Charge carrier nonadiabatic dynamics in non-metal doped graphitic carbon nitride

Agrawal, Sraddha; Vasenko, Andrey S.; Trivedi, Dhara J.; Prezhdo, Oleg V.

doi:10.1063/5.0079085

Title: Charge carrier nonadiabatic dynamics in non-metal doped graphitic carbon nitride

Journal Article · 28 February 2022 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/5.0079085 · OSTI ID:1979020

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Univ. of Southern California, Los Angeles, CA (United States); Univ. of Southern California, Los Angeles, CA (United States)
National Research University of Higher School of Economics, Moscow (Russian Federation); Russian Academy of Sciences (RAS), Moscow (Russian Federation)
Clarkson Univ., Potsdam, NY (United States)
Univ. of Southern California, Los Angeles, CA (United States)

Graphitic carbon nitride (GCN) has attracted significant attention due to its excellent performance in photocatalytic applications. Non-metal doping of GCN has been widely used to improve the efficiency of the material as a photocatalyst. Using a combination of time-domain density functional theory with nonadiabatic molecular dynamics, we study the charge carrier dynamics in oxygen and boron doped GCN systems. The reported simulations provide a detailed time-domain mechanistic description of the charge separation and recombination processes that are of fundamental importance while evaluating the photovoltaic and photocatalytic performance of the material. The appearance of smaller energy gaps due to the presence of dopant states improves the visible light absorption range of the doped systems. At the same time, the nonradiative lifetimes are shortened in the doped systems as compared to the pristine GCN. In the case of boron doped at a carbon (B–C–GCN), the charge recombination time is very long as compared to the other two doped systems owing to the smaller electron–phonon coupling strength between the valence band maximum and the trap state. The results suggest B–C–GCN as the most suitable candidate among three doped systems studied in this work for applications in photocatalysis. Finally, this work sheds light into the influence of dopants on quantum dynamics processes that govern GCN performance and, thus, guides toward building high-performance devices in photocatalysis.

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Research Organization:: Univ. of Southern California, Los Angeles, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC); National Science Foundation (NSF)

Grant/Contract Number:: SC0014429

OSTI ID:: 1979020

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 9 Vol. 156; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (58)

Polymeric Photocatalysts Based on Graphitic Carbon Nitride Cao, Shaowen; Low, Jingxiang; Yu, Jiaguo Advanced Materials, Vol. 27, Issue 13 https://doi.org/10.1002/adma.201500033	journal	February 2015
Density functional theory and the band gap problem Perdew, John P. International Journal of Quantum Chemistry, Vol. 28, Issue S19 https://doi.org/10.1002/qua.560280846	journal	March 1985
Recent Advances of Graphitic Carbon Nitride-Based Structures and Applications in Catalyst, Sensing, Imaging, and LEDs Wang, Aiwu; Wang, Chundong; Fu, Li Nano-Micro Letters, Vol. 9, Issue 4 https://doi.org/10.1007/s40820-017-0148-2	journal	June 2017
One step synthesis of oxygen doped porous graphitic carbon nitride with remarkable improvement of photo-oxidation activity: Role of oxygen on visible light photocatalytic activity Qiu, Pengxiang; Xu, Chenmin; Chen, Huan Applied Catalysis B: Environmental, Vol. 206 https://doi.org/10.1016/j.apcatb.2017.01.058	journal	June 2017
Doping of graphitic carbon nitride for photocatalysis: A reveiw Jiang, Longbo; Yuan, Xingzhong; Pan, Yang Applied Catalysis B: Environmental, Vol. 217 https://doi.org/10.1016/j.apcatb.2017.06.003	journal	November 2017
Self-assembled synthesis of defect-engineered graphitic carbon nitride nanotubes for efficient conversion of solar energy Mo, Zhao; Xu, Hui; Chen, Zhigang Applied Catalysis B: Environmental, Vol. 225 https://doi.org/10.1016/j.apcatb.2017.11.041	journal	June 2018
Unveiling the origin of boosted photocatalytic hydrogen evolution in simultaneously (S, P, O)-Codoped and exfoliated ultrathin g-C3N4 nanosheets Liu, Qinqin; Shen, Jiyou; Yu, Xiaohui Applied Catalysis B: Environmental, Vol. 248 https://doi.org/10.1016/j.apcatb.2019.02.020	journal	July 2019
Boron doped g-C3N4 with enhanced photocatalytic UO22+ reduction performance Lu, Changhai; Chen, Rongyue; Wu, Xi Applied Surface Science, Vol. 360 https://doi.org/10.1016/j.apsusc.2015.11.112	journal	January 2016
Metal-doped graphitic carbon nitride (g-C3N4) as selective NO2 sensors: A first-principles study Zhang, Hong-ping; Du, Aijun; Gandhi, Neha S. Applied Surface Science, Vol. 455 https://doi.org/10.1016/j.apsusc.2018.06.034	journal	October 2018
Mechanical properties and thermal conductivity of graphitic carbon nitride: A molecular dynamics study Mortazavi, Bohayra; Cuniberti, Gianaurelio; Rabczuk, Timon Computational Materials Science, Vol. 99 https://doi.org/10.1016/j.commatsci.2014.12.036	journal	March 2015
One-step synthesis of oxygen doped g-C3N4 for enhanced visible-light photodegradation of Rhodamine B Tran, Doan An; Nguyen Pham, Chi Thanh; Nguyen Ngoc, Tri Journal of Physics and Chemistry of Solids, Vol. 151 https://doi.org/10.1016/j.jpcs.2020.109900	journal	April 2021
Graphitic carbon nitride based nanocomposites for the photocatalysis of organic contaminants under visible irradiation: Progress, limitations and future directions Xu, Bentuo; Ahmed, Mohammad Boshir; Zhou, John L. Science of The Total Environment, Vol. 633 https://doi.org/10.1016/j.scitotenv.2018.03.206	journal	August 2018
Defect Engineered g-C ₃ N ₄ for Efficient Visible Light Photocatalytic Hydrogen Production Tay, Qiuling; Kanhere, Pushkar; Ng, Chin Fan Chemistry of Materials, Vol. 27, Issue 14 https://doi.org/10.1021/acs.chemmater.5b02344	journal	July 2015
Graphitic Carbon Nitride (g-C ₃ N ₄ )-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability? Ong, Wee-Jun; Tan, Lling-Lling; Ng, Yun Hau Chemical Reviews, Vol. 116, Issue 12 https://doi.org/10.1021/acs.chemrev.6b00075	journal	May 2016
Decoherence Allows Model Reduction in Nonadiabatic Dynamics Simulations Trivedi, Dhara J.; Prezhdo, Oleg V. The Journal of Physical Chemistry A, Vol. 119, Issue 33 https://doi.org/10.1021/acs.jpca.5b05869	journal	August 2015
Corrugation Matters: Structure Models of Single Layer Heptazine-Based Graphitic Carbon Nitride from First-Principles Studies Gao, Qian; Zhuang, Xinying; Hu, Shuanglin The Journal of Physical Chemistry C, Vol. 124, Issue 8 https://doi.org/10.1021/acs.jpcc.0c00411	journal	February 2020
Concentric Approximation for Fast and Accurate Numerical Evaluation of Nonadiabatic Coupling with Projector Augmented-Wave Pseudopotentials Chu, Weibin; Prezhdo, Oleg V. The Journal of Physical Chemistry Letters, Vol. 12, Issue 12 https://doi.org/10.1021/acs.jpclett.0c03853	journal	March 2021
Observation of an Excitonic Quantum Coherence in CdSe Nanocrystals Dong, Shuo; Trivedi, Dhara; Chakrabortty, Sabyasachi Nano Letters, Vol. 15, Issue 10 https://doi.org/10.1021/acs.nanolett.5b02786	journal	September 2015
Synergistic Effects of Boron and Sulfur Co-doping into Graphitic Carbon Nitride Framework for Enhanced Photocatalytic Activity in Visible Light Driven Hydrogen Generation Babu, Pradeepta; Mohanty, Satyaranjan; Naik, Brundabana ACS Applied Energy Materials, Vol. 1, Issue 11 https://doi.org/10.1021/acsaem.8b00956	journal	October 2018
Enhancing Photocatalytic Activity of Graphitic Carbon Nitride by Codoping with P and C for Efficient Hydrogen Generation Wang, Hao; Wang, Bo; Bian, Yaru ACS Applied Materials & Interfaces, Vol. 9, Issue 26 https://doi.org/10.1021/acsami.7b02445	journal	June 2017
Band Engineering of Carbon Nitride Monolayers by N-Type, P-Type, and Isoelectronic Doping for Photocatalytic Applications Makaremi, Meysam; Grixti, Sean; Butler, Keith T. ACS Applied Materials & Interfaces, Vol. 10, Issue 13 https://doi.org/10.1021/acsami.8b01729	journal	March 2018
Graphitic Carbon Nitride: Synthesis, Properties, and Applications in Catalysis Zhu, Junjiang; Xiao, Ping; Li, Hailong ACS Applied Materials & Interfaces, Vol. 6, Issue 19 https://doi.org/10.1021/am502925j	journal	September 2014
The PYXAID Program for Non-Adiabatic Molecular Dynamics in Condensed Matter Systems Akimov, Alexey V.; Prezhdo, Oleg V. Journal of Chemical Theory and Computation, Vol. 9, Issue 11 https://doi.org/10.1021/ct400641n	journal	October 2013
Advanced Capabilities of the PYXAID Program: Integration Schemes, Decoherence Effects, Multiexcitonic States, and Field-Matter Interaction Akimov, Alexey V.; Prezhdo, Oleg V. Journal of Chemical Theory and Computation, Vol. 10, Issue 2 https://doi.org/10.1021/ct400934c	journal	January 2014
Persistent Electronic Coherence Despite Rapid Loss of Electron–Nuclear Correlation Akimov, Alexey V.; Prezhdo, Oleg V. The Journal of Physical Chemistry Letters, Vol. 4, Issue 22 https://doi.org/10.1021/jz402035z	journal	November 2013
Auger-Mediated Electron Relaxation Is Robust to Deep Hole Traps: Time-Domain Ab Initio Study of CdSe Quantum Dots Trivedi, Dhara J.; Wang, Linjun; Prezhdo, Oleg V. Nano Letters, Vol. 15, Issue 3 https://doi.org/10.1021/nl504982k	journal	February 2015
Functional carbon nitride materials — design strategies for electrochemical devices Kessler, Fabian K.; Zheng, Yun; Schwarz, Dana Nature Reviews Materials, Vol. 2, Issue 6 https://doi.org/10.1038/natrevmats.2017.30	journal	May 2017
A metal-free polymeric photocatalyst for hydrogen production from water under visible light Wang, Xinchen; Maeda, Kazuhiko; Thomas, Arne Nature Materials, Vol. 8, Issue 1 https://doi.org/10.1038/nmat2317	journal	November 2008
Dual-defect-modified graphitic carbon nitride with boosted photocatalytic activity under visible light Katsumata, Hideyuki; Higashi, Fumiya; Kobayashi, Yuya Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-49949-6	journal	October 2019
A facile approach to synthesize novel oxygen-doped g-C3N4 with superior visible-light photoreactivity Li, Jianghua; Shen, Biao; Hong, Zhenhua Chemical Communications, Vol. 48, Issue 98 https://doi.org/10.1039/c2cc35862j	journal	January 2012
Graphitic carbon nitride based nanocomposites: a review Zhao, Zaiwang; Sun, Yanjuan; Dong, Fan Nanoscale, Vol. 7, Issue 1 https://doi.org/10.1039/c4nr03008g	journal	January 2015
Graphitic carbon nitride “reloaded”: emerging applications beyond (photo)catalysis Liu, Jian; Wang, Hongqiang; Antonietti, Markus Chemical Society Reviews, Vol. 45, Issue 8 https://doi.org/10.1039/c5cs00767d	journal	January 2016
Recent progress in g-C ₃ N ₄ based low cost photocatalytic system: activity enhancement and emerging applications Yin, Shengming; Han, Jianyu; Zhou, Tianhua Catalysis Science & Technology, Vol. 5, Issue 12 https://doi.org/10.1039/c5cy00938c	journal	January 2015
Recent advances in non-metal modification of graphitic carbon nitride for photocatalysis: a historic review Zhou, Li; Zhang, Huayang; Sun, Hongqi Catalysis Science & Technology, Vol. 6, Issue 19 https://doi.org/10.1039/c6cy01195k	journal	January 2016
Boron-doped graphitic carbon nitride nanosheets for enhanced visible light photocatalytic water splitting Thaweesak, Supphasin; Wang, Songcan; Lyu, Miaoqiang Dalton Transactions, Vol. 46, Issue 32 https://doi.org/10.1039/c7dt00933j	journal	January 2017
Oxygen self-doped g-C ₃ N ₄ with tunable electronic band structure for unprecedentedly enhanced photocatalytic performance Wei, Fangyan; Liu, Yang; Zhao, Heng Nanoscale, Vol. 10, Issue 9 https://doi.org/10.1039/c7nr09660g	journal	January 2018
Graphitic carbon nitride (g-C ₃ N ₄ ) electrodes for energy conversion and storage: a review on photoelectrochemical water splitting, solar cells and supercapacitors Safaei, Javad; Mohamed, Nurul Aida; Mohamad Noh, Mohamad Firdaus Journal of Materials Chemistry A, Vol. 6, Issue 45 https://doi.org/10.1039/c8ta08001a	journal	January 2018
Ab initio nonadiabatic molecular dynamics of charge carriers in metal halide perovskites Li, Wei; She, Yalan; Vasenko, Andrey S. Nanoscale, Vol. 13, Issue 23 https://doi.org/10.1039/d1nr01990b	journal	January 2021
Classical Path Approximation for the Boltzmann Density Matrix Miller, William H. The Journal of Chemical Physics, Vol. 55, Issue 7 https://doi.org/10.1063/1.1676560	journal	October 1971
Influence of the exchange screening parameter on the performance of screened hybrid functionals Krukau, Aliaksandr V.; Vydrov, Oleg A.; Izmaylov, Artur F. The Journal of Chemical Physics, Vol. 125, Issue 22 https://doi.org/10.1063/1.2404663	journal	December 2006
Regarding the validity of the time-dependent Kohn–Sham approach for electron-nuclear dynamics via trajectory surface hopping Fischer, Sean A.; Habenicht, Bradley F.; Madrid, Angeline B. The Journal of Chemical Physics, Vol. 134, Issue 2 https://doi.org/10.1063/1.3526297	journal	January 2011
Quantum decoherence in mixed quantum‐classical systems: Nonadiabatic processes Bittner, Eric R.; Rossky, Peter J. The Journal of Chemical Physics, Vol. 103, Issue 18 https://doi.org/10.1063/1.470177	journal	November 1995
Evaluation of quantum transition rates from quantum-classical molecular dynamics simulations Prezhdo, Oleg V.; Rossky, Peter J. The Journal of Chemical Physics, Vol. 107, Issue 15 https://doi.org/10.1063/1.474312	journal	October 1997
Decoherence-induced surface hopping Jaeger, Heather M.; Fischer, Sean; Prezhdo, Oleg V. The Journal of Chemical Physics, Vol. 137, Issue 22 https://doi.org/10.1063/1.4757100	journal	December 2012
Phonon-induced pure-dephasing of luminescence, multiple exciton generation, and fission in silicon clusters Liu, Jin; Neukirch, Amanda J.; Prezhdo, Oleg V. The Journal of Chemical Physics, Vol. 139, Issue 16 https://doi.org/10.1063/1.4825401	journal	October 2013
Ab initio quantum dynamics of charge carriers in graphitic carbon nitride nanosheets Agrawal, Sraddha; Lin, Wei; Prezhdo, Oleg V. The Journal of Chemical Physics, Vol. 153, Issue 5 https://doi.org/10.1063/5.0010628	journal	August 2020
A review of the current status of graphitic carbon nitride Rono, Nicholas; Kibet, Joshua K.; Martincigh, Bice S. Critical Reviews in Solid State and Materials Sciences https://doi.org/10.1080/10408436.2019.1709414	journal	January 2020
Recent developments of doped g-C ₃ N ₄ photocatalysts for the degradation of organic pollutants Liu, Xiaolu; Ma, Ran; Zhuang, Li Critical Reviews in Environmental Science and Technology, Vol. 51, Issue 8 https://doi.org/10.1080/10643389.2020.1734433	journal	March 2020
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/physrevb.47.558	journal	January 1993
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium Kresse, G.; Hafner, J. Physical Review B, Vol. 49, Issue 20, p. 14251-14269 https://doi.org/10.1103/physrevb.49.14251	journal	May 1994
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/physrevb.54.11169	journal	October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/physrevb.59.1758	journal	January 1999
Van der Waals density functionals applied to solids Klimeš, Jiří; Bowler, David R.; Michaelides, Angelos Physical Review B, Vol. 83, Issue 19 https://doi.org/10.1103/physrevb.83.195131	journal	May 2011
Quantum Zeno Effect Rationalizes the Phonon Bottleneck in Semiconductor Quantum Dots Kilina, Svetlana V.; Neukirch, Amanda J.; Habenicht, Bradley F. Physical Review Letters, Vol. 110, Issue 18 https://doi.org/10.1103/physrevlett.110.180404	journal	May 2013
Density-Functional Theory for Time-Dependent Systems Runge, Erich; Gross, E. K. U. Physical Review Letters, Vol. 52, Issue 12 https://doi.org/10.1103/physrevlett.52.997	journal	March 1984
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/physrevlett.77.3865	journal	October 1996
Trajectory Surface Hopping in the Time-Dependent Kohn-Sham Approach for Electron-Nuclear Dynamics Craig, Colleen F.; Duncan, Walter R.; Prezhdo, Oleg V. Physical Review Letters, Vol. 95, Issue 16 https://doi.org/10.1103/physrevlett.95.163001	journal	October 2005
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data Momma, Koichi; Izumi, Fujio Journal of Applied Crystallography, Vol. 44, Issue 6 https://doi.org/10.1107/s0021889811038970	journal	October 2011

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Charge carrier nonadiabatic dynamics in non-metal doped graphitic carbon nitride

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