Benjamin Lasorne
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View article: How an Equi-ensemble Description Systematically Outperforms the Weighted-ensemble Variational Quantum Eigensolver
How an Equi-ensemble Description Systematically Outperforms the Weighted-ensemble Variational Quantum Eigensolver Open
Calculating excited states in chemistry is crucial to provide insight into photoinduced molecular behavior beyond the ground state, enabling innovations in spectroscopy, material sciences, and drug design. While several approaches have bee…
View article: Quantum-computing within a bosonic context: Assessing finite basis effects on prototypical vibrational Hamiltonian spectra
Quantum-computing within a bosonic context: Assessing finite basis effects on prototypical vibrational Hamiltonian spectra Open
Quantum computing has recently been emerging in theoretical chemistry as a realistic avenue meant to offer computational speedup to challenging eigenproblems in the context of strongly-correlated molecular systems or extended materials. Mo…
View article: Wavepacket and reduced-density approaches for high-dimensional quantum dynamics: Application to the nonlinear spectroscopy of asymmetrical light-harvesting building blocks
Wavepacket and reduced-density approaches for high-dimensional quantum dynamics: Application to the nonlinear spectroscopy of asymmetrical light-harvesting building blocks Open
Excitation-energy transfer (EET) and relaxation in an optically excited building block of poly(phenylene ethynylene) (PPE) dendrimers are simulated using wavepackets with the multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) …
View article: Wavepacket and reduced-density approaches for high-dimensional quantum dynamics: Application to the nonlinear spectroscopy of asymmetrical light-harvesting building blocks
Wavepacket and reduced-density approaches for high-dimensional quantum dynamics: Application to the nonlinear spectroscopy of asymmetrical light-harvesting building blocks Open
Excitation-energy transfer (EET) and relaxation in an optically excited building block of poly(phenylene ethynylene) (PPE) dendrimers are simulated using wavepackets with the multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) …
View article: Ab Initio Polaritonic Chemistry on Diverse Quantum Computing Platforms: Qubit, Qudit, and Hybrid Qubit-Qumode Architectures
Ab Initio Polaritonic Chemistry on Diverse Quantum Computing Platforms: Qubit, Qudit, and Hybrid Qubit-Qumode Architectures Open
Trying to export ab initio polaritonic chemistry onto emerging quantum computers raises fundamental questions. A central one is how to efficiently represent both fermionic and bosonic degrees of freedom on the same platform, in order to de…
View article: Transformation-Free Generation of a Quasi-Diabatic Representation from the State-Average Orbital-Optimized Variational Quantum Eigensolver
Transformation-Free Generation of a Quasi-Diabatic Representation from the State-Average Orbital-Optimized Variational Quantum Eigensolver Open
In the present work, we examine how the recent quantum-computing algorithm known as the state-average orbital-optimized variational quantum eigensolver (SA-OO-VQE), viewed within the context of quantum chemistry as a type of multiconfigura…
View article: Transformation-free generation of a quasi-diabatic representation from the state-average orbital-optimized variational quantum eigensolver
Transformation-free generation of a quasi-diabatic representation from the state-average orbital-optimized variational quantum eigensolver Open
In the present work, we examine how the recent quantum-computing algorithm known as the state-average orbital-optimized variational quantum eigensolver (SA-OO-VQE), viewed within the context of quantum chemistry as a type of multiconfigura…
View article: Visible‐Light Organic Photosensitizers Based on 2‐(2‐Aminophenyl)benzothiazoles for Photocycloaddition Reactions
Visible‐Light Organic Photosensitizers Based on 2‐(2‐Aminophenyl)benzothiazoles for Photocycloaddition Reactions Open
We have studied 2‐(2‐aminophenyl)benzothiazole and related derivatives for their photophysical properties in view of employing them as new and readily tunable organic photocatalysts. Their triplet energies were estimated by DFT calculation…
View article: Excitation-Energy Transfer and Vibronic Relaxation through Light-Harvesting Dendrimer Building Blocks: a Nonadiabatic Perspective
Excitation-Energy Transfer and Vibronic Relaxation through Light-Harvesting Dendrimer Building Blocks: a Nonadiabatic Perspective Open
The light-harvesting excitonic properties of poly(phenylene ethynylene) (PPE) extended dendrimers (tree-like π-conjugated macromolecules) involve a directional cascade of local excitation-energy transfer (EET) processes occurring from the …
View article: Density functional theory beyond the Born-Oppenheimer approximation: Exact mapping onto an electronically non-interacting Kohn-Sham molecule
Density functional theory beyond the Born-Oppenheimer approximation: Exact mapping onto an electronically non-interacting Kohn-Sham molecule Open
This work presents an alternative, general, and in-principle exact extension of electronic Kohn-Sham density functional theory (KS-DFT) to the fully quantum-mechanical molecular problem. Unlike in existing multi-component or exact-factoriz…
View article: Unitary transformations within density matrix embedding approaches: A perspective on the self-consistent scheme for electronic structure calculation
Unitary transformations within density matrix embedding approaches: A perspective on the self-consistent scheme for electronic structure calculation Open
In this work, we introduce an original self-consistent scheme based on the\none-body reduced density matrix ($\\gamma$) formalism. A significant feature of\nthis methodology is the utilization of an optimal unitary transformation of the\nH…
View article: On the unusual Stokes shift in the smallest PPE dendrimer building block: Role of the vibronic symmetry on the band origin?
On the unusual Stokes shift in the smallest PPE dendrimer building block: Role of the vibronic symmetry on the band origin? Open
1,3-bis(phenylethynyl)benzene is the primary chromophore of light-harvesting polyphenylene ethynylene (PPE) dendrimers. It is experimentally known to share the same absorption spectrum as its pair of diphenylacetylene (aka. tolane) meta-su…
View article: Laser-controlled electronic symmetry breaking in a phenylene ethynylene dimer: Simulation by the hierarchical equations of motion and optimal control
Laser-controlled electronic symmetry breaking in a phenylene ethynylene dimer: Simulation by the hierarchical equations of motion and optimal control Open
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View article: Dynamical approximations for composite quantum systems: assessment of error estimates for a separable ansatz
Dynamical approximations for composite quantum systems: assessment of error estimates for a separable ansatz Open
Numerical studies are presented to assess error estimates for a separable (Hartree) approximation for dynamically evolving composite quantum systems which exhibit distinct scales defined by their mass and frequency ratios. The relevant err…
View article: Analytical Nonadiabatic Couplings and Gradients within the State-Averaged Orbital-Optimized Variational Quantum Eigensolver
Analytical Nonadiabatic Couplings and Gradients within the State-Averaged Orbital-Optimized Variational Quantum Eigensolver Open
We introduce several technical and analytical extensions to our recent state-averaged orbital-optimized variational quantum eigensolver (SA-OO-VQE) algorithm (see Yalouz et al. Quantum Sci. Technol. 2021, 6, 024004). Motivated by the limit…
View article: Dynamical approximations for composite quantum systems: Assessment of error estimates for a separable ansatz
Dynamical approximations for composite quantum systems: Assessment of error estimates for a separable ansatz Open
Numerical studies are presented to assess error estimates for a separable (Hartree) approximation for dynamically evolving composite quantum systems which exhibit distinct scales defined by their mass and frequency ratios. The relevant err…
View article: Analytical nonadiabatic couplings and gradients within the state-averaged orbital-optimized variational quantum eigensolver
Analytical nonadiabatic couplings and gradients within the state-averaged orbital-optimized variational quantum eigensolver Open
In this work, we introduce several technical and analytical extensions to our recent state-averaged orbital-optimized variational quantum eigensolver (SA-OO-VQE) algorithm (see Ref. [S. Yalouz et al. ,Quantum Sci. Technol. 6, 024004 (2021)…
View article: Separation of scales: dynamical approximations for composite quantum systems*
Separation of scales: dynamical approximations for composite quantum systems* Open
We consider composite quantum-dynamical systems that can be partitioned into weakly interacting subsystems, similar to system–bath type situations. Using a factorized wave function ansatz, we mathematically characterize dynamical scale sep…
View article: Funneling dynamics in a phenylacetylene trimer: Coherent excitation of donor excitonic states and their superposition
Funneling dynamics in a phenylacetylene trimer: Coherent excitation of donor excitonic states and their superposition Open
Funneling dynamics in conjugated dendrimers has raised great interest in the context of artificial light-harvesting processes. Photoinduced relaxation has been explored by time-resolved spectroscopy and simulations, mainly by semiclassical…
View article: Diabatization around Conical Intersections with a New Phase-Corrected Valence-Bond-Based Compression Approach
Diabatization around Conical Intersections with a New Phase-Corrected Valence-Bond-Based Compression Approach Open
In the present work, the valence-bond-based compression approach for diabatization (VBCAD), previously presented in the literature [J. Phys. Chem. Lett. 2020, 11, 5295-5301] in the case of avoided crossings, is extended to the more general…
View article: Quantum light-induced nonadiabatic phenomena in the absorption spectrum of formaldehyde: Full- and reduced-dimensionality studies
Quantum light-induced nonadiabatic phenomena in the absorption spectrum of formaldehyde: Full- and reduced-dimensionality studies Open
The coupling of a molecule to a cavity can induce conical intersections of the arising polaritonic potential energy surfaces. Such intersections give rise to the strongest possible nonadiabatic effects. By choosing an example that does not…
View article: Separation of scales: Dynamical approximations for composite quantum systems
Separation of scales: Dynamical approximations for composite quantum systems Open
We consider composite quantum-dynamical systems that can be partitioned into weakly interacting subsystems, similar to system-bath type situations. Using a factorized wave function ansatz, we mathematically characterize dynamical scale sep…
View article: Striking Generic Impact of Light-Induced Non-Adiabaticity in Polyatomic Molecules
Striking Generic Impact of Light-Induced Non-Adiabaticity in Polyatomic Molecules Open
Non-adiabaticity, i.e., the effect of mixing electronic states by nuclear motion, is a central phenomenon in molecular science. The strongest nonadiabatic effects arise due to the presence of conical intersections of electronic energy surf…
View article: A Novel Valence-Bond-Based Automatic Diabatization Method by Compression
A Novel Valence-Bond-Based Automatic Diabatization Method by Compression Open
A novel valence-bond-based automatic diabatization method by compression, called valence-bond-based compression approach for dibatization (VBCAD), is presented in this Letter. It is a "black-box" type method that provides an automatic diab…
View article: Striking light-induced nonadiabatic fingerprint in the low-energy vibronic spectra of polyatomic molecules
Striking light-induced nonadiabatic fingerprint in the low-energy vibronic spectra of polyatomic molecules Open
Nonadiabaticity, i.e., the effect of mixing electronic states by nuclear motion, is a central phenomenon in molecular science. The strongest nonadiabatic effects arise due to the presence of conical intersections of electronic energy surfa…
View article: Statistical distributions of the tuning and coupling collective modes at a conical intersection using the hierarchical equations of motion
Statistical distributions of the tuning and coupling collective modes at a conical intersection using the hierarchical equations of motion Open
We investigate the possibility of extracting the probability distribution of the effective environmental tuning and coupling modes during the nonadiabatic relaxation through a conical intersection. Dynamics are dealt with an open quantum s…
View article: Femtosecond wave-packet revivals in ozone
Femtosecond wave-packet revivals in ozone Open
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View article: A generalized vibronic-coupling Hamiltonian for molecules without symmetry: Application to the photoisomerization of benzopyran
A generalized vibronic-coupling Hamiltonian for molecules without symmetry: Application to the photoisomerization of benzopyran Open
We present a model for the lowest two potential energy surfaces (PESs) that describe the photoinduced ring-opening reaction of benzopyran taken as a model compound to study the photochromic ring-opening reaction of indolinobenzospiropyran …