89 citations · 533 across the 17 of their papers we have counts for
17 papers
High-Order Response Functions with Duschinsky Coupling and Finite Temperature: Application to Two-Dimensional Resonance Raman Spectroscopy
Luca Nils Philipp, Tomislav Begušić
In this work, we derive closed-form expressions for multi-time correlation functions underlying higher-order nonlinear spectroscopic response functions within the harmonic approxim…
Two-dimensional IR-Raman spectroscopy of vibrational polaritons: Role of dipole surfaces
Xinwei Ji, Tomislav Begusic, Tao E. Li
Nonlinear spectroscopy provides a unique perspective to understand time-resolved molecular dynamics under vibrational strong coupling (VSC). Herein, equilibrium-nonequilibrium cavi…
Real-time operator evolution in two and three dimensions via sparse Pauli dynamics
Tomislav Begušić, Garnet Kin-Lic Chan
We study real-time operator evolution using sparse Pauli dynamics, a recently developed method for simulating expectation values of quantum circuits. On the examples of energy and…
i-PI 3.0: a flexible and efficient framework for advanced atomistic simulations
Yair Litman, Venkat Kapil, Yotam M. Y. Feldman +13
Atomic-scale simulations have progressed tremendously over the past decade, largely due to the availability of machine-learning interatomic potentials. These potentials combine the…
Fast and converged classical simulations of evidence for the utility of quantum computing before fault tolerance
Tomislav Begušić, Johnnie Gray, Garnet Kin-Lic Chan
A recent quantum simulation of observables of the kicked Ising model on 127 qubits implemented circuits that exceed the capabilities of exact classical simulation. We show that sev…
Simulating quantum circuit expectation values by Clifford perturbation theory
Tomislav Begušić, Kasra Hejazi, Garnet Kin-Lic Chan
The classical simulation of quantum circuits is of central importance for benchmarking near-term quantum devices. The fact that gates belonging to the Clifford group can be simulat…
Computational Design of Molecular Probes for Electronic Pre-Resonance Raman Scattering Microscopy
Jiajun Du, Xuecheng Tao, Tomislav Begušić +1
Recently developed electronic pre-resonance stimulated Raman scattering (epr-SRS) microscopy, in which the Raman signal of a dye is significantly boosted by setting the incident la…
Two-dimensional infrared-Raman spectroscopy as a probe of water's tetrahedrality
Tomislav Begušić, Geoffrey A. Blake
Two-dimensional spectroscopic techniques combining terahertz (THz), infrared (IR), and visible pulses offer a wealth of information about coupling among vibrational modes in molecu…
Equilibrium-nonequilibrium ring-polymer molecular dynamics for nonlinear spectroscopy
Tomislav Begušić, Xuecheng Tao, Geoffrey A. Blake +1
Two-dimensional Raman and hybrid terahertz/Raman spectroscopic techniques provide invaluable insight into molecular structure and dynamics of condensed-phase systems. However, corr…
Applicability of the thawed Gaussian wavepacket dynamics to the calculation of vibronic spectra of molecules with double-well potential energy surfaces
Tomislav Begušić, Enrico Tapavicza, Jiří Vaníček
Simulating vibrationally resolved electronic spectra of anharmonic systems, especially those involving double-well potential energy surfaces, often requires expensive quantum dynam…
Finite-temperature, anharmonicity, and Duschinsky effects on the two-dimensional electronic spectra from ab initio thermo-field Gaussian wavepacket dynamics
Tomislav Begušić, Jiří Vaníček
Accurate description of finite-temperature vibrational dynamics is indispensable in the computation of two-dimensional electronic spectra. Such simulations are often based on the d…
On-the-fly ab initio semiclassical evaluation of third-order response functions for two-dimensional electronic spectroscopy
Tomislav Begušić, Jiří Vaníček
Ab initio computation of two-dimensional electronic spectra is an expanding field, whose goal is improving upon simple, few-dimensional models often employed to explain experiments…
On-the-fly ab initio semiclassical evaluation of vibronic spectra at finite temperature
Tomislav Begušić, Jiří Vaníček
To compute and analyze vibrationally resolved electronic spectra at zero temperature, we have recently implemented the on-the-fly ab initio extended thawed Gaussian approximation […
Semiclassical Approach to Photophysics Beyond Kasha's Rule and Vibronic Spectroscopy Beyond the Condon Approximation. The Case of Azulene
Antonio Prlj, Tomislav Begušić, Zhan Tong Zhang +7
Azulene is a prototypical molecule with an anomalous fluorescence from the second excited electronic state, thus violating Kasha's rule, and with an emission spectrum that cannot b…
Single-Hessian thawed Gaussian approximation: The missing rung on the ladder
Tomislav Begušić, Manuel Cordova, Jiří Vaníček
To alleviate the computational cost associated with on-the-fly ab initio semiclassical calculations of molecular spectra, we propose the single-Hessian thawed Gaussian approximatio…
On-the-fly ab initio semiclassical evaluation of absorption spectra of polyatomic molecules beyond the Condon approximation
Aurélien Patoz, Tomislav Begušić, Jiří Vaníček
To evaluate vibronic spectra beyond the Condon approximation, we extend the on-the-fly ab initio thawed Gaussian approximation by considering the Herzberg-Teller contribution due t…
On-the-fly ab initio semiclassical evaluation of time-resolved electronic spectra
Tomislav Begušić, Julien Roulet, Jiří Vaníček
We present a methodology for computing vibrationally and time-resolved pump-probe spectra, which takes into account all vibrational degrees of freedom and is based on the combinati…