 19 (33) ◽  
pp. 22169-22176 ◽  
Author(s):  
K. Wilma ◽  
T. Unger ◽  
S. Tuncel Kostakoğlu ◽  
M. Hollfelder ◽  
C. Hunger ◽  
...  
Keyword(s):  
Molecular Dynamics ◽  
Excited State ◽  
Molecular Dynamics Simulations ◽  
Time Resolved ◽  
Time Resolved Spectroscopy ◽  
Excited State Dynamics ◽  
Donor Acceptor ◽  
Dynamics Simulations

We present a full characterisation of a new donor–acceptor CuPc-PBI-dyad using time-resolved spectroscopy as well as molecular dynamics simulations.

Sign in / Sign up

Export Citation Format

Share Document