About

Dipti Jasrasaria is an Assistant Professor in the Department of Chemistry at The University of Chicago. Her research focuses on understanding how microscopic interactions between atoms and electrons in materials influence their macroscopic behaviors. She employs theory and simulation techniques, including electronic structure calculations, molecular dynamics simulations, and quantum dynamics, to model complex materials under experimentally relevant conditions. Her work aims to elucidate optoelectronic, dynamical, and transport phenomena in materials systems, with the goal of developing design principles to optimize materials for applications such as quantum information and energy conversion. Jasrasaria's educational background includes an A.B. in Chemistry and Statistics from Harvard University, an M.Phil in Scientific Computing from the University of Cambridge, and a Ph.D. in Chemistry from the University of California, Berkeley. She has also conducted postdoctoral research at Columbia University. Her contributions to the field have been recognized through several awards, including the ACS Young Investigator Award in Theory, the ACS COMP Wiley Computers in Chemistry Outstanding Postdoc Award, and the Frederick A. Howes Scholar in Computational Science. She works closely with experimental groups to synthesize and characterize novel materials, integrating theoretical insights with experimental efforts.

Research topics

• Physics
• Optoelectronics
• Materials science
• Chemistry
• Molecular physics
• Atomic physics
• Chemical physics
• Condensed matter physics
• Optics
• Quantum mechanics

Selected publications

• Correlating Structure and Function in Chiral Perovskites

  Knowledge@UChicago (University of Chicago) · 2026-01-01

  otherOpen accessSenior author

  Within the last five years, growing attention has been given to a new class of semiconductors called chiral perovskites. These perovskites have potential applications in light-based electronics, such as high-contrast LED displays and next-generation solar cells. A defining aspect of chiral perovskites is that their crystal structures contain chiral organic molecules, which give these perovskites unique properties, including the potential to filter electrons based on their spins. However, scientists currently lack a clear theoretical understanding of how a chiral perovskite’s molecular structure can affect its spin-filtering properties, and this has limited the ability to design new chiral perovskites with better performance and stability. We hypothesize that circular atomic vibrations called chiral phonons may mediate this relationship. In this exploratory research, I will use a machine learning model of the perovskite’s interatomic interactions, MACE, to calculate the circular vibrations of various chiral perovskites containing different organic molecules. I will characterize the energies and group velocities of these vibrations and use animations to visualize the vibrations. Our goal is to identify whether circular atomic vibrations exist in chiral perovskites, and if they do, uncover how these vibrations may help explain the functions of the material. This research will further current understanding of chiral perovskites, which is necessary for future research to design highly efficient light-based technologies.

  PublisherOA PDFDOI

• Simulating anharmonic vibrational polaritons beyond the long wavelength approximation

  The Journal of Chemical Physics · 2025-01-02 · 4 citations

  article1st authorCorresponding

  In this work, we investigate anharmonic vibrational polaritons formed due to strong light-matter interactions in an optical cavity between radiation modes and anharmonic vibrations beyond the long-wavelength limit. We introduce a conceptually simple description of light-matter interactions, where spatially localized cavity radiation modes couple to localized vibrations. Within this theoretical framework, we employ self-consistent phonon theory and vibrational dynamical mean-field theory to efficiently simulate momentum-resolved vibrational-polariton spectra, including effects of anharmonicity. Numerical simulations in model systems demonstrate the accuracy and applicability of our approach.

  PublisherDOI

• Strong anharmonicity dictates ultralow thermal conductivities of type-I clathrates

  Physical review. B./Physical review. B · 2025-06-25 · 3 citations

  article1st authorCorresponding
  PublisherDOI

• Simulating anharmonic vibrational polaritons beyond the long wavelength approximation

  arXiv (Cornell University) · 2024-09-12

  preprintOpen access1st authorCorresponding

  In this work we investigate anharmonic vibrational polaritons formed due to strong light-matter interactions in an optical cavity between radiation modes and anharmonic vibrations beyond the long-wavelength limit. We introduce a conceptually simple description of light-matter interactions, where spatially localized cavity radiation modes couple to localized vibrations. Within this theoretical framework, we employ self-consistent phonon theory and vibrational dynamical mean-field theory to efficiently simulate momentum-resolved vibrational-polariton spectra, including effects of anharmonicity. Numerical simulations in model systems demonstrate the accuracy and applicability of our approach.

  PublisherOA PDFDOI

• Strong anharmonicity dictates ultralow thermal conductivities of type-I clathrates

  arXiv (Cornell University) · 2024-09-12

  preprintOpen access1st authorCorresponding

  Type-I clathrate solids have attracted significant interest due to their ultralow thermal conductivities and subsequent promise for thermoelectric applications, yet the mechanisms underlying these properties are not well understood. Here, we extend the framework of vibrational dynamical mean-field theory (VDMFT) to calculate temperature-dependent thermal transport properties of $X_8$Ga$_{16}$Ge$_{30}$, where $X=$ Ba, Sr, using a many-body Green's function approach. We find that nonresonant scattering between cage acoustic modes and rattling modes leads to a reduction of acoustic phonon lifetimes and thus thermal conductivities. Moreover, we find that the moderate temperature dependence of conductivities above 300 K, which is consistent with experimental measurements, cannot be reproduced by standard perturbation theory calculations, which predict a $T^{-1}$ dependence. Therefore, we conclude that nonperturbative anharmonic effects, including four- and higher-phonon scattering processes, are responsible for the ultralow thermal conductivities of type-I clathrates.

  PublisherOA PDFDOI

• Nonperturbative Simulation of Anharmonic Rattler Dynamics in Type-I Clathrates with Vibrational Dynamical Mean-Field Theory

  arXiv (Cornell University) · 2024-02-12

  preprintOpen access1st authorCorresponding

  We use vibrational dynamical mean-field theory (VDMFT) to study the vibrational structure of type-I clathrate solids, specifically X$_8$Ga$_{16}$Ge$_{30}$, where X=Ba,Sr. These materials are cage-like chemical structures hosting loosely bound guest atoms, resulting in strong anharmonicity, short phonon lifetimes, and ultra-low thermal conductivities. Presenting the methodological developments necessary for this first application to three-dimensional, atomistic materials, we validate our approach through comparison to molecular dynamics simulations and show that VDMFT is extremely accurate at a fraction of the cost. Through the use of nonperturbative methods, we find that anharmonicity is dominated by four-phonon and higher-order scattering processes, and it causes rattler modes to shift up in frequency by 50% (10 cm$^{-1}$) and to have lifetimes of less than 1 ps; this behavior is not captured by traditional perturbation theory. Furthermore, we analyze the phonon self-energy and find that anharmonicity mixes guest rattling modes and cage acoustic modes, significantly changing the character of the harmonic phonons.

  PublisherOA PDFDOI

• Nonperturbative simulation of anharmonic rattler dynamics in type-I clathrates with vibrational dynamical mean-field theory

  Physical review. B./Physical review. B · 2024-08-14 · 6 citations

  articleOpen access1st authorCorresponding

  We use vibrational dynamical mean-field theory (VDMFT) to study the vibrational structure of type-I clathrate solids, specifically ${X}_{8}{\mathrm{Ga}}_{16}{\mathrm{Ge}}_{30}$, where $X=\text{Ba,}\phantom{\rule{4.pt}{0ex}}\text{Sr}$. These materials are cagelike chemical structures hosting loosely bound guest atoms, resulting in strong anharmonicity, short phonon lifetimes, and ultralow thermal conductivities. Presenting the methodological developments necessary for application to three-dimensional, atomistic materials, we validate our approach through comparison to molecular dynamics simulations and show that VDMFT is extremely accurate at a fraction of the cost. Through the use of nonperturbative methods, we find that anharmonicity is dominated by four-phonon and higher-order scattering processes, and it causes rattler modes to shift up in frequency by 50% $(10 {\mathrm{cm}}^{\ensuremath{-}1})$ and to have lifetimes of less than 1 ps; this behavior is not captured by traditional perturbation theory. Furthermore, we analyze the phonon self-energy and find that anharmonicity mixes guest rattling modes and cage acoustic modes, significantly changing the character of the harmonic phonons.

  PublisherOA PDFDOI

• Two-Dimensional Electronic Spectroscopy Reveals Dynamics within the Bright Fine Structure of CdSe Quantum Dots

  The Journal of Physical Chemistry Letters · 2024-02-05 · 11 citations

  article

  Semiconductor quantum dots are characterized by a discrete excitonic structure featuring coarse as well as fine structure. The lowest fine structure states have splittings into bright-dark states which are now well confirmed by single dot spectroscopy. In contrast, the splitting of the lowest coarse exciton into bright-bright fine structure states has not been observed nor the dynamics between these states. Here, we use the unique combination of time and energy resolution of two-dimensional electronic spectroscopy to directly observe the fine structure splittings into a bright-bright doublet. These splittings are strongly size dependent, with population relaxation on the <100 fs time scale.

  PublisherDOI

• Circumventing the Phonon Bottleneck by Multiphonon-Mediated Hot Exciton Cooling at the Nanoscale

  arXiv (Cornell University) · 2023-01-17 · 1 citations

  preprintOpen access1st authorCorresponding

  In semiconductor materials, hot exciton cooling is the process by which highly excited carriers nonradiatively relax to form a band edge exciton. While cooling plays an important role in determining the thermal losses and quantum yield of a system, the timescales and mechanism of cooling are not well understood in confined semiconductor nanocrystals (NCs). A mismatch between electronic energy gaps and phonon frequencies in NCs has led to the hypothesis of a phonon bottleneck, in which cooling would be extremely slow, while enhanced electron-hole interactions in NCs have been used to explain cooling that would occur on ultrafast timescales. Here, we develop an atomistic approach for describing phonon-mediated exciton dynamics, and we use it to simulate hot exciton cooling in NCs of experimentally relevant sizes. Our framework includes electron-hole correlations as well as multiphonon processes, both of which are necessary to accurately describe the cooling process. We find that cooling occurs on timescales of tens of femtoseconds in CdSe cores, in agreement with experimental measurements, through a cascade of relaxation events that are mediated by efficient multiphonon emission. Cooling timescales increase with increasing NC size due to decreased exciton-phonon coupling (EXPC), and they are an order of magnitude larger in CdSe-CdS core-shell NCs because of reduced EXPC to low- and mid-frequency acoustic modes.

  PublisherOA PDFDOI

• Detecting, distinguishing, and spatiotemporally tracking photogenerated charge and heat at the nanoscale

  arXiv (Cornell University) · 2023-05-23

  preprintOpen access

  Since dissipative processes are ubiquitous in semiconductors, characterizing how electronic and thermal energy transduce and transport at the nanoscale is vital for understanding and leveraging their fundamental properties. For example, in low-dimensional transition metal dichalcogenides (TMDCs), excess heat generation upon photoexcitation is difficult to avoid since even with modest injected exciton densities, exciton-exciton annihilation still occurs. Both heat and photoexcited electronic species imprint transient changes in the optical response of a semiconductor, yet the unique signatures of each are difficult to disentangle in typical spectra due to overlapping resonances. In response, we employ stroboscopic optical scattering microscopy (stroboSCAT) to simultaneously map both heat and exciton populations in few-layer \ch{MoS2} on relevant nanometer and picosecond length- and time scales and with 100-mK temperature sensitivity. We discern excitonic contributions to the signal from heat by combining observations close to and far from exciton resonances, characterizing photoinduced dynamics for each. Our approach is general and can be applied to any electronic material, including thermoelectrics, where heat and electronic observables spatially interplay, and lays the groundwork for direct and quantitative discernment of different types of coexisting energy without recourse to complex models or underlying assumptions.

  PublisherOA PDFDOI

Frequent coauthors

• Eran Rabani

  82 shared

• Joeson Wong

  52 shared

• Harry A. Atwater

  California Institute of Technology

  52 shared

• Cora M. Went

  University of California, Berkeley

  51 shared

• H. Weaver

  University of Edinburgh

  51 shared

• Naomi S. Ginsberg

  University of California, Berkeley

  18 shared

• Daniel Weinberg

  Lawrence Berkeley National Laboratory

  8 shared

• Avishek Das

  University of California, Berkeley

  7 shared

Labs

• The Jasrasaria GroupPI

Education

• Ph.D., Chemistry

  University of California Berkeley

  2022

• M.Phil., Scientific Computing

  University of Cambridge

  2017

• A. B., Chemistry

  Harvard University

  2016

Awards & honors

• ACS PHYS Young Investigator Award in Theory (2024)
• American Chemical Society Outstanding Postdoc Award (2024)
• Frederick A. Howes Scholar in Computational Science (2023)
• ACS COMP Chemical Computing Group Excellence Award for Gradu…
• Department of Energy Computational Science Graduate Fellowsh…